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Nontrivial spin orders with magnetic chirality emerge in a particular class of magnetic materials with structural chirality, which are frequently referred to as chiral magnets. Various interesting physical properties are expected to be induced in chiral magnets through the coupling of chiral magnetic orders with conduction electrons and electromagnetic fields. One promising candidate for achieving these couplings is a chiral spin soliton lattice. Here, we review recent experimental observations mainly carried out on the monoaxial chiral magnetic crystal CrNb3S6 via magnetic imaging using electron, neutron, and X-ray beams and magnetoresistance measurements, together with the strategy for synthesizing chiral magnetic materials and underlying theoretical backgrounds. The chiral soliton lattice appears under a magnetic field perpendicular to the chiral helical axis and is very robust and stable with phase coherence on a macroscopic length scale. The tunable and topological nature of the chiral soliton lattice gives rise to nontrivial physical properties. Indeed, it is demonstrated that the interlayer magnetoresistance scales to the soliton density, which plays an essential role as an order parameter in chiral soliton lattice formation, and becomes quantized with the reduction of the system size. These interesting features arising from macroscopic phase coherence unique to the chiral soliton lattice will lead to the exploration of routes to a new paradigm for applications in spin electronics using spin phase coherence.
“Chirality” is one of the essential concepts behind the symmetry properties of nature at all length scales. Helical structures, i.e., three-dimensional spirals winding around a principal axis, can be chiral when the components exhibit a fixed sense of the rotation. Among the wide variety of chiral helices, we can infer the essence of chiral objects, namely, that they intrinsically involve dynamical motion.
Indeed, natural philosophers and scientists have been aware of such a dynamical aspect of helical structures for a long time. Goethe mentioned what he called “a spiral tendency in nature” when observing that the leaves around the shoot of a plant often exhibit a regular spiral or helical arrangement. This is a rather literary phrase, quoted from the book “Symmetry” by Herman Weyl,1) providing a suitable description of the world around us. The spiral or helical arrangement of leaves and flowers, named phyllotaxis, has been the subject of much study among botanists.
Similar pattern formations of three-dimensional helices including two-dimensional spirals are widely found in various systems. For instance, on a macroscopic scale, such patterns appear in architectural spiral staircases, whirlpools in water, typhoons (hurricanes) in the Pacific (Atlantic) Ocean, and galaxies in the universe. In general, the symmetry breaking of the upside-down reflection is essential for defining the chirality of whirlpools, which again reminds us of the three-dimensional structure and consequent dynamical nature of chiral helical objects.
Immanuel Kant was the first natural philosopher to discuss the significant meaning of the distinction of mirror images, i.e., left- and right-handedness, in the eighteenth century. The scientific investigation of chirality started with the discovery of the (natural) optical rotation of linearly polarized light in quartz or aqueous solutions of tartaric acid or sugar by Arago and Biot. In 1848, Louis Pasteur demonstrated that the direction of (natural) optical rotation is determined by the handedness of the crystal structure after the careful and painstaking separation of sodium ammonium tartrate crystals into those with two different types of crystal shape. These pioneering studies helped reveal the existence of chiral molecules and crystals at the atomic length scale.
Lord Kelvin first introduced the word “chirality” and provided its celebrated definition in the Baltimore lectures on “Molecular Dynamics and the Wave Theory of Light” in 1884. Lecture notes made by one of the audience were published in 1904 after being supplemented by Lord Kelvin,2) where he stated, “I call any geometrical figure, or group of points,
A hundred years later, the concept of chirality was refined by Laurence Barron3,4) so as to distinguish the dynamical aspect of chirality from non-chiral phenomena. Barron introduced two types of enantiomorphism to be differentiated as true and false chirality.4) “True chirality is exhibited by systems that exist in two distinct enantiomeric states that are interconverted by space inversion (parity
Meanwhile, space inversion involves geometrical symmetry, while time reversal involves dynamical motion. As described above, the essence of the helical structure should be seen as a combination of spatial rotation and translation. In this respect, the refined definition indicates that the concept of chirality makes a connection between geometry and dynamics. Static helical structures are obviously distinguished in terms of the original definition of chirality describing left- or right-handedness. However, when motion is involved, the concept of chirality holds only for a dynamical object that breaks mirror symmetry or parity (
In condensed matter physics, chiral symmetry breaking in materials plays an essential role in stabilizing a macroscopic ordered state with a left- or right-handed incommensurate (IC) twist of multicomponent order parameters. This kind of IC state accommodates topological discommensuration (DC). Typical examples are an incommensurate helical magnetic structure and concomitant topological DCs, shown in Figs. 1 and 2, which are the main issues in this review. The physical picture is in contrast with the case of charge density wave and collinear spin magnetic structures in terms of orientational degrees of freedom.
Figure 1. (Color online) Left- and right-handed helimagnetic structures and soliton lattices.
Figure 2. (Color online) Formation of a chiral soliton lattice (CSL) under a magnetic field applied perpendicular to the helical axis. In the continuum limit, the CSL structure can be depicted as a twisted rubber ribbon. As the magnetic field increases from (a) zero to (e) the critical field strength, the spatial period of the CSL increases and eventually reaches infinity at the critical field.
There are two categories of helimagnetic structures. The first are called Yoshimori-type or symmetric helimagnets. The microscopic mechanism of symmetric helimagnets involves the frustration among exchange interactions. In the 1950's, it was pointed out by Yoshimori,7) Kaplan,8) and Villain9) that the magnetic structure of MnO210) can be interpreted as a helimagnetic structure. The early research on helimagnetism was reviewed by Nagamiya.11) In the 2000's, multiferroic materials were found to exhibit new aspects of frustration-driven non-collinear magnetic structures and related functionalities in the non-chiral helimagnetic materials.12)
The other type of helimagnetic structures, which are chiral, are stabilized by an antisymmetric exchange interaction envisioned by Dzyaloshinskii based on symmetry considerations.13–16) Namely, the antisymmetric exchange interaction is the source of the chiral helimagnet. The microscopic mechanism was revealed to be due to the relativistic spin–orbit interaction in the framework of perturbation theory by Moriya,17) which is applicable to the case of insulating magnets. The antisymmetric exchange interaction, which is sometimes called the Dzyaloshinskii–Moriya (DM) interaction as a generic term irrespective of the system under investigation, imprints an asymmetric electronic structure to the antisymmetric spin–spin interaction in the form of
When
Therefore, in the CHM structure realized in the chiral crystal, the degeneracy between the left- and right-handed helical structures is lifted at the level of the Hamiltonian. Namely, the macroscopic DM interaction appears in the Landau free energy as the Lifshitz invariant.14) Theoretical and experimental works on this topic until the early 1980's were well reviewed by Izyumov.18) In addition, Dzyaloshinskii's work activated the research field of improper ferroelectricity, where the physical outcome of the Lifshitz invariant was intensively studied.19,20)
The helimagnetic structures of the Yoshimori and Dzyaloshinskii types exhibit similar spin structures at first glance. However, there is a profound difference in the level of chiral symmetry that is broken. In the former case, the chiral symmetry is not broken at the level of the Hamiltonian, but the helimagnetic structure spontaneously breaks the chiral symmetry. Therefore, the symmetric helimagnet does not have any macroscopic protection and is easily fragmented into multiple domains. On the other hand, in the latter case, the Hamiltonian itself breaks the chiral symmetry because of the DM interaction and the magnetic structure is forced to break the chiral symmetry. An essential feature of the CHM structure is that it is protected by the crystal chirality. In Fig. 3, we summarize the basic properties of symmetric and chiral helimagnets.
Figure 3. (Color online) Basic properties of symmetric and chiral helimagnets.
Significant differences arise in the response of magnetic structures to an external magnetic field as well as elementary excitations. Under a static magnetic field perpendicular to the helical axis, the symmetric helimagnetic structure undergoes a discontinuous transition into a fan structure and then continuously approaches the forced ferromagnetic state.11) On the other hand, in a chiral helimagnet, the ground state continuously transforms into a periodic array of commensurate (C) domains partitioned by IC chiral twists. This discommensurate state, a major subject of this review article, has several names, i.e., a chiral soliton lattice (CSL), helicoid, or magnetic kink crystal (MKC).14,18) Throughout the present paper, we use the term chiral soliton lattice. As the magnetic field strength increases, the spatial period of the CSL increases and finally reaches infinity at the critical field strength, as depicted in Fig. 2. The rotation angle of the helix is considerably different from that formed in symmetric helimagnets because of the origin of the helix. As a result, the symmetric helimagnetic structure has a short period of typically less than 1 nm while the CHM has a period of 1–100 nm order. The dispersion of the spin wave is also different for the two structures.
Almost a half century after its theoretical prediction,14) direct experimental observation of the CSL was achieved by Togawa et al. in the monoaxial hexagonal crystal of the chiral helimagnet CrNb3S621) which has a magnetic phase transition temperature
Theoretically, the CSL has some special features to be noted. (1) In the CSL state, the translational symmetry along the helical axis is spontaneously broken. Therefore, the corresponding Goldstone mode becomes phonon-like.14,22) (2) The CSL state has infinite degeneracy associated with an arbitrary choice of the center of mass position. Consequently, the CSL can exhibit coherent sliding motion.23) (3) The CSL exerts a magnetic superlattice potential on the conduction electrons coupled to it. This coupling causes a magneto-resistance effect.24,25) (4) Quantum spins carried by conduction electrons generate spin-transfer torque on the CSL.26) Some of these physical properties have already been demonstrated experimentally.25,27)
In this review, we describe how nontrivial spin orders with magnetic chirality emerge in chiral helimagnets and the kinds of physical properties induced in chiral magnets through the coupling of chiral magnetic orders with conduction electrons and electromagnetic fields. A general introduction to chiral helimagnetism including the definition of chirality is given in the present section. In Sect. 2, we present a list of representative molecule-based and inorganic chiral magnets and briefly describe the strategy for synthesizing these chiral magnets. In Sect. 3, we explain how chiral magnetic structures are observed and analyzed by experimental methods using particle beams. In particular, the experimental demonstration of the existence of the CSL and its characteristics including macroscopic phase coherence are explained in detail. In Sect. 4, nontrivial physical properties including negative magnetoresistance and discretization (quantization) effects are described. We see that the soliton density plays an important role as an order parameter in the IC–C phase transition of the CSL formation, governing the physical properties. In Sect. 5, we summarize the fundamental physical background of the CSL from theoretical viewpoints. Finally, we discuss the meaning of macroscopic phase coherence in condensed matter physics. Some supplementary and technical materials are given in Appendix.
To design chiral materials, there are two possible strategies. One is suitable for molecular-based materials, where the ligand itself is chiral, i.e., it possesses low symmetry and the symmetry of the crystal class is also low such as monoclinic or orthorhombic. The other is useful for inorganic materials, where the building block has low symmetry while the crystal class has high symmetry such as tetragonal, hexagonal, rhombohedral, or cubic.
Molecule-based chiral magnets that has been reported are shown in Table I.28–44) The space groups for molecule-based chiral magnets are typically triclinic
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To obtain noncentrosymmetric (polar or chiral) molecule-based magnets, the geometric symmetry of chiral crystals must be controlled in the molecular structure as well as in the entire crystal structure. A major strategy relating to crystal design for magnetic materials exhibiting long-range magnetic ordering and spontaneous magnetization involves the generation of an extended array of paramagnetic metal ions (M) with bridging ligands (L). Namely, chirality induction plays an important role in the design of molecule-based chiral magnets.
High-spin nitroxide or nitronylnitroxide radicals, cyanide ions, or oxalate dianions are frequently used for bridging ligands. The cyanide-bridged Prussian-blue and oxalate-bridged systems are generally obtained as bimetallic assemblies with two- or three-dimensional (2-D or 3-D) networks by the reaction of a hexacyanometalate [M
Some chiral amines,28–34) nitroxide radicals,35,36) nitonylnitroxide radicals,37) and amino acids38–40) serve as ligands for the chiral source in the entire crystal structures of these systems. For oxalate-bridged systems, some chiral countercations are used.41–43) For instance, in cyanide-bridged systems, a target magnetic compound can be generated by the reaction between a hexacyanometalate [M
Spontaneous chiral symmetry breaking during crystallization (called spontaneous crystallization) occurs in some molecule-based chiral magnets.44) In this case, crystals with one handedness can be selected from those with the other handedness.
Table II is a list of major chiral inorganic helimagnetic materials. CrNb3S6,46,47) CsCuCl3,48) and YbNi3Al949) have a monoaxial crystalline structure with a principal axis, while MnSi,50) FeGe,51) Fe
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As described in Sect. 2.1 for the synthesis of molecule-based chiral magnetic materials, chiral organic ligands can be employed because chirality induction works effectively. On the other hand, to synthesize chiral inorganic magnets, spontaneous crystallization should be required, which results in chiral symmetry breaking of the crystals. It is already known that several hundred chiral crystals are obtained by the spontaneous crystallization among over 5 million crystals. However, the effective strategy or design for spontaneous crystallization still remains to be established. As a consequence, only the chiral inorganic compounds that have been reported so far are being materials to be examined.
Some inorganic magnetic materials belonging to a chiral space group have been unexpectedly found and reported over several decades. Dzyaloshinskii14) theoretically predicted the possibility of the CHM in 1964. In the 1970's, there were several studies of the magnetic structure for the B20-type compound MnSi crystallizing in the
Crystal design and the creation of inorganic chiral magnets are important to obtain a wide variety of crystals. From the viewpoint of crystal symmetry, there are two approaches to obtain chiral crystals. The first approach is to use group 13, 14, or 15 elements to construct crystals, such as MnSi,50) FeGe,51) and Fe
The synthetic methods for these inorganic chiral magnets are chemical transport, flux, solution, and hydrothermal methods. For instance, for the synthesis of YbNi3Al9,49) MnSi, and Fe
Chiral crystal structures have left and right enantiomorphs, and the thermodynamical energies of these two enantiomorphs are the same. Therefore, these two structures are easily mixed and the crystals grow as racemic twinned ones, having left and right enantiomeric domains. Recent progress in crystallization techniques, discussed in Sect. 2.3, can avoid this difficulty in inorganic compounds.
For inorganic compounds, it is still a major challenge to control the crystallographic chirality. Most inorganic chiral magnetic materials form racemic twinned crystals, having left- and right-handed crystalline domains in a specimen. In this case, unique properties, ranging from a CHM structure to physical properties such as magneto-chiral dichroism (MChD),56) cannot be detected experimentally because they can be canceled by the left- and right-handed crystalline domains in the sample. Therefore, it is very important to synthesize chiral magnetic compounds with a homochiral domain. Ohsumi et al. reported that the domain sizes of the left- and right-handed crystals in a racemic twinned CsCuCl3 are of 10 µm order.57) This means that it is necessary to separate the left- and right-handed domains during the crystallization process.
On the other hand, there are some exceptional compounds that break the chiral symmetry and spontaneously form only the left- or right-handed crystal domain. Transition-metal monosilicides with a B20-type chiral crystal structure are among the few compounds forming a homochiral crystal domain. Single crystals of helimagnetic MnSi form the left-handed crystal domain, and polarized neutron diffraction experiments have probed the left-handed spiral structure.58,59) In such homochiral inorganic crystals, it is difficult to synthesize single crystals having the opposite crystalline chirality such as right-handed MnSi. Dyadkin et al. reported that polycrystalline MnSi contains left- and right-handed crystalline domains.60) In this sense, there is some room to synthesize the opposite homochiral crystals. We show two crystallization techniques to segregate or control the crystallographic chirality in the crystallization process.
Even racemic twinned compounds such as CsCuCl3 sometimes form a homochiral crystal when the sample size is of submillimeter order.61) As discussed here, water-soluble compounds can produce homochiral crystals using a novel crystallization technique that induces spontaneous crystallization with stirring. Using a conventional crystallization technique, the water-soluble B20-type compound NaClO3 forms racemic twinned crystals. However, with stirring of the solution during the crystallization process, crystalline specimens surprisingly form a homochiral domain.62)
This crystallization technique is also applied to chiral magnetic materials. CsCuCl3 is a water-soluble chiral magnet, single crystals of which are prepared from an aqueous solution containing CsCl and CuCl2 by slow evaporation of a slightly acidified solution.63) When the solution is constantly stirred using a Teflon stirrer bar during the crystallization process, hundreds of single crystals can be obtained from the solution with a size of 0.4–1.0 mm diameter and 1–3 mm length. Figure 4 shows photographs of single crystals obtained by the conventional crystallization technique without stirring and by the novel method with stirring.64) The samples obtained without stirring have a zigzag shape, indicating that many crystalline nuclei combined during the crystallization process. Absolute structure analysis using X-rays shows that the obtained samples form racemic twinned crystals. On the other hand, the samples obtained with stirring have a quartz-crystal-like shape, indicating that only one crystalline nucleus grew. This suggests that the aqueous stream due to stirring prevents each growing nuclei from combining during the crystallization process. Absolute structure analysis indicates that over 70% of the obtained crystalline samples form homochiral crystals, having only the left- or right-handed chiral crystalline domain.
Figure 4. (Color online) Photographs of single crystalline CsCuCl3 obtained by crystallization (a) without stirring (conventional method) and (b) with stirring (novel method).
This crystallization technique can only be applied to water-soluble compounds. The problem is that most inorganic compounds are insoluble in water. In this respect, the method can be extended to water-insoluble materials by using the flux method. In this case, the flux can act as a solution with a high temperature. Therefore, the flux method with stirring has strong potential to obtain homochiral crystals.
The tri-arc Czochralski method is known as a powerful technique to grow single crystals of intermetallic compounds such as transition-metal monosilicides. In the case of Fe
This idea for preparing seed crystals can be applied to chiral compounds forming racemic twinned domains as discussed in Sect. 2.3.2. If we grow a single crystal from a small homochiral seed crystal, it may inherit the chirality of the seed crystal and grow as a homochiral large single crystal.
Magnetic structures in materials are examined by analyzing the real- and/or reciprocal-space data obtained in scattering experiments using particle beams such as neutron, X-ray, photon, electron, and muon beams. The precise detection of the scattering or deflection of particle beams in the reciprocal space allows us to make a quantitative analysis of magnetic structures. On the other hand, real-space images are useful for making intuitive and qualitative interpretations of magnetic structures. In this section, we briefly summarize experimental methods using electron, neutron, and X-ray beams to observe and analyze magnetic structures. Then, a demonstration is given of the existence of the chiral magnetic soliton lattice in monoaxial chiral magnets including the determination of crystalline and magnetic chirality using these complementary methods.
Electrons have charge and thus are deflected by the Lorentz force when they pass through an area with an electric and/or magnetic field. Based on this simple mechanism, an electron beam probes electromagnetic structures in materials. Hence, the method is frequently called Lorentz microscopy.67–71)
In the following subsections, we provide a brief introduction to the methods of observing and analyzing magnetic structures using an electron beam. In particular, the principle and capacities of real-space observation and reciprocal-space analysis in transmission electron microscopy (TEM) are given. As shown later, these methods are very useful for the detection of chiral magnetic orders in chiral magnets.21)
An electron beam in a TEM system is accelerated by a large voltage of typically 10–100 kV order.72,73) Thus, it has a very short wavelength λ of picometer order (e.g.,
Multiple electromagnetic lenses are set in a commercial transmission electron microscope to magnify or reduce the intensity distribution map of the electron beam. Although the physical distance between adjacent electromagnetic lenses is fixed, the optical abilities of an electromagnetic lens (e.g., focal length and thus the magnification) are altered simply by changing the excitation current in each lens. This optical setup of the TEM system allows flexible control of the electron optical conditions and the collection of the real-space images as well as the reciprocal scattering data, similarly to optical microscopy.
To observe magnetic structures, magnetic imaging almost always requires a low magnetic field around the sample. For this purpose, the objective lens of the microscope is either switched off or only weakly excited. To examine the field dependence, it can be gradually excited by changing the current of the objective lens.
The features of the electron beam and TEM mentioned above enable the analyses of magnetic structures in both real and reciprocal spaces at various magnifications in Lorentz microscopy. That is, the distribution of electric and magnetic fields inside and outside materials can be visualized in a real-space image with a spatial resolution of nm order or higher,71) which is useful for directly observing magnetic structures. Simultaneously, the scattering or deflection of an electron beam, reflecting the electromagnetic potential, can be directly detected in the reciprocal space at a camera length of up to 100 m order in the same area as that in which the real-space images are obtained.70)
The complementary data set obtained from the same area of the specimen is an advantage of Lorentz microscopy, which is in contrast with the reciprocal-space data analysis via scattering experiments using other particle beams such as a neutron beam. However, TEM analysis is only applicable to thin specimens, where the physical conditions are different from those in bulk specimens used in neutron experiments. This means that careful consideration is required to understand the physical meaning of TEM images and scattering data.
As described above, Lorentz transmission electron microscopy is named after the Lorentz force acting on an electron beam in the presence of an electric and/or magnetic field. This term is mainly based on a “particle” picture of electrons. The principle of Lorentz microscopy is also described quantitatively on the basis of the wave optical Aharanov–Bohm effect.68) In the latter case, electric and magnetic fields shift the phase of the electron beam as a “wave” and deflect the propagation direction of the wavefront of the electron beam.
In this respect, the term Lorentz microscopy has a rather broad meaning; it can include a branch of methods for investigating magnetic and electrostatic structures.69,70) For instance, electron holography74) can be regarded as one of the quantitative techniques of Lorentz microscopy. The term electron interferometry is also used instead of Lorentz microscopy when focusing on the “wave” nature and interference phenomena of electrons.
Indeed, various qualitative and quantitative modes of Lorentz microscopy have been developed, as described in review articles and books,68–70,74) since Hale et al. first reported TEM images of magnetic domain structures in 1959.75) Several representative and useful modes of Lorentz microscopy are introduced in the following subsections.
The Fresnel mode of Lorentz microscopy is used to analyze magnetic structures qualitatively. Figure 5 shows the principle of the Fresnel mode and how the twist of a chiral soliton in the CSL is visualized depending on its magnetic chirality.
Figure 5. (Color online) Schematic drawings of electron beam deflection by magnetic fields in magnetic structures and the principle of the Fresnel and DPC modes of Lorentz microscopy. Ray diagrams of an electron beam illustrate the relation between the contrast formed in Lorentz micrographs obtained by the Fresnel and DPC modes and the twist of a chiral soliton in the CSL. The direction of the magnetization m transverse to the electron beam is determined from the bright and dark contrast. The intensity profile maps of the in-plane m and its spatial gradient
An electron beam passing through the magnetic structure formed in a magnetic thin film is deflected by the Lorentz force in the region with magnetic moments transverse to electron beam propagation. Thus, in a defocused plane, a bright or dark contrast pattern appears in locations where the magnitude of the in-plane magnetization m is not uniform, such as at the boundary of magnetic domains.
The relation between the contrast pattern and the direction of magnetic moments is reversed depending on the defocusing condition as schematically drawn in Fig. 5. Therefore, by examining the bright or dark contrast pattern in Lorentz Fresnel micrographs taken under a fixed defocus condition, the magnetic structure is identified qualitatively. Roughly speaking, an intensity profile map of the spatial gradient of m is obtained in the Fresnel mode when the configuration of magnetic moments is close to being divergence-free.
A 2-D map of the in-plane m distribution can be reconstructed from a series of defocused Fresnel images. More precisely, the relative phase distribution is retrieved by using the transport-intensity equation (TIE) based on the propagation theory of an electron beam.76–78) Then, the in-plane m map obtained is frequently presented in a color-wheel code to see the magnetic structure intuitively, although the information is essentially the same as the original phase map in a gray scale.
The TIE method can provide quantitative data of magnetic structures only when used under appropriate experimental conditions,79–81) although there seem to have been many misleading statements on this method, particularly on its spatial resolution. The results obtained by TIE phase retrieval should be consistent with the original Fresnel images. In this sense, the proper consideration of Fresnel images is very important to understand the images reconstructed by the TIE method.
There have been many studies of the real-space imaging of magnetic structures in cubic helimagnetic crystals by Lorentz Fresnel microscopy including the TIE method since the first reports of Fresnel micrographs of Fe0.5Co0.5Si82,83) and FeGe.84,85) Again, it should be noted that Lorentz microscopy, in principle, only detects an in-plane component of magnetic moments in the specimen. Thus, additional experimental methods with careful consideration are required to analyze real-space images by Lorentz microscopy86) and specify a detailed magnetic structure even in the case of a CHM and CSL.
Experiments involving small-angle electron scattering (SAES), also known as low-angle electron diffraction, are required to detect an electron beam deflected at a small angle by an electric or magnetic field inside or outside a material.
Such small-angle scattering experiments are frequently performed using neutron and X-ray beams, referred to as small-angle neutron scattering (SANS)87) and small-angle X-ray scattering (SAXS),88,89) respectively. SANS and SAXS have been widely utilized to analyze materials with internal structures such as micrometer-size domain structures, fine textures, and long-range periodic order from the nano- to microscale. Furthermore, neutrons interact with magnetic moments localized at atoms, which enables the very precise analysis of magnetic structures in the reciprocal space by SANS.89)
SAES experiments were first performed in the early 1960's90–92) when various modes of TEM had begun to be developed. Pioneering studies on SAES experiments on magnetic structures in magnetic materials were reported by Goringe and Jakubovics, and Wade separately in 1967.93,94) There are currently few studies focusing on the SAES detection of electric and magnetic fields. However, SAES is very effective for revealing the nature of magnetic structures in magnetic materials including chiral magnets.21)
In SAES, there are two kinds of magnetic scattering or deflection of an electron beam from magnetic structures, both of which appear at a very small angle in the reciprocal space.
First, the magnetic deflection of an electron beam occurs in magnetic materials due to the Lorentz force or the phase shift originating from the Aharanov–Bohm effect. The deflection angle β is given as
Second, when materials exhibit long-range periodic magnetic structures at the nano- or microscale, magnetic Bragg diffraction appears in the reciprocal space at an angle smaller than that of Bragg diffraction due to the crystalline lattice. Some magnetic materials exhibit periodic magnetic structures (e.g., stripe magnetic domains) with a period of typically 100 nm or µm order, giving a magnetic Bragg diffraction angle as small as
To detect such a small deflection angle of an electron beam, the camera length, which corresponds to the magnification in scattering experiments, should be greatly magnified. It was reported that in conventional TEM systems, the camera length was successfully expanded to more than 3 km and tuned down to zero continuously by adjusting the electron optical system.70,95,96)
Scanning transmission electron microscopy73) allows another type of Lorentz microscopy, where the deflection of the electron beam is collected with a segmented detector at each scanning point.97) Then, a differential phase contrast (DPC) map is constructed by calculating difference signals from opposing segments at each scanning point.68) Various kinds of detectors have been employed with bi-split,97) quadrant,98) annular quadrant,99) and pixelated100) geometries, which brought about significant improvements in the quality of DPC images. Furthermore, with the assistance of recent developments in aberration correction for electron optics,101,102) the DPC mode has achieved a spatial resolution better than 1 nm.27,71,100)
The Fresnel mode of Lorentz microscopy and SAES experiments have significantly contributed to confirming the existence of the CHM and CSL in CrNb3S6.21)
Figure 6 shows an example of Lorentz micrographs obtained at 110 K in the absence and presence of an external field perpendicular to the helical c-axis. A bright and dark contrast pattern repeatedly appears perpendicular to the c-axis and is very straight and regular in almost all the regions of the specimen observed. The contrast changes in a nearly sinusoidal manner with 48 nm period at 0 Oe. This sinusoidal pattern of in-plane magnetic moments is observed in a series of Lorentz Fresnel micrographs taken at various defocus values of less than 8 µm, and the contrast is reversed when defocusing in the opposite direction. As the field strength increases, the period
Figure 6. Lorentz Fresnel micrographs of the CHM and CSL in CrNb3S6 at 110 K. (a) 0 Oe. (b) 2080 Oe. For TEM observations, thin specimens, typically of 5 µm width, 13 µm length, and 70 nm thickness, were fabricated using a focused ion beam (FIB) etching machine. A magnetic field was applied in the direction normal to the thin platelet specimen using the objective lens of a microscope. The scale was calibrated using SAES data. The defocus value is, respectively, 2 µm and 900 nm in the underfocused direction in (a) and (b). The wide curved dark fringes are bend contours caused by electron scattering through the slightly curved TEM specimen.
The sinusoidal magnetic pattern of the CHM was precisely examined in the reciprocal space. For the CHM, two characteristic features are expected to be observed in SAES data. First, magnetic diffraction spots should appear at
Figure 7 shows such expected behavior for the CHM. A pair of diffraction spots were found at (48 nm)−1 along the c-axis close to the 000 diffraction spot. The spatial frequency detected was consistent with that obtained by SANS experiments47) as well as the period observed in real-space Lorentz images. More importantly, no higher harmonic spots were observed within the sensitivity of the SAES signal detection using films, a CCD camera, and imaging plates.
Figure 7. (Color online) Series of SAES data at 0 Oe taken from CrNb3S6 with the camera length magnified by different orders of magnitude. (a) 30 cm, (b) 30 m, and (c) 300 m. The 000 and 001 spots of Bragg diffraction give a spatial frequency of (1.2 nm)−1 in the reciprocal space. The CHM provides a pair of magnetic satellite spots with a spatial frequency of (48 nm)−1 close to the 000 spot indicated by blue arrows. (c) Elliptical shape of the central spot due to magnetic deflection.
Magnetic deflection from the CHM is also detected in SAES experiments. Figure 7(c) presents the elliptical shape of the central spot along the c-axis in SAES taken at a very long camera length of 300 m. The size of the central spot is about
The CHM gradually transforms into the CSL in magnetic fields perpendicular to the c-axis. Figure 6(b) shows that the sinusoidal pattern of the CHM transforms into another periodic pattern segmented by dark contrast lines, which is ascribed to the CSL. Figure 8(a) presents a similar periodic pattern in a different TEM specimen taken at a larger magnification. It is partitioned by three contrast lines, that is, a central dark contrast line accompanied with two adjacent bright contrast lines under the underfocused condition, which is consistent with the contrast expected for a left-handed CSL as depicted in Fig. 5.
Figure 8. Lorentz Fresnel micrograph and SAES data of the CSL at 2500 Oe in a CrNb3S6 specimen with
Namely, the analyses of the contrast pattern of the CSL in Lorentz microscopy are directly connected to the identification of the magnetic chirality of the CSL. As shown in Fig. 5, in the present TEM experimental configuration, forced FM domains in the CSL and the forced FM state have out-of-plane magnetic moments toward the applied vertical magnetic field. They are parallel to the propagation direction of the electron beam, thus do not cause any change in the specific contrast in Lorentz micrographs. Meanwhile, the
It was clarified that the CSL has left-handed magnetic chirality in the specimens presented in Figs. 6 and 8. Moreover, the CHM should inherit the same magnetic chirality because the CSL develops from the CHM. It was found that most of the area of the crystal has left-handed magnetic chirality but very small regions have the opposite magnetic chirality (see Fig. 9) in a particular bulk CrNb3S6 single crystal when the magnetic chirality of the crystal is locally examined by Lorentz microscopy.
Figure 9. Lorentz Fresnel micrograph of crystalline grains with different magnetic chirality taken under the underfocused condition at 1781 Oe at 100 K. The region with right-handed magnetic chirality is sandwiched by those with left-handed magnetic chirality.
Figure 10(a) shows an experimental plot of
Figure 10. (Color online) (a) Experimental plot of
No periodic pattern due to the CSL is observed above
The CHM and CSL are very straight and perpendicular to the chiral helical axis and appear over most of the specimen as partially shown in Fig. 6. In particular, in most cases, the CHM has hardly any structural dislocations and is resistant to crystal defects, which potentially exist in specimens, and scratch defects extrinsically formed by the irradiation of an FIB along the [001] direction during TEM specimen fabrication (see Fig. 11). The specific features of high stability and robustness originate from the fact that both the CHM and CSL are manifestations of the macroscopic order of spin magnetic moments. Indeed, the chiral magnetic orders are macroscopically induced in CrNb3S6 by the DM interaction, which is allowed in the system because the hexagonal crystal of CrNb3S6 belongs to the noncentrosymmetric chiral space group.
Figure 11. Lorentz Fresnel micrograph of CrNb3S6 at 0 Oe. The contrast modulation along the horizontal direction is due to a marked change in the thickness of the specimen caused by the irradiation of a focused gallium ion beam.
The magnetic neutron scattering technique is one of the most direct ways to probe the chiral magnetic structure. This topic has been extensively studied by many authors.104–106) We briefly review the general reasons why polarized neutron scattering is useful for later discussions. The magnetic neutron scattering is caused by the magnetic dipolar interaction between the electron magnetic moment (
Under a magnetic field, however, neutron spins are forced to be parallel to the external field. Thus, polarized neutron scattering is not applicable to the detection of the CSL state. Here we only mention unpolarized elastic neutron scattering. Neutron scattering in the CSL state was first studied by Izyumov and Laptev.107) We will describe the structure of the CSL in Sect. 5.5, and here we only mention the results for the neutron scattering cross section, which is given by
The CSL structure is given later by Eq. (27). From the formulae for the Fourier transformations,108)
Figure 12. (Color online) Profile of unpolarized elastic neutron scattering cross section.
In the case of zero field, only the first component
Figure 13. (Color online) Relative strengths of the higher harmonic peaks. (a)
To observe chiral incommensurate magnetic ordering experimentally, we should ensure very small pitch angles. As the pitch angle is mainly determined by the ratio of the exchange interaction to the DM interaction, the magnetic period can be of 10–100 nm order. In some cases, the angular resolution of thermal neutron diffractometers is not high enough to separate fundamental Bragg and magnetic satellite peaks. As a result, some compounds with the chiral helimagnetic ordering and CSL may be misinterpreted as FM ordering.
For example, a thermal neutron diffraction study of CrNb3S6 first showed FM ordering. However, Moriya and Miyadai theoretically proposed CHM ordering with very long period,46) and Miyadai et al. observed a magnetic satellite peak at
As we mentioned, polarized neutron diffraction can distinguish the left- and right-handed spiral magnetic structures. In the case of chiral magnetic materials, Ishida et al. first detected the left-handed chiral helimagnetic structure of the cubic chiral magnet MnSi by observing magnetic satellite peaks using polarized SANS.59)
Here, we introduce preliminary results for probing the CSL of MnSi using polarized SANS, measured at TAIKAN (BL15) in the Materials and Life Science Experimental Facility (MLF) of the Japan Proton Accelerator Research Complex (J-PARC).109) MnSi has several chiral helimagnetic domains along the
Figure 14. (Color online) Reciprocal line profiles along (a) the
One problem of SANS is that the technique cannot determine magnetic structures from magnetic structure analysis because it detects only one or two magnetic satellite peaks around
Figure 15 shows a high-resolution powder neutron diffractogram of CrNb3S6 obtained at SuperHRPD (BL08) in MLF of J-PARC. As indicated by the vertical arrows shown in Fig. 15, the magnetic satellite peaks are separated from the nuclear
Figure 15. (Color online) Neutron powder diffractogram around the nuclear
X-rays are known as one of the most powerful experimental probes for determining crystal structures of compounds. The chiral crystal structures are generally determined by an absolute structure analysis.
The intensities of a pair of reflections at
We emphasize that the neutron diffraction technique cannot determine the crystal chirality. Most nuclear species (elements) have no anomalous scattering in terms of the nuclear scattering amplitude. Therefore, there is no difference in the nuclear scattering intensity between
X-rays also play a very important role in magnetic structure studies in chiral science. It is well known that X-rays couple with the charge of electrons, which is independent of the magnetic structure in the compounds. However, X-rays are also scattered by magnetic electrons, and magnetic diffraction can be observed using X-rays.114,115) The problem is that the signal of the magnetic scattering is extremely small compared with that of the charge scattering. Highly brilliant synchrotron radiation sources make it possible to detect X-ray magnetic diffraction signals. The magnetic Bragg peaks due to antiferromagnetic and helimagnetic ordering have been observed since the 1970s.116,117) Using polarized X-ray beams, it is possible to detect the chirality of crystalline and helimagnetic structures. Here, we introduce some experimental results using circularly polarized X-rays.
As we mentioned, the crystalline chirality can be determined by absolute structure analysis using X-rays. However, the problem is that the method can only be applied to samples of sub-mm order, because the samples must be smaller than the beam diameter. Moreover, in the case of racemic twinned crystals, the Flack parameter merely indicates the ratio between the left- and right-handed crystalline domains in the sample and does not give information on how the left- and right-handed domains are distributed in the sample.
However, the circularly polarized resonant X-ray diffraction technique can solve such problems. To detect the crystallographic chirality, Dmitrienko proposed a theoretical prediction by observing the anisotropy of the tensor of susceptibility (ATS) scattering.118) Using the polarization of X-rays, the crystallographic chirality can be easily determined just by examining the intensity of one site of the reflection that is forbidden by the screw-axis in the crystal but recovered by the ATS scattering. This method follows the way that polarized neutron diffraction determines the chirality in helimagnetic structures.
The experimental results were first observed for α-quartz with the space group of
Figure 16 shows longitudinal scan profiles of
Figure 16. (Color online) Reciprocal scan profiles of CsCuCl3 at (a)
Moreover, using a microbeam, the technique realizes scanning X-ray imaging of the crystalline chirality in a large area.57) It gives the chiral domain distribution in racemic twinned crystals. Therefore, it will be an essential method to evaluate new crystallization techniques for controlling chiral crystalline domains.
The circularly polarized X-ray diffraction technique can detect the helicity of spiral magnetic structures. Blume and Gibbs proposed the polarization dependence of magnetic X-ray scattering.120) Using the circular polarization of X-rays, the helimagnetic chirality can be evaluated by observing magnetic satellite reflections in the same way that polarized neutron diffraction can be used to determine the chirality. Experimental results have been observed for some multiferroic compounds using circular polarization since 2009.121–123)
This experimental technique will be applied to detecting helimagnetic chirality in chiral magnetic materials. As we have discussed, the pitch angle of the CHM ordering is usually very small. In order to separate fundamental Bragg and magnetic satellite peaks, the angular resolution must be high. However, this is not a problem for synchrotron radiation, having much better angular resolution than neutron sources. In this sense, circularly polarized X-rays will be a very powerful probe to determine the helimagnetic chirality in chiral magnets.
The existence of the IC magnetic phase and the transformation process into the forced FM state can be examined by magnetization measurements, particularly under an applied magnetic field normal to the helical c-axis. The nontrivial behavior of the magnetization is later described by Eq. (40) and shown in Fig. 39 in the theoretical part (Sect. 5) as well as in the literature.124,125)
In 1965, the downward convex behavior of the magnetization was first calculated by Dzyaloshinskii.16) For CrNb3S6, the magnetic structure was investigated experimentally by small-angle neutron diffraction at zero magnetic field.47) Below
Meanwhile, a steep change in the magnetization toward
Figure 17 shows the magnetization of a CrNb3S6 single crystal when a magnetic field is applied along the helical c-axis. When increasing the magnetic field at a fixed temperature, the magnetization exhibits a linear increase in its magnitude at a small magnetic field followed by a sudden rise toward a certain value of the magnetic field at temperatures below
Figure 17. (Color online) Magnetization curves as a function of magnetic field and temperature. Black arrows in (a) and (b) indicate the positions of kinks and peaks in the M–H and M–T characteristics, respectively. (d) Magnetic phase diagram of CrNb3S6 single crystal based on the magnetization measurement.
Figure 17(d) shows the magnetic phase diagram of the CrNb3S6 single crystal constructed using the magnetization data. It is clear that the locations of the kink structure recognized in the field dependence of the magnetization are smoothly connected with those for the peak found in the temperature dependence. As discussed on the basis of the chiral XY model in the literature,103,124) these anomalies found in the magnetization are ascribed to the critical magnetic field
Detailed features of the magnetic phase diagram for CrNb3S6 have been discussed in several papers. Specific heat measurements were performed around
The CSL couples with conduction electrons and gives rise to nontrivial physical properties. In terms of the magnetotransport, the CSL is a nonlinear array of magnetic soliton kinks, each of which acts as a strong scattering potential for conduction electrons with itinerant spins. Therefore, a nontrivial magnetoresistance (MR) is induced along the helical axis. Moreover, the number of magnetic soliton kinks correlates to the magnitude of the MR.
In CrNb3S6, Cr atoms are in the trivalent state and have localized electrons with spins of
In this subsection, the MR effects in bulk and micrometer-size single crystals of CrNb3S6 are introduced. It is shown that the nature of the MR strongly depends on the dimension of the crystal.
Figure 18 shows the interlayer resistance as a function of temperature at zero magnetic field and the interlayer MR in a bulk CrNb3S6 single crystal. The crystal is the same as that used in the magnetization measurements presented in Fig. 17.
Figure 18. (Color online) (a) Optical micrographs of CrNb3S6 single crystal. For interlayer MR measurements, two electrodes for voltage detection are attached to the
The interlayer resistance clarifies that the phase transition occurs at a temperature of 132 K (
Figure 18(c) presents the interlayer MR examined with field steps of 2 Oe at 110 K. The magnetic field is applied by using a superconducting persistent current mode, so as to prevent the field from overshooting the target value, and kept as constant as possible during the MR measurements. The MR curves measured at 1 and 5 mA coincide with each other, indicating that no Joule heating occurs in this range of current.
The interlayer MR exhibits a rapid reduction toward 1570 Oe at 110 K. This value is consistent with
Above
The contribution of the anisotropic magnetoresistance (AMR) to the interlayer MR is considered as a constant background in these experiments because the spin configuration of the CSL is predominantly oriented within the ab-plane and is thus always perpendicular to the current flow direction along the c-axis.
Figure 19 shows the interlayer MR measured at various temperatures at 5 mA. A negative change in the interlayer MR toward
Figure 19. (Color online) Interlayer MR at 5 mA at various temperatures from 10 to 180 K. A negative MR is observed below
Figure 20 presents a data set of the normalized negative MR curves. All the MR curves almost lie on a single curve and are qualitatively fitted by a theoretical equation of the soliton density
Figure 20. (Color online) Normalized MR curves in the temperature range where a negative MR is observed below
The empirical scaling law of the MR behavior indicates that the magnitude of MR is proportional to the number of magnetic soliton kinks, as naively expected. The change in MR due to CSL formation is noticeable since the magnitude of MR becomes extremely large with the accumulation of magnetic soliton kinks, for example, up to ∼4000 in the present crystal, although the resistance induced by a single magnetic soliton kink is much smaller than the total change in MR.
The CSL is a thermodynamic stable phase. Hence, CSL formation could be identified even when sweeping the temperature instead of the magnetic field, namely, regardless of the sweeping direction in the magnetic phase diagram.
Figure 21 shows the interlayer resistance as a function of temperature at various magnetic fields. A sharp peak in
Figure 21. (Color online) Interlayer resistance as a function of temperature with a current of 5 mA at various magnetic fields. (a) 300 Oe, (b) 900 Oe, (c) 1600 Oe, and (d) 2500 Oe. The sharp peak in
The magnetic phase diagram constructed solely on the basis of the interlayer MR data is presented in Fig. 22(a). Solid squares indicate the onset of the change in the interlayer MR, while other symbols correspond to the locations of anomalies found in the R–T measurements, as described for Fig. 21.
Figure 22. (Color online) Magnetic phase diagram of CrNb3S6. Various kinds of anomalies found in the interlayer MR measurements are given as a function of magnetic field and temperature in (a), while the critical fields identified by the magnetization measurements are shown in (b). Figures adapted from Ref. 25. © 2013 American Physical Society.
To compare the magnetic phase diagram with that obtained by the magnetization measurements, all the data obtained by the interlayer MR and magnetization measurements are plotted in the same magnetic phase diagram in Fig. 22(b). As mentioned before, it has already been reported in the literature that
The interlayer MR due to CSL formation is revealed to correlate to the population of solitons, namely, the soliton density in the bulk CrNb3S6 crystal.25) In this connection, it is interesting to see how the MR changes with the system size.27)
Figure 23 shows the interlayer MR data for a micrometer-size crystal of CrNb3S6. Crystal pieces of typically
Figure 23. (Color online) Interlayer MR data at various temperatures for a micrometer-size crystal of CrNb3S6. (a) Scanning ion micrograph of the crystal with electrodes. (b) MR curves obtained with increasing (red) and decreasing (blue) field at 10 K. The linear dependence above
Hysteresis of the interlayer MR was clearly observed at low temperatures in the micrometer-size CrNb3S6 crystal, as shown in Fig. 23(b). The interlayer MR takes different paths with increasing (red) and decreasing (blue) field. With increasing field, the MR gradually decreases toward a minimum MR value at a saturation field
The values of
Figure 24. (Color online) Interlayer MR of the micrometer-size CrNb3S6 crystal for various angles between the applied field and the specimen plane. The field is kept perpendicular to the helical c-axis. The specimen dimensions are
Many fine steps in the interlayer MR are found at low and high fields both with increasing and decreasing field as shown in Fig. 25, which shows a magnification of the data presented in Fig. 23(b). The steps have many different plateau widths and the magnitude of the jumps varies between 16 and 2060 µΩ. Seven steps, counted from zero field along branches representing the increasing and decreasing field, are found at almost the same MR value irrespective of the swept direction of the field. Steps also appear at higher fields close to
Figure 26 shows the interlayer MR data for a different CrNb3S6 crystal of 25 µm width along the c-axis. All the features observed are consistent with the results obtained for the crystal of 10 µm width along the c-axis presented in Fig. 23. Hysteresis and steps with many different plateau widths appear during CSL formation. The magnitudes of the jumps are integer multiples of
Figure 26. (Color online) Interlayer MR for a different micrometer-size crystal of CrNb3S6. The dimensions of the crystal are
A part of the MR curves obtained for the micrometer-size crystals lies on a single curve, as indicated by a dotted line in Fig. 26(b). This curve follows the behavior of the soliton density curve
Theoretical works129) predict that soliton confinement in a finite-size system induces discrete changes in the soliton period and density along the order parameter of the soliton density curve, which supports the experimental MR data of micrometer-size crystals. The deviation of the MR curve from the ideal soliton density curve is significant at low fields with increasing field and at high fields with decreasing field because of the hysteresis induced in micrometer-size crystals.
Minor hysteresis loops of the interlayer MR are examined for the micrometer-size CrNb3S6 crystal. Two kinds of minor MR loops were measured. The first type of minor loop was measured by the following procedure. The initial state was prepared by increasing the magnetic field from zero field to above
Figure 27. (Color online) Minor hysteresis loop of the interlayer MR in the micrometer-size CrNb3S6 crystal. The measured crystal is the same as that in Fig. 23. The MR data above
The minor MR loops indicate that any point in the hysteresis region can be obtained by the procedure of changing the field, indicating that the number of solitons is tunable in the system. A part of the minor MR loops lies on a single curve as indicated by a dotted line in Figs. 27(b) and 27(d), which qualitatively follows the behavior of the soliton density curve
The interlayer MR curves for temperatures between 10 and 160 K are shown in Fig. 28. Hysteresis appear in the interlayer MR for a wide temperature range below
Figure 28. (Color online) Dependence of interlayer MR on temperature between 10 and 160 K. Figures adapted from Ref. 27. © 2015 American Physical Society.
The interlayer MR varies smoothly for the bulk CrNb3S6 crystal in accord with the calculated soliton density,25) while a part of the interlayer MR curves in the micrometer-size crystal exhibits a similar tendency with dozens of fine MR steps.27) The soliton density plays a role of the order parameter for the continuous IC–C phase transition14,18,21,124,131,132) associated with CSL formation. The observations support the scenario that each soliton creates a spin dependent scattering potential for itinerant spins. At low temperatures, where the scattering path lengths are long, the interlayer MR involves scattering from all the solitons and therefore is used to measure the soliton density. To realize these phenomena, the perfect registry of solitons across the CSL is required. Indeed, at temperatures below 110 K a fine MR structure appears in the form of a sequence of steps along a portion of the branches obtained with increasing and decreasing field in Fig. 28, suggesting that discrete changes in the soliton density are responsible for the stepwise (discretized) changes in MR.
Lorentz TEM contributes to understanding the microscopic nature of the steps and plateaus observed in the interlayer MR curves. Evidence of multiple states of the CSL is observed directly within a grain having reversed crystalline chirality. This is a very interesting example of exchange pinning at a boundary where the DM interaction changes sign.
Analyses of high-resolution DPC micrographs69,71) reveal the spin configuration in a region containing such a grain, as shown in Figs. 29(a)–29(c). A schematic illustration of the obtained spin configuration is given in Fig. 29(d). A magnetic field applied perpendicular to the plane causes magnetic moments to be oriented in the plane near the grain boundary, i.e., perpendicular to the applied field direction. Two
Figure 29. (Color online) Lorentz DPC micrographs of the CSL in a narrow crystal grain of right-handed magnetic chirality sandwiched by wide regions of left-handed magnetic chirality in a magnetic field of 1450 Oe at 100 K. The grain boundaries are indicated by arrows in (a). The contrast and direction of the magnetic moment are schematically presented in (b) and (c). (d) Schematic of the spin configuration of the CSL around boundaries where the magnetic chirality switches. Solitons can be confined between the boundaries. Figures adapted from Ref. 27. © 2015 American Physical Society.
The Lorentz Fresnel micrographs in Fig. 30 clarify that the spin configuration at the boundaries remains the same even at fields above
Figure 30. (Color online) Lorentz Fresnel micrograph, taken under the underfocused condition, at 100 K in a magnetic field of 2270 Oe, above
Figure 31. (Color online) Lorentz Fresnel micrographs of the CSL, taken under the underfocused condition, around a 1-µm-width crystal grain of right-handed magnetic chirality in a magnetic field of 1560 Oe (a), 1771 Oe (b), and 1781 Oe (c) at 100 K. The chiral boundaries and confined right-handed solitons are indicated by red arrows and blue arrowheads, respectively. The number of solitons confined in the right-handed grain is given in (a) to (c). The initial number of confined solitons is 20. Figures adapted from Ref. 27. © 2015 American Physical Society.
Figure 32 provides solid evidence for confinement pinning. Namely, the direct observation of plateaus and stepwise jumps of the soliton period and density is presented for field-strength changes of 1 Oe. In the Lorentz Fresnel microscopy observations, the spacing between contrast lines within the grain remains constant within the experimental resolution independent of the magnetic field within a single plateau. Therefore, it is concluded that the solitons in the region with right-handed magnetic chirality are indeed confined.
Figure 32. (Color online) Soliton period and corresponding soliton density as a function of field, which are measured in a series of Lorentz Fresnel images monitored with steps of 1 Oe during cycling of the magnetic field up to
The original prediction of soliton confinement was made for a system with a very limited number of solitons,129,130,133) in which the solitons were pinned at both edges of a finite-size specimen or thin film. The length of plateau in soliton numbers will increase as the confinement region and the number of solitons involved become smaller, which enables the detection of MR or magnetization anomalies in a MnSi thin film associated with the nucleation or annihilation processes of “two” soliton twists.130)
Here, for crystals with macroscopic length scales, namely, in which tens or hundreds solitons are involved in the confinement, stepwise changes due to single-soliton events are distinguished during the IC–C transition to the forced FM state. Indeed, 20 solitons are confined in the case of the chirality grain shown in Fig. 31 and about 200 solitons are involved for the MR data in Figs. 23 and 25. These findings are consistent with microscopic observations via Lorentz micrographs and small-angle electron scattering data showing that solitons strongly correlate with each other over ten micrometers.21)
In an infinite soliton lattice, the period outside the confined region should change continuously. Outside a grain, the spacing indeed varies continuously with the field strength, such as for the case when 20 or 16 solitons are found in the right-handed grain. However, a sudden increase in the slope is also frequently observed outwith the grain, e.g., as seen at around 1300 and 1900 Oe in Fig. 33. This is consistent with the fact that the soliton lattice is not infinite outside the grain, and is confined over a distance on the order of the macroscopic size. The confinement pinning occurring outwith the grain, namely, between the chiral well and a free edge of the crystal, is over a length scale of 10 and 7 µm.
Figure 33. (Color online) Soliton period as a function of applied magnetic field in three regions. The inset in (a) shows the sample dimensions. Data taken from inside the right-handed grain are given in (red) solid squares, while (magenta) open circles and (dark blue) solid circles are used to exhibit data taken from inside the left-handed grains on the left and right, respectively. Figures adapted from Ref. 27. © 2015 American Physical Society.
The length scales over which distinct plateaus are observed are striking. This requires a high degree of coherence of the CSL in order that the CSL at the separate edges works cooperatively to allow the escape or injection of a single soliton. The pinning mechanism in operation for the confinement in the 1 µm grain probably differs from the pinning that must occur at free edges, as observed in the 10 µm samples, but nevertheless confinement occurs in each situation. Single soliton changes are observed even in finite-size MR samples at high fields where the soliton density is smallest. This is consistent with single soliton decrease in the chirality grain throughout the increasing field branch, thereby reflecting the long-range coherence of the CSL. However, the spacing of the CSL becomes slightly irregular at high fields close to
Soliton confinement and consequent discretization effects occur, depending on the system size. Figure 34 shows how the CSL changes the number of solitons in the chirality grains with widths of about 500 nm, 1 µm, and 1.5 µm, which initially contains 10, 20, and 32 confined solitons, respectively. With increasing the number of initial solitons in the chirality grains, the curve of the normalized soliton number shifts towards a lower field and approaches the ideal soliton density curve given by the dashed curve in Fig. 34(b). Similar behavior is found in micrometer-size crystals, as presented in Figs. 26 and 27, and bulk crystals, as shown in Fig. 18, indicating that TEM and MR data have the same origin of the soliton confinement and discretization effects. Figure 35 summarizes how discretization or quantization effects become prominent depending on the initial soliton number.
Figure 34. (Color online) Normalized soliton number as a function of normalized field in TEM specimens with chirality grains of different widths with increasing field. Square (red), triangle (purple), and circle (green) dots represent data for 1.5-µm-wide, 1-µm-wide, and 500-nm-wide chirality grains, which initially contain 32, 20, and 10 confined solitons, respectively. Figures adapted from Ref. 27. © 2015 American Physical Society.
Figure 35. (Color online) System size dependence of MR and soliton density. With reducing initial number of solitons in the system, discretization (quantization) effects become prominent.
From a technological viewpoint, the confinement discretizes the soliton density, thereby enabling the use of solitons as individual and countable objects. More practically, counting the number of solitons via electric measurements can be accomplished with relative ease, which allows us to exploit the discreteness of the soliton density for data storage applications.
In this section, we present a summary of the underlying theory of the CSL.
The possible microscopic origins of the DM interaction are briefly summarized in this subsection. Chiral magnetic crystals are classified into three classes: magnetic insulators, metals where localized and itinerant spins coexist, and metals with only itinerant spins.
The first class corresponds to the case originally discussed by Moriya.17) The Hamiltonian which describes two magnetic ions is
In the second case, the particle–hole fluctuations of the itinerant electrons mediate the DM interaction between the localized spins. This corresponds to a generalized Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction. In this case, the crystal symmetry is embedded in the complex one-particle hopping, and the resultant DM interaction should appropriately reflect the crystal symmetry.134) CrNb3S6 and YbNi3Al9 belong to this category.
The third case is the most nontrivial.135) It is expected that after integrating out the one-particle degrees of freedom with spin–orbit coupling being treated as a perturbation, a coupling of the spin fluctuations eventually has the effective form of the DM interaction.136) B20 compounds such as MnSi, FeGe, and Fe
The CHM structure is an incommensurate magnetic structure with a single propagation vector. The magnetic structure is specified by the symmetry-adapted 2-D basis
The chiral space group
For the real 2-D (or complex 1-D) symmetry-adapted basis
Figure 36. (Color online) For a CHM ordering to be realized, the crystal point group needs to have 2-D (or complex 1-D) irreducible representations. This means the point group elements must have a threefold (
A necessary condition for the monoaxial DM vector to exist is that a magnetic crystal belongs to a chiral space group
The most prominent feature of the LI is its ability to stabilize discommensuration in a background incommensurate helical structure. The LI-induced discommensuration has a topological texture protected by crystal chirality. In the pioneering work by Dzyaloshinskii,14–16) it was shown that in the case of
|
As an example, we consider the point group
Figure 37. Stereographic projections to illustrate the structure of the point group
From now on, as a canonical example of a monoaxial chiral helimagnet, we consider the case of CrNb3S6. The most prominent feature of this compound is its classical 1-D nature as a magnetic system, i.e., 2-D layered magnetic structures are weakly coupled via the interlayer exchange and DM interactions. Then, the system is well described as a classical 1-D chiral helimagnet.
Recently, Shinozaki et al.143) have applied a hybrid method called the 2dMC-1dMF method to take account of the spin correlation effect in the layer and they estimated the transition temperature. Consequently, the three interaction parameters in CrNb3S6 were estimated as the interlayer DM interaction strength
In the following discussion, we consider only the ground state at zero temperature. Taking the limit as
Furthermore, the spatial modulation of the magnetic structure,
The ground state of the model in Eq. (23) was first given by Dzyaloshinskii16) in the magnetic system, followed by de Gennes131) in the context of the magnetic-field-induced transition in a cholesteric liquid crystal. Variational analysis gives the stationary configuration of the φ field, which is given by
In Fig. 38(a), we show the spatial distribution of
Figure 38. (Color online) (a) Spatial distributions of the phase
Using
In this state, the elliptic modulus κ is simply a constant of integral. Its value is determined by minimizing the energy with respect to κ. By noting that
A set of Eqs. (34) and (36) gives the field dependence of
The magnetization averaged over the spatial period is given by
Figure 39. Magnetization curve of the CSL state.
Here we mention the stability of the CSL in the magnetic field plane formed by the components parallel and perpendicular to the helical axis. It was recently found145) that for field directions almost parallel or perpendicular to the helical axis, the transition from the incommensurate CSL to the commensurate forced-FM state is continuous, while for intermediate angles the transition is discontinuous and the IC and C states coexist on the transition line.
In the previous subsection, we considered the CSL in an infinite system. Now, it is natural to search for a confinement effect in a finite system, where spins on both ends are fixed. In Ref. 129, it was found by numerical analysis that in the case of
Using Eq. (32), we obtain the total energy
Figure 40. (Color online) (a) Total energy of confined CSLs given by Eq. (42) as functions of h for
The CSL exhibits rich dynamical properties. First, the whole CSL system behaves as an elastic crystal lattice that consists of solitons, as shown in Fig. 41(a). The phonon-like excitations (CSL phonon) of the scalar sine-Gordon soliton lattice were first studied by Sutherland,146) and the case of a CSL was discussed in Refs. 23 and 147. He pointed out that the phonon mode obeys the Lamé equation of the Jacobi form108) as discussed below. Note that oscillations around individual solitons highly correlate with each other via the long-range interaction, which decays in an exponential manner at large distances. The CSL phonon is a direct manifestation of broken translational symmetry.
Figure 41. (Color online) Dynamical motion associated with the CSL state. (a) Phonon-like excitations around the CSL, which correspond to the Goldstone mode associated with the translational symmetry breaking. (b) Collective translation of the whole CSL.
Second, because of broken Galilean symmetry, the CSL exhibits collective sliding motion, i.e., the whole CSL is translated in a coherent manner, as shown in Fig. 41(b). This motion corresponds to the Galilean boost of the CSL,148) and its physical consequences were discussed in Ref. 26. In this subsection, we discuss the CSL phonon, and the coherent sliding will be discussed in the next subsection. Note that there is an isolated soliton which surfs over the background CSL,149) which we do not discuss in this review.
We consider dynamical fluctuations around the stationary soliton lattice configuration,
Figure 42. (Color online)
By expanding the Hamiltonian
Figure 43. Spatial profile of
We see that the soliton parts contribute to the gap formation, while the forced-FM (commensurate) domains do not. For an arbitrary value of
In the region where the approximation (50) is valid, the eigenvalue equations
The φ-mode spectrum,
I. Valence band: The valence band is specified by
We obtain the energy spectrum of the φ and θ fluctuations, which are depicted in Figs. 44(a) and 44(b), respectively. Here it should be noted that in the description of the φ-mode, we consider the fluctuations around the spatially modulating configuration
Figure 44. (Color online) Schematic landscape of the energy spectra for (a) φ and (b) θ fluctuations. In (c) and (d), we depict snapshots of the spatial distribution of the φ fluctuation corresponding to the band top [white circle indicated in (a)] and the zero mode [black circle indicated in (a)].
II. Conduction band: The conduction band is specified by
The normalized wave function at the bottom (
Using the orthonormal basis
We consider spin resonance in the CSL state, where, in addition to the static magnetic field to stabilize the CSL, a uniform rf field is applied parallel to the helical z-axis. In this case, the rf field couples with
For the valence band (
The first Brillouin zone of the CSL is
In Fig. 45(a), we schematically depict the distribution of the resonance energy levels, which become more dense upon increasing the magnetic field strength. In Fig. 45(b), we show the resonance frequencies
Figure 45. Energy dispersion of the CSL phonon in the reduced zone scheme for (a-1) smaller and (a-2) larger magnetic field strengths. The vertical broken lines indicate the Brillouin zone boundaries
Next we consider the sliding motion of the CSL [Fig. 41(b)]. In the continuum limit, the soliton lattice has continuous degeneracy related to the choice of the center of mass position, i.e.,
Figure 46.
Because the φ-mode is gapless, there is no excess energy associated with
Next we construct a Lagrangian for the collective dynamics. The kinetic (Berry phase) term is written as
Using the expansion (72) and the relation
Now that we have obtained the Lagrangian (79), we consider how to trigger the sliding motion. As pointed out in Ref. 26, the sliding is caused via the spin-torque transfer from the itinerant quantum spins to the localized magnetic moments which form the CSL. More directly, the sliding motion of the CSL is caused by applying a time-dependent magnetic field parallel to the helical axis.152) Here we briefly present the latter case.
The Zeeman coupling of the CSL with
A general form of the Euler–Lagrange–Rayleigh equation of motion for a generalized coordinate q is given by
The relaxation of the soliton lattice is caused by the Gilbert damping and its intrinsic relaxation time is expressed by
Next, let us consider a typical case of an AC field,
Figure 47. Time dependences of (a) longitudinal field
The CSL, being protected by the broken chiral symmetry, possesses a robust coherence. Owing to this circumstance, the CSL behaves as a coherent single domain, which can be referred to as a giant deformable body. Then it is natural to investigate its dynamics under a confinement potential caused by pinning. Within the small amplitude approximation, the confined dynamics reduces to a small oscillation under a nonlinear potential and resonant dynamics is expected to occur. The non-linearity stems from the nonlinear structure of the CSL.
To model the boundary pinning, we introduce the boundary pinning field
Now, we consider the energy cost associated with the shift of Z. In the analytical approach presented in this section, we assume weak pinning and that the spatial profile of φ simply causes a parallel translation. The variable
Provided that the displacement
To estimate the quantities, we choose
Because the sliding motion of the CSL accompanies the dynamical deformation of the spin texture, we naturally expect a spin motive force (SMF) to occur152) and to be strongly amplified in the configuration presented in Fig. 48. The external pinning may be realized by attaching FM bars on both sides of the monoaxial chiral helimagnet. The effective electric field that acts when the conduction electrons are adiabatically subjected to a spatially modulated spin structure along the z-axis has the form153)
Figure 48. (Color online) Schematic picture of amplification of the spin motive force by the resonant oscillation of the weakly pinned CSL.
Substituting the linear solution, (86), into Eq. (48), we obtain the SMF at the resonance frequency
In this review, we have presented experimental and theoretical overviews on (monoaxial) chiral helimagnets and the chiral spin soliton lattice unique to these systems. Starting from the strategy for synthesizing chiral magnetic materials, the static and dynamical properties of the CSL including the consequent nontrivial MR and quantization effects are given together with the underlying physical mechanisms from theoretical viewpoints. In this final section, future perspectives from more general viewpoints are discussed.
As seen in the previous sections, one of the surprising characteristics of the CSL is the robust phase coherence at the macroscopic length scale. Indeed, the spin states of the CSL and their observed behavior are direct consequences of an orientational coherence extending over macroscopic distances across huge numbers of magnetic spins.
The CSL with long-range coherence poses several intriguing and unanswered questions. It has so far only been found in a particular class of monoaxial chiral helimagnets, but could be realized and function in other chiral systems such as chiral nematic liquid crystals. In tetragonal, hexagonal, and trigonal systems, there is only one principal crystal axis and consequently the crystal symmetry allows the existence of only one helical axis. These three crystal classes can support a robust CSL structure.
There is an interesting analogy to the notion of generalized thermodynamic rigidity associated with the long-range order in condensed matter physics. In some systems, the rigidity is characterized with reference to a phase, as in the cases of superfluidity and superconductivity. The magnetic order parameter of the CSL is represented by
We summarize this analogy among light, charge, and spin in terms of phase coherence. Figure 49 shows the coherent and incoherent states of each property. For the light, a laser and normal light are the coherent and incoherent states of the light, respectively. For the charge, the former is superconductivity, while the latter is the electronic state in normal metals or semiconductors. For the spin, the CSL in chiral helimagnets is the macroscopic spin order with phase coherence, whereas magnetic domains in ferromagnetic materials correspond to the incoherent state. The research activities on lasers and superconductivity have been important for many decades and provided novel concepts in electronics and generated various kinds of novel device applications. In this respect, it may be expected that chiral magnetism can also innovate the concept of phenomena related to spin electronics as well as information processing technology. This new research field may be called “spin phase electronics” because it benefits from the control and manipulation of spin phase coherence in chiral spin orders.
Figure 49. (Color online) Coherent and incoherent states of light, charge, and spin.
Acknowledgments
We would like to thank the following scientists for fruitful discussions: A. S. Ovchinnikov, I. G. Bostrem, and Vl. E. Sinitsyn of Ural federal University; T. Koyama, K. Harada, and S. Mori of Osaka Prefecture University; S. McVitie, D. McGrouther, D. MacLaren, and R. L. Stamps of University of Glasgow; A. Leonov and A. N. Bogdanov of IFW Dresden; M. Mito of Kyushu Institute of Technology; Y. Kato, Y. Masaki, and M. Shinozaki of University of Tokyo; and I. Proskurin, F. Goncalves, S. Nishihara, and J. Akimitsu of Hiroshima University. We sincerely appreciate enlightening discussions with T. Ogawa of Kyoto University through the lectures on the philosophy of the concept of chirality. We acknowledge support from JSPS Grants-in-Aid for Scientific Research (Grant Numbers 25220803, 25600103, 25287087, 26400368, 15H03680, and 15H05885), the JSPS Brain Circulation Project (R2507), the JSPS Core-to-Core Program “Advanced Research Networks”, the JST Program of PRESTO, the NanoSquare program in Osaka Prefecture University, and the MEXT Program for Promoting the Enhancement of Research Universities (Hiroshima University).
We give a brief introduction to the Lamé equation, which describes the elementary excitations of the CSL. The Jacobi form of the Lamé equation is
Then Eq. (A·3) is rewritten as
Requiring
Figure A·1. (a) Two branches of the parameter α, which labels the propagating solution of the Lamé equation, and (b) the corresponding spectrum.
Then, the spectrum covers the region
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Author Biographies
Yoshihiko Togawa was born in Hyogo, Japan in 1974. He obtained his B.Eng (1997), M.Eng (1999), Ph.D (2002) degrees from the University of Tokyo. He was a JSPS research fellow at the University of Tokyo (1999–2002), and a researcher at Frontier Research System, RIKEN (2002–2008). In 2009, he moved to Osaka Prefecture University as a special lecturer and principle investigator in the tenure-track program, and became a special associate professor in 2012. Since 2014, he has been a associate professor with tenure at Department of Physics and Electronics, Osaka Prefecture University. He has also been PRESTO researcher at Japan Science and Technology Agency since 2013, and a honorary research fellow at the University of Glasgow since 2014. He has been working on experimental studies on various topics of condensed matter physics, in particular, the dynamics of quantum condensates with many degrees of freedom including visualization of structures and dynamics of superconducting vortices, magnetic domains, and chiral magnetic orders using electron microscopy. His current research interest is the exploration of spin phase electronics using chiral magnetism and electron physics using electron beams.
Yusuke Kousaka was born in Aichi, Japan in 1979. He obtained his B.Sc (2003), M.Sc (2005), D.Sc (2009) degrees from Aoyama Gakuin University. He was a postdoctoral research fellow at Aoyama Gakuin University (2009–2014). Since 2014, he has been an assistant professor at Hiroshima University. He has worked on synthesis of novel compounds and crystal growth of large and high-quality crystals in strongly correlated electron systems including chiral inorganic magnetic materials. He also has expertise in analysis of crystalline and magnetic structures using neutron and X-ray beams. His current research interest is homochiral crystal growth of inorganic compounds.
Katsuya Inoue was born in Saga in 1964. He obtained his D.Sc. (1993) degree from the University of Tokyo. He became a JSPS research fellow in 1992 (DC), 1993–1994 (PD), and got position of a Lecturer in the Kitasato University in 1994.4. In 1996.1 he moved to Institute for Molecular Science (IMS) as an Associate Professor. He has been Professor in Hiroshima University since 2004. Since 2014, he has also been working at Center for Chiral Science in Hiroshima University as Director. In 2015, he was awarded a Distinguished Professor, Hiroshima University. His main topic is the development of novel functional magnets.
Jun-ichiro Kishine was born in Kyoto, Japan in 1967. He obtained his B.Sc. (1991) degree from Tokyo University of Science, and M.Sc. (1993), and D.Sc. (1996) degrees from the University of Tokyo. He was a research associate (1996–2003) in Institute for Molecular Science. During this period, he was a visiting scientist in Massachusetts Institute of Technology as a Monbusho Overseas Research Fellow. Then, he moved to Kyushu Institute of Technology as an associate professor (2003–2012). Since 2012, he has been a professor in the Open University of Japan. He has worked on theory of condensed matter physics such as superconductivity and magnetism in strongly correlated electron systems, quasi-one-dimensional systems and other systems. His current research interest is chiral symmetry breaking in materials and its physical outcome.
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