arXiv subjects

Mingqiang Gu

Publications and source records attributed to Mingqiang Gu.

At least 19 recordsLinked to original sources

arXiv2026

Coupling Chirality, Polar Order, and Altermagnetic Spin Splitting in a Hybrid Manganese Chloride

Hybrid manganese halides enable the coexistence of molecular chirality, polar order, and magnetic exchange within a single lattice. Here, we combine first-principles calculations with spin-space-group analysis to investigate the synthesized enantiomeric pair [(R)/(S)-MPA]2[MnCl4(H2O)] (MPA = beta-methylphenethylammonium). We predict that its compensated magnetic state hosts altermagnetic spin splitting in the nonrelativistic limit, and that the coupled chiral, polar, and magnetic degrees of freedom define a symmetry-related manifold. From this manifold, we derive simple sign rules for the electronic and magneto-optical response: reversing both chirality and polarity, or reversing the magnetic domain alone, inverts the spin splitting throughout the Brillouin zone, whereas reversing chirality alone or polarity alone changes the spin-splitting sign only in symmetry-selected regions. With spin-orbit coupling, reversing chirality or magnetic order flips the Kerr rotation angle, while changing the polar variant leaves it unchanged. These results reveal a chemically accessible route to translate molecular handedness into symmetry-controlled spin splitting and magneto-optical readout in hybrid manganese halides. Critically, we show that the sign and momentum pattern of the splitting are governed by the interplay of the chiral, polar, and magnetic degrees of freedom. This interplay opens the possibility to control the spin splitting through a judicious design of the organic cations, by modulating their chirality and polarity.

cond-mat.mtrl-sci↗

arXiv2026

Excitations across the equilibrium and photoinduced `hidden' states of magnetoresistive manganites

"Hidden" phases, generated using ultrafast laser pulses (few hundred femtoseconds), with properties distinct from thermodynamic equilibrium, are appealing for technologies because they can be long-lived, with lifetimes of hours or weeks, and reversible with temperature sweeping or extra pulses. In this regard, La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LCMO) stands out due to its tunability through epitaxial strain, which can drive the bulk ferromagnetic metal (FMM) into an antiferromagnetic insulator (AFI), and its susceptibility to photo-induced transitions. Indeed, AFI LCMO displays a long-lived photo-induced transition into a putative 'hidden' phase whose exact nature and excitations are still largely unknown. Here, we combine ultrafast photo-excitation in the near infrared with in situ transport, x-ray absorption (XAS), and Resonant Inelastic X-ray Scattering (RIXS) to investigate the excitations (polarons, phonons, and orbital) of the photo-excited phase of LCMO and contrast them with the thermodynamic phases achieved through strain and temperature. In the thermodynamic regime, we establish the correlation between polarons and transport, placing them in the 'strong coupling' regime of the Holstein model. Upon photo-excitation of LCMO-AFI, we uncover a long-lived phase characterized by the softening of the polaron excitations, the partial suppression of the Jahn-Teller distortion, and nearly unchanged phonons, showing the emergence of a photo-excited state absent in the equilibrium phase diagram. Finally, by varying temperature, epitaxial strain, and photo-excitation fluence, we construct a polaron phase diagram and identify the key spectroscopic signatures of each phase. Our laser-RIXS approach establishes a versatile platform for exploring photo-induced 'hidden' phases in quantum materials in non-stroboscopic conditions.

cond-mat.str-el↗

arXiv2025

Magnetic order dependent photoluminescence from high energy excitons in hBN protected few-layer CrSBr

The detection and manipulation of the spin configurations in layered magnetic semiconductors hold significant interest for developing spintronic devices in two-dimensional limit. In this letter, we report a systematical study on the photoluminescence (PL) from the high energy excitons in few-layer CrSBr and its application on detecting the spin configurations. Besides the broad excitonic emission peak (Xl) at around 1.34 eV, we also observed another strong excitonic emission peak (Xh) at around 1.37 eV in hBN encapsulated 2L sample, which splits into two peaks in 3L and 4L samples. With help of the first principles calculations, we conclude that the Xh peak is associated with the transition between the top valence band and the second lowest conduction band, which is forbidden by the inversion symmetry in 1L CrSBr. Furthermore, the position and intensity of the Xh peak are strongly dependent on the interlayer magnetic order of the CrSBr samples, which provides an efficient way to probe their spin configurations. In addition, when the magnetic field is applied at the easy axis direction, we resolve an intermediate magnetic state besides the antiferromagnetic and ferromagnetic states in 3L and 4L samples. Our results reveal few-layer CrSBr as an ideal platform to study the interaction between the excitons and magnetism.

cond-mat.mes-hall↗

arXiv2025

Topotactic Reduction-Driven Crystal Field Excitations in Brownmillerite Manganite Thin Films

Topotactic reduction of perovskite oxides offers a powerful approach for discovering novel phenomena, such as superconducting infinite-layer nickelates and polar metallicity, and is commonly accompanied by the emergence of multiple valence states and/or complex crystal fields of transition metals. However, understanding the complex interplay between crystal chemistry, electronic structure, and physical properties at the spin- and orbital-resolved levels in these reduced systems remains elusive. Here, we combine x-ray absorption spectroscopy, resonant inelastic x-ray scattering (RIXS), and density functional theory calculations to uncover topotactic metal-insulator transition and orbital-specific crystal field excitations in brownmillerite La0.67Ca0.33MnO2.5 thin films. We reveal the Mn valence states to be predominantly Mn2+/Mn3+, along with their corresponding populations at octahedral and tetrahedral sites, which effectively weaken the Mn-O hybridization compared to the parent perovskite phase. As a result, La0.67Ca0.33MnO2.5 films exhibit an antiferromagnetic insulating ground state. Moreover, by combining the RIXS measurements on selected single-valence manganites, specifically MnO, LaMnO3, and CaMnO3, with orbital- and spin-resolved density-of-states calculations, we identify the dd excitations of octahedrally and tetrahedrally coordinated Mn2+/Mn3+ ions, directly linking the microscopic electronic structure to the macroscopic magnetic/electrical properties.

cond-mat.mtrl-sci↗

arXiv2025

Sliding ferroelectric control of unconventional magnetism in stacked bilayers

The control of unconventional magnetism, which displays ferromagnetism-like properties with compensated magnetization, has drawn intense attention for advancing antiferromagnetic spintronics. Here, through symmetry analysis, we propose a general stacking rule, characterized by a connection operator linking two stacked bilayers, for controlling unconventional magnetism via sliding ferroelectricity. Such rule enables the simultaneous switching of both electric polarization and nonrelativistic spin splitting or anomalous Hall effect in altermagnets, a class of collinear unconventional magnets. By comprehensively surveying the 80 layer groups, we identify all the stacking orders that allow for such two types of simultaneous switching. Furthermore, we extend the stacking rule to collinear compensated ferrimagnets, where the opposite-spin sublattices are not connected by any symmetry operator, yet the net magnetization remains zero. Combined with first-principles calculations, we demonstrate the sliding ferroelectric control of spin polarization and anomalous Hall effect in the altermagnetic AgF2 and Fe2MoSe4 bilayers. Our work provides a symmetry strategy for achieving ferroelectric control of unconventional magnetism in bilayer systems and opens avenues for exploring new types of magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2024

Ferroelectric switchable altermagnetism

We propose a novel ferroelectric switchable altermagnetism effect, the reversal of ferroelectric polarization is coupled to the switching of altermagnetic spin splitting. We demonstrate the design principles for the ferroelectric altermagnets and the additional symmetry constraints necessary for switching the altermagnetic spin splitting through flipping the electric polarization based on the state-of-the-art spin-group symmetry techniques. 22 ferroelectric altermagnets are found by screening through the 2001 experimental reported magnetic structures in the MAGNDATA database and 2 of them are identified as ferroelectric switchable altermagnets. Using the hybrid improper ferroelectric material [C(NH2)3]Cr(HCOO)3 as an example, we show how the altermagnetic spin splitting is tightly coupled to the ferroelectric polarization, providing an ideal platform for designing electric-field-controllable multiferroic devices. Finally, we find that such manipulation of altermagnetism can be detected by monitoring the physical quantities that are related to the non-vanishing Berry curvature dipole, such as the linearly polarized photogalvanic spin current.

cond-mat.mtrl-sci↗

arXiv2023

Hard X-ray Generation and Detection of Nanometer-Scale Localized Coherent Acoustic Wave Packets in SrTiO$_3$ and KTaO$_3$

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the strain wavepacket and the energy absorption efficiency, which are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO$_3$ and KTaO$_3$ single crystals, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2023

Emergent giant ferroelectric properties in cost-effective raw zirconia dioxide

Ferroelectric fluorite dioxides like hafnium (HfO2)-based materials are considered to be one of the most potential candidates for nowadays large-scale integrated-circuits (ICs). While zirconia (ZrO2)-based fluorites materials, which has the same structure as HfO2 and more abundant resources and lower cost of raw materials, is usually thought to be anti- or ferroelectric-like. Here we reported a giant ferroelectric remnant polarization (Pr) amounted to 53 {\mu}C/cm2 in orthorhombic ZrO2 thin film at room temperature. This ferroelectricity arises from an electric field induced anti-ferroelectric to ferroelectric phase transition which is particularly noticeable at 77 K. Our work reveals the intrinsic ferroelectricity in ZrO2 thin films and offers a new pathway to understand the ferroelectricity origin in fluorite oxides.

cond-mat.mtrl-sci↗

arXiv2023

Chiral charge density wave and backscattering-immune orbital texture in monolayer 1T-TiTe2

Non-trivial electronic states are attracting intense attention in low-dimensional physics. Though chirality has been identified in charge states with a scalar order parameter, its intertwining with charge density waves (CDW), film thickness and the impact on the electronic behaviors remain less well understood. Here, using scanning tunneling microscopy, we report a 2 x 2 chiral CDW as well as a strong suppression of the Te-5p hole-band backscattering in monolayer 1T-TiTe2. These exotic characters vanish in bilayer TiTe2 with a non-CDW state. Theoretical calculations approve that chirality comes from a helical stacking of the triple-q CDW components and therefore can persist at the two-dimensional limit. Furthermore, the chirality renders the Te-5p bands an unconventional orbital texture that prohibits electron backscattering. Our study establishes TiTe2 as a promising playground for manipulating the chiral ground states at the monolayer limit and provides a novel path to engineer electronic properties from an orbital degree.

cond-mat.mtrl-sci↗

arXiv2022

Spin-phonon dispersion in magnetic materials

Microscopic coupling between the electron spin and the lattice vibration is responsible for an array of exotic properties from morphic effects in simple magnets to magnetodielectric coupling in multiferroic spinels and hematites. Traditionally, a single spin-phonon coupling constant is used to characterize how effectively the lattice can affect the spin, but it is hardly enough to capture novel electromagnetic behaviors to the full extent. Here, we introduce a concept of spin-phonon dispersion to project the spin moment change along the phonon crystal momentum direction, so the entire spin change can be mapped out. Different from the phonon dispersion, the spin-phonon dispersion has both positive and negative frequency branches {even in the equilibrium ground state}, which correspond to the spin enhancement and spin reduction, respectively. Our study of bcc Fe and hcp Co reveals that the spin force matrix, that is, the second-order spatial derivative of spin moment, is similar to the vibrational force matrix, but its diagonal elements are smaller than the off-diagonal ones. This leads to the distinctive spin-phonon dispersion. The concept of spin-phonon dispersion expands the traditional Elliott-Yafet theory in nonmagnetic materials to the entire Brillouin zone in magnetic materials, thus opening the door to excited states in systems such as CoF$_2$ and NiO, where a strong spin-lattice coupling is detected in the THz regime.

cond-mat.mtrl-sci↗

arXiv2022

Observation of magnetism induced topological edge state in antiferromagnetic topological insulator MnBi4Te7

Breaking time reversal symmetry in a topological insulator may lead to quantum anomalous Hall effect and axion insulator phase. MnBi4Te7 is a recently discovered antiferromagnetic topological insulator with TN ~12.5 K, which is constituted of alternatively stacked magnetic layer (MnBi2Te4) and non-magnetic layer (Bi2Te3). By means of scanning tunneling spectroscopy, we clearly observe the electronic state present at a step edge of a magnetic MnBi2Te4 layer but absent at non-magnetic Bi2Te3 layers at 4.5 K. Furthermore, we find that as the temperature rises above TN, the edge state vanishes, while the point defect induced state persists upon temperature increasing. These results confirm the observation of magnetism induced edge states. Our analysis based on an axion insulator theory reveals that the nontrivial topological nature of the observed edge state.

cond-mat.mtrl-sci↗

arXiv2022

Layer Hall effect induced by hidden Berry curvature in antiferromagnetic insulators

The layer Hall effect describes electrons spontaneously deflected to opposite sides at different layers, which has been experimentally reported in the MnBi$_2$Te$_4$ thinfilms under perpendicular electric fields [Gao et al., Nature 595, 521 (2021)]. Here, we reveal a universal origin of the layer Hall effect in terms of the so-called hidden Berry curvature, as well as material design principles. Hence, it gives rise to zero Berry curvature in momentum space but nonzero layer-locked hidden Berry curvature in real space. We show that compared to that of a trivial insulator, the layer Hall effect is significantly enhanced in antiferromagnetic topological insulators. Our universal picture provides a paradigm for revealing the hidden physics as a result of the interplay between the global and local symmetries, and can be generalized in various scenarios.

cond-mat.mes-hall↗

arXiv2022

Role of hidden spin polarization in non-reciprocal transport of antiferromagnets

The discovery of hidden spin polarization (HSP) in centrosymmetric nonmagnetic crystals, i.e., spatially distributed spin polarization originated from local symmetry breaking, has promised an expanded material pool for future spintronics. However, the measurements of such exotic effects have been limited to subtle space- and momentum-resolved techniques, unfortunately hindering their applications. Here, we theoretically predict macroscopic non-reciprocal transports induced by HSP when coupling another spatially distributed quantity, such as staggered local moments in a PT-symmetric anti-ferromagnet. By using a four-band model Hamiltonian, we demonstrate that HSP plays a crucial role in determining the asymmetric bands with respect to opposite momenta. Such band asymmetry leads to non-reciprocal nonlinear conductivity, exemplified by tetragonal CuMnAs via first-principles calculations. We further provide the material design principles for large nonlinear conductivity, including two-dimensional nature, multiple band crossings near the Fermi level, and symmetry protected HSP. Our work not only reveals direct spintronic applications of HSP (such as N\'eel order detection), but also sheds light on finding observables of other ''hidden effects'', such as hidden optical polarization and hidden Berry curvature.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast Suppression of the Ferroelectric Instability in KTaO$_3$

We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \kto. % We use ultrafast near-UV (central wavelength 266\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\,\AA\, and $< 10$~fs pulse duration). We observe changes in the diffuse intensity that we conclude are associated with a hardening of the soft transverse optical and transverse acoustic phonon branches along $\Gamma$ to $X$ and $\Gamma$ to $M$. Using ground- and excited-state interatomic force constants from density functional theory (DFT) and assuming the phonon populations can be described by a time-dependent temperature, we fit the quasi-equilibrium thermal diffuse intensity to the experimental time-dependent intensity. We obtain the instantaneous lattice temperature and density of photoexcited charge carriers as a function of time delay. The DFT calculations demonstrate that photoexcitation transfers charge from oxygen $2p$ derived $\pi$-bonding orbitals to Ta $5d$ derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

cond-mat.mtrl-sci↗

arXiv2021

Crossover between bulk and interface photovoltaic mechanisms in ferroelectric vertical heterostructure

Bulk photovoltaic (BPVE) effect in crystals lacking inversion symmetry offers great potential for optoelectronic applications due to its unique properties such as above bandgap photovoltage and switchable photocurrent. Because of their large spontaneous polarizations, ferroelectric materials are ideal platforms for studying BPVE. However, identifying the origin of experimentally observed photovoltaic response is often challenging due to the entanglement between bulk and interface effects, leading to much debate in the field. This issue is particularly pronounced in vertical heterostructures, where the two effects are comparable. Here we report a crossover between bulk- and interface-dominant response in vertical BiFeO3 heterostructures when changing the photon energy. We show that well above-bandgap excitation leads to bulk photovoltaic response, but band-edge excitation requires interface band bending to separate the photocarriers. Our findings not only help to clarify contradicting reports in the literature, but also lay the ground for a deeper understanding of ferroelectric photovoltaic effect and its applications in various devices.

cond-mat.mtrl-sci↗

arXiv2021

Pressure-tuned intralayer exchange in superlattice-like MnBi2Te4/(Bi2Te3)n topological insulators

The magnetic structures of MnBi2Te4(Bi2Te3)n can be manipulated by tuning the interlayer coupling via the number of Bi2Te3 spacer layers n, while the intralayer ferromagnetic (FM) exchange coupling is considered too robust to control. By applying hydrostatic pressure up to 3.5 GPa, we discover opposite responses of magnetic properties for n = 1 and 2. MnBi4Te7 stays at A-type antiferromagnetic (AFM) phase with a decreasing Néel temperature and an increasing saturation field. In sharp contrast, MnBi6Te10 experiences a phase transition from A-type AFM to a quasi-two-dimensional FM state with a suppressed saturation field under pressure. First-principles calculations reveal the essential role of intralayer exchange coupling from lattice compression in determining these magnetic properties. Such magnetic phase transition is also observed in 20% Sb-doped MnBi6Te10 due to the in-plane lattice compression.

cond-mat.mtrl-sci↗

arXiv2021

Correlation Between Spin and Orbital Dynamics During Laser-Induced Femtosecond Demagnetization

Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at the center of laser-induced ultrafast demagnetization. In this paper, we introduce a concept of the spin-orbital correlation diagram, where spin angular momentum is plotted against orbital angular momentum, much like the position-velocity phase diagram in classical mechanics. We use four sets of highly accurate time-resolved x-ray magnetic circular dichroism (TR-XMCD) data to construct four correlation diagrams for iron and cobalt. To our surprise, a pattern emerges. The trace on the correlation diagram for iron is an arc, and at the end of demagnetization, it has a pronounced cusp. The correlation diagram for cobalt is different and appears more linear, but with kinks. We carry out first-principles calculations with two different methods: time-dependent density functional theory (TDDFT) and time-dependent Liouville density functional theory (TDLDFT). These two methods agree that the experimental findings for both Fe and Co are not due t experimental errors. It is the spin-orbit coupling that correlates the spin dynamics to the orbital dynamics.Microscopically, Fe and Co have different orbital occupations, which leads to distinctive correlation diagrams. We believe that this correlation diagram presents a useful tool to better understand spin and orbital dynamics on an ultrafast time scale. A brief discussion on the magnetic anisotropy energy is also provided.

cond-mat.mtrl-sci↗

arXiv2021

Interlayer magnetophononic coupling in MnBi2Te4

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise 'forbidden' by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

cond-mat.mtrl-sci↗