Quantum interference in density wave systems

When hearing “pi-phase” and “quantum oscillations”, would you immediately jump to Berry phase? In a recent collaborative work, we have shown that a new kind of “pi-phase shift”, i.e., that between quantum oscillations in longitudinal resistivities along orthogonal directions, in the prototypical spin density wave material Cr, is caused by quantum interference effects between coupled semiclassical orbits. For an in-depth introduction, see this note which was a presentation given at the “Magneticians’ meeting” at Johns Hopkins University in 2023.

Y. Feng, Y. Wang, T. F. Rosenbaum, P. B. Littlewood, and H. Chen, “Quantum interference in superposed lattices”, Proc. Natl. Acad. Sci. 121, e2315787121 (2024).

Unexpected symmetry in kagome spin ice revealed by electrical transport

Since the original proposal by Anderson on spin liquid being a possible mechanism for high-Tc superconductivity, electrical transport in frustrated quantum spin systems has always been one of the most enticing topics in condensed matter physics. However, a majority of quantum spin ice and spin liquid candidates are good insulators, making it challenging for standard electrical transport techniques. In contrast, in the few cases of metallic frustrated spin systems, transport experiments usually lead to surprising discoveries.

In this collaborative work, through electrical transport experiments on a recently identified metallic kagome spin ice compound HoAgGe, we made another surprising discovery: There exists a time-reversal-like degeneracy for certain noncollinear ice-rule states on field-induced magnetic plateaus, which have the same energy and magnetization, but different sizes of the anomalous Hall effect (AHE). Since the AHE transforms as a pseudovector with fixed length under all magnetic group operations, the symmetry operation underlying such a degeneracy is beyond the standard paradigm of magnetic space group for classifying magnetic structures.

Through comprehensive neutron refinement and numerical search in the degenerate ice-rule manifold, we are able to nail down the spin structures of the degenerate states and to come up with a microscopic model for calculating their transport properties. Again surprisingly, we find that the degenerate spin structures have exactly the same band structure, but different Berry curvatures in momentum space, and hence different sizes of the anomalous Hall effect. Although the Berry curvature is more related to the geometric properties of the Bloch wavefunctions than to the eigenenergies, it is hard to imagine without seeing that real physical systems with identical band structures can have different Berry curvatures.

Our systematic experimental and theoretical efforts elucidated the rather subtle symmetry operation that connects the degenerate states, which critically relies on a reversal of lattice distortion in the structure of HoAgGe. Since the Berry connection inherently depends on the atomic location in a unit cell, while the latter is largely invisible to the momentum space Hamiltonian, the distortion reversal in such a quasi-symmetry operation eventually changes the size of the AHE but not the band structure.

Our work is built upon the active research in the topical areas of quantum spin ice systems and anomalous transport in noncollinear antiferromagnets, but advances these fields by cross-disciplinary findings that crucially require ingredients from both: The massive ground state degeneracy of frustrated spin systems provides a reservoir for novel noncollinear spin configurations that host characteristic anomalous transport properties. Our work also points to the special role of lattice distortion and distortion reversal in quantum spin systems. In particular, our theoretical analysis indicates that similar phenomena should generally occur in quantum spin systems with nontrivial lattice distortion and relatively weak spin-orbit coupling.

Transporting the shape of spin

Spintronics exploits the idea of using electron spin instead of charge to encode and process information. But can electrons carry more than just spin across diverse materials? Our work answers with a resounding yes, unveiling the transport of spin “shape” in solids. The word “shape” means how spin is distributed spatially about the center of mass of a single electron wave packet. In practice it can be described by the multipole moments of spin distributions. We have isolated the part of such multipole moments that does not depend on how the wave packets are constructed, thus having an absolute meaning. Similar to spin, the well-defined spin or magnetic multipole moments can then be transported by electrons driven by external fields. As one example, we showed that an electric current flowing through phosphorene subjected to a perpendicular electric field can generate magnetic octupole moments. Such octupole moments are manifested by accumulation of spins with alternating signs at square sample corners, as illustrated in the figure below. Our work propels the emergence of “multipoletronics,” a promising new phase beyond spintronics.

A wave packet carrying magnetic octupole moments and the corresponding corner spin pattern in monolayer phosphorene.

Muhammad Tahir and Hua Chen, Transport of Spin Magnetic Multipole Moments Carried by Bloch Quasiparticles, Phys. Rev. Lett. 131, 106701 (2023).

From spintronics to multipoletronics: How CSU research could allow for big developments in data processing (CSU SOURCE)

An alternative to magnetization

In the ordinary Hall effect, it is the magnetic field that tells which way the electric currents driven by a voltage bias should be deflected, simply through the Lorentz force. In a ferromagnetic conductor, it is the direction of the magnetization that determines that of the transverse anomalous Hall current flow, despite the more complicated microscopic mechanisms. However, for antiferromagnets when the magnetization vanishes but the anomalous Hall effect does not, how can the electrons know which way they should be deflected? In this work we answered this question by introducing a new quantity named as electronic chiralization (EC), that is determined by the spatial gradients of the microscopic magnetization rather than its mean. EC transforms in exactly the same way as the anomalous Hall vector under all space group operations, including continuous translation, and is free from the difficulties of defining multipole moments of infinite systems. Moreover, EC provides intuitive guidance for the search of new unconventional magnetic systems hosting the AHE as it suggests what types of spin and charge textures are necessary for the AHE. To demonstrate this we provided two novel, experimentally relevant examples: charge-ordered kagome spin ice, and 2D Dirac electrons skew-scattered by a magnetic charge texture. The former may solve the puzzle of the experimentally observed AHE in certain frustrated spin systems that lack long-range magnetic dipole order, while the latter demonstrates another paradigm of noncollinear magnetic textures, magnetic charge or monopole, that can give rise to the AHE, in contrast to the well-known scalar spin chirality and skyrmions.

Electronic chiralization as an indicator of the anomalous Hall effect in unconventional magnetic systems
Hua Chen, Phys. Rev. B 106, 024421 (2022).

Realization of kagome spin ice in an intermetallic compound

Spin ices are exotic phases of matter characterized by frustrated spins obeying local “ice rules,” in analogy with the electric dipoles in water ice. Namely, on a tetrahedron with one spin or electric dipole moment sitting on each vertex, only the two-in-two-out configurations are allowed. Such a local constraint can lead to a macroscopic number of degenerate ground states or an extensive ground state entropy, which was first calculated by Pauling for water ice. In two dimensions, one can similarly define ice rules for in-plane Ising-like spins arranged on a kagome lattice, so that only one-in-two-out or two-in-one-out configurations are allowed. Such ice rules can result from either nearest neighbor ferromagnetic exchange coupling or long-range dipolar coupling between the spins, which can lead to different multi-stage ordering behavior under changing temperature. However, there have been very few materials systems that can be described as kagome spin ice.


In a recent Research Article published in Science [1], a multi-national team involving two CSU Physics faculty members Hua Chen and Kate Ross demonstrated that an intermetallic compound HoAgGe is a realization of the kagome ice state. Through experimental and theoretical approaches including magnetometry, thermodynamic measurements, neutron scattering, and Monte Carlo simulations, they have established that the low-temperature (<15K) spin states of the system can be reasonably well captured by a classical spin model hosting the kagome ice physics. The relatively high temperatures at which the spin ice behavior appears, in comparison with that in conventional 3D spin ices, are mainly due to the metallic nature of the system, which allows strong RKKY interaction between local Ho moments mediated by conduction electrons. The coexisting metallicity and spin ice phenomena may lead to other exotic physics such as interaction between electric currents and effective magnetic monopoles that deserves future study.

[1] Kan Zhao*, Hao Deng*, Hua Chen*, Kate A. Ross, Vaclav Petříček, Gerrit Günther, Margarita Russina, Vladimir Hutanu, and Philipp Gegenwart, “Realization of the kagome spin ice state in a frustrated intermetallic compound”, Science 367, 1218-1223 (2020).

Geometric Dynamics of Magnetization: Electronic Contribution

Magnetization dynamics has been routinely studied using the Landau-Lifshitz-Gilbert (LLG) equation. Although the LLG equation has a quantum mechanical origin and reflects the fact that magnetization and angular momentum of electrons are really the same thing, it has been used most of the time as a classical equation. The reason for it is that magnetism can be viewed as a condensate of the underlying quantum mechanical degrees of freedom, through which their wavefunctions become an identical macroscopic quantity and acquire the physical meaning of the order parameter, similar to the reason why light is formed by photons but one can still describe it classically in daily life.

However, in certain cases the quantum mechanical nature of the underlying electrons contributing to the magnetism can still manifest in the magnetization dynamics. In a recent paper by Bangguo Xiong, Xiao Li, and Qian Niu (UT Austin) and Hua Chen (CSU), we have given examples of such nontrivial modifications to the classical LLG equation due to the coupling between the magnetization and the microscopic electronic degrees of freedom [1]. The theory is based on the semiclassical wavepacket approach, which captures the slow, long-wavelength dynamics of electrons in a solid by constructing wavepackets which respond to electromagnetic fields as classical point-like objects. There are, however, remnant quantum effects appearing in their equations of motion through the so-called Berry curvatures. We find that in the absence of external fields the gyromagnetic ratio appearing in the LLG equation acquires an additional correction inversely proportional to one kind of Berry curvatures of the electrons. In the presence of an electric field, we find that the electric field modifies the “effective magnetic field” coupled to the magnetization, the gyromagnetic ratio, as well as the damping in the LLG equations. Electric field (or current) effects on magnetization dynamics are usually described as spin-orbit torques in the spintronics community, which are conventionally calculated as the linear response of spin density to electric fields. However, our theory points out that such an approach misses some important contributions to the magnetization dynamics that are due to the dynamical coupling between the magnetization and the electrons. One interesting example of such new contributions, due to the modification to the damping term, is that a current may turn a hard axis of the magnetization into an easy axis and offer a new scenario for electrically-induced magnetic switching. Such an effect is demonstrated using a model of ferromagnet/topological insulator bilayer.

 

[1] Bangguo Xiong, Hua Chen, Xiao Li, and Qian Niu, “Geometric Dynamics of Magnetization: Electronic Contribution”, Phys. Rev. B 98, 035123 (2018)

Electrical switching of the topological anomalous Hall effect in a non-collinear antiferromagnet above room temperature

First discovered by Edwin Hall in 1881, the anomalous Hall effect describes the transverse flow of electric currents under a longitudinal electric field in a ferromagnetic metal with its magnetization perpendicular to the measurement plane. By flipping the magnetization direction of the ferromagnet the transverse current also changes sign. The behavior looks similar to electrons moving under the Lorentz force of a pair of orthogonal electric and magnetic fields, but the most interesting fact about the anomalous Hall effect is that it is definitely not due to the Lorentz force, since it exists even when the external magnetic field is zero, and the dipole field due to the magnetization is orders of magnitude too weak to explain it.

A century-long expedition in both experiment and theory has finally led us to a comprehensive microscopic understanding of the origin of the anomalous Hall effect. Basically it involves several contributions (intrinsic, skew scattering, and side jump), all having to do with time-reversal symmetry breaking (i.e. the material must be magnetic), and spin-orbit coupling (i.e. motion of an electron is correlated with its spin state). A quantized version of the anomalous Hall effect was predicted by the 2016 Nobel laureate F.D.M. Haldane and was experimentally verified in 2014. The geometric understanding of the quantum Hall effect (by another Nobel laureate of 2016, David Thouless) as well as the quantum anomalous Hall effect, basically paves the way to the booming topological phenomena in modern condensed matter physics.

However, just when people started to think that the anomalous Hall effect was almost fully understood, new surprises came. In 2014 together with Qian Niu and Allan MacDonald at UT Austin, we theoretically predicted that there can be large anomalous Hall effect in certain antiferromagnets, in which the total magnetization vanishes [1]. The reason why this was surprising is that it had been a conventional wisdom that the anomalous Hall effect is proportional to the net magnetization, and therefore should be zero in antiferromagnets. However, the understanding of the symmetry properties of the anomalous Hall effect gives a rather convincing argument that our prediction must be true, and the conventional wisdom is incorrect. In the original PRL we predicted the noncollinear antiferromagnets Mn3Ir, Mn3Pt, and Mn3Rh, which have cubic structures, to be such “anomalous Hall antiferromagnets”. In 2015 a beautiful experiment was done by the group of Satoru Nakatsuji at the University of Tokyo, where a large anomalous Hall effect at room temperature was measured in a closely related material, Mn3Sn, which has a hexagonal symmetry [2]. Subsequent experimental and theoretical works have demonstrated more interesting properties related to the anomalous Hall effect in the antiferromagnets family, including the magneto-optic Kerr effect, anomalous Nernst effect, Weyl fermions in the band structure, etc.

In a most recent paper published in Nature Electronics [3], a team formed by Prof. Zhi-Qi Liu at Beihang University and his colleagues on the experiment side, and Hua Chen (CSU) and Allan MacDonald (UT Austin) on the theory side, have successfully demonstrated the anomalous Hall effect in Mn3Pt, one of the first cubic anomalous Hall antiferromagnets predicted in our 2014 paper. The experimental team has successfully grown high-quality thin films of Mn3Pt epitaxially on a substrate of the ferroelectric material BaTiO3, and have measured its anomalous Hall effect. What is more intriguing is that Mn3Pt has a strange phase transition at about 360K, between a low-temperature noncollinear antiferromagnetic phase, and a high-temperature collinear antiferromagnetic phase, but only the former can have the anomalous Hall effect because of symmetry. The ferroelectric BaTiO3 substrate further makes it possible to slightly change the transition temperature through piezoelectric strain when an external electric field is applied. Thus by keeping the temperature constant, the Mn3Pt can be switched between the noncollinear and the collinear phases by electric fields, and the anomalous Hall effect is switched on and off accordingly. This is the first time that electric switching of the anomalous Hall effect is realized in an antiferromagnet and may lead to fancy device concepts in future electronics and spintronics.

 

[1] Hua Chen, Qian Niu, and Allan H. MacDonald, “Anomalous Hall effect arising from noncollinear antiferromagnetism”, Phys. Rev. Lett. 112, 017205 (2014).

[2] Satoru Nakatsuji, Naoki Kiyohara, and Tomoya Higo, “Large anomalous Hall effect in a non-collinear antiferromagnet at room temperature”, Nature 527, 212 (2015).

[3] Z. Q. Liu, Hua Chen, J. M. Wang, J. H. Liu, K. Wang, Z. X. Feng, H. Yan, X. R. Wang, C. B. Jiang, J. M. D. Coey, and A. H. MacDonald, “Electrical switching of the topological anomalous Hall effect in a non-collinear antiferromagnet above room temperature”, Nature Electronics, 1, 172-177 (2018).