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Liangbo Liang

Publications and source records attributed to Liangbo Liang.

At least 19 recordsLinked to original sources

Nanoscale Imaging of Strain-Controlled Altermagnetic Domains in {\alpha}-MnTe

Altermagnets combine compensated magnetic order with momentum-dependent spin splitting, offering a route to spintronic functionality without the stray fields of conventional ferromagnets. Mechanical strain provides a promising means of controlling their N\'eel order, yet the microscopic pathway by which strain reorganizes an altermagnetic texture remains unresolved. Here, we combine scanning nitrogen-vacancy magnetometry with a piezo-driven uniaxial strain cell to directly image the strain-driven evolution of magnetic domains in bulk {\alpha}-MnTe at room temperature. By applying uniaxial stress along the nearest-neighbor Mn-Mn bond direction, we find that compressive strain reorganizes the magnetic texture through domain coalescence, increasing the size of the largest connected domain while reducing the domain-wall density. On sweeping toward tensile strain direction, however, the domain network follows a distinct trajectory from that observed during the compressive sweep. Instead, the large connected regions fragment into a new metastable configuration, producing pronounced hysteresis in the maximum domain size and stray-field distribution. These results identify domain connectivity and topology as key carriers of strain-induced magnetic memory. Our work reveals domain coalescence and hysteretic fragmentation as the microscopic pathway of strain control in {\alpha}-MnTe and establishes a route toward strain-programmable altermagnetic textures and reconfigurable spintronic devices.

cond-mat.mtrl-sci

Magneto-optic phonon resonances in magnetic topological EuCd2As2 via helical Raman spectroscopy

EuCd2As2 materials have two magnetic ordering states: antiferromagnetic (AFM) and ferromagnetic (FM) when their chemical tunability is utilized. While AFM-EuCd2As2 has a nonzero magnetoelectric response due to its symmetry breaking with spin configuration, FM-EuCd2As2 is an ideal candidate for studies of Weyl physics because of its minimum number of Weyl points with opposite chirality. In this article, we examine cryogenic low-frequency Raman spectroscopy of phonon modes in FM-EuCd2As2 crystals using circular polarization configurations, with support from density functional theory calculations, and investigate in-plane magneto-anisotropy by linear polarization configuration below the Curie temperature (Tc = 26 K). We attribute the anomalous enhancements in Raman intensities below the Curie temperature are due to spin-phonon coupling. Furthermore, we see that A-mode peaks can be distinguished by magneto-helical Raman spectroscopy through the magneto-optic effect and that the degree of circular polarization (DCP) of 12.5 meV peak reaches 60% at 4.2 K and becomes saturated. We also examine AFM-EuCd2As2 below N\'eel temperature (TN = 9 K) to compare with FM-EuCd2As2, but we hardly observe spin-phonon coupling and find negligible DCP values due to almost zero net magnetization. Our results contribute to the understanding of the phonon dynamics and the interplay between topology and magnetism in FM-EuCd2As2, through helical light and external magnetic fields. This lays the foundation for utilizing state-of-the-art Weyl systems for applications in thermoelectrics, phononic devices, and topological quantum computing.

cond-mat.mtrl-sci

Raman Digital Twin of Monolayer Janus Transition Metal Dichalcogenides

Monolayer transition metal dichalcogenides (TMDs) are a key class of two-dimensional (2D) materials with broad technological potential. Their Janus counterparts exhibit unique properties due to broken out-of-plane symmetry and further enrich the functionalities of TMDs. However, experimental synthesis and identification of Janus TMDs remain challenging. It is thus highly desirable to have a rapid, simple, and in situ characterization technique to monitor, in real time, the conversion process from the parent to Janus structure. Raman spectroscopy stands out for such a task as it is a powerful, non-destructive, and very commonly used tool to characterize 2D materials both in situ and ex situ. To realize the full potential of Raman spectroscopy on rapid characterization of Janus TMDs, we present a computational "Raman digital twin" library for various monolayer Janus TMDs in both 2H and Td phases. We focus on group-6 TMDs: MoS$_2$, WS$_2$, MoSe$_2$, WSe$_2$, MoTe$_2$, WTe$_2$ and their Janus variants: MoSSe, MoSTe, MoSeTe, WSSe, WSTe, and WSeTe. Using first-principles density functional theory (DFT), we calculate their vibrational properties and predict distinct Raman fingerprints. These phonon and Raman signatures reflect each material's structural symmetry and atomic composition, enabling clear identification via Raman spectroscopy. Our theoretical work supports experimental efforts by providing benchmarks for material identification, structural analysis, and quality control. The computational library expedites the discovery and development of Janus 2D materials, facilitating tighter integration between theoretical predictions and experimental validation.

cond-mat.mtrl-sci

Mo Atom Rearrangement Drives Layer-Dependent Reactivity in Two-Dimensional MoS2

Two-dimensional (2D) materials offer a valuable platform for manipulating and studying chemical reactions at atomic level, owing to the ease of controlling their microscopic structure at the nanometer scale. While extensive research has been conducted on the structure-dependent chemical activity of 2D materials, the influence of structural transformation during the reaction remains largely unexplored. In this work, we report the layer-dependent chemical reactivity of MoS2 during a nitridation atomic substitution reaction and attribute it to the rearrangement of Mo atoms. Our results show that the chemical reactivity of MoS2 decreases as the number of layers is reduced in the few-layer regime. In particular, monolayer MoS2 exhibits significantly lower reactivity compared to its few-layer and multilayer counterparts. Atomic-resolution transmission electron microscope (TEM) reveals that MoN nanonetworks form as reaction products from monolayer and bilayer MoS2, with the continuity of the MoN crystals increasing with layer number, consistent with the local conductivity mapping data. The layer-dependent reactivity is attributed to the relative stability of the hypothetically formed MoN phase which retain the number of Mo atomic layers present in the precursor. Specifically, the low chemical reactivity of monolayer MoS2 is attributed to the high energy cost associated with Mo atom diffusion and migration necessary to form multi-layer Mo lattices in the thermodynamically stable MoN phase. This study underscores the critical role of lattice rearrangement in governing chemical reactivity and highlights the potential of 2D materials as versatile platforms for advancing the understanding of materials chemistry at atomic scale.

cond-mat.mtrl-sci

Probing Boron Vacancy Defects in hBN via Single Spin Relaxometry

Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to discover, read out, and spatially map arbitrary spin-based quantum sensors at the nanoscale. Using the boron vacancy ($\mathrm{V}_\mathrm{B}^-$) center in hexagonal boron nitride$\unicode{x2013}$an emerging two-dimensional spin system$\unicode{x2013}$as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time ($T_1$) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $\mathrm{V}_\mathrm{B}^-$. Cross-relaxation between NV and $\mathrm{V}_\mathrm{B}^-$ ensembles significantly reduces NV $T_1$, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h$^{10}$B$^{15}$N. Our method demonstrates interactions between 3D and 2D spin sensors, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.

cond-mat.mtrl-sci

Defect Engineering in Large-Scale CVD-Grown Hexagonal Boron Nitride: Formation, Spectroscopy, and Spin Relaxation Dynamics

Recently, numerous techniques have been reported for generating optically active defects in exfoliated hexagonal boron nitride (hBN), which hold transformative potential for quantum photonic devices. However, achieving on-demand generation of desirable defect types in scalable hBN films remains a significant challenge. Here, we demonstrate that formation of negative boron vacancy defects, VB-, in suspended, large-area CVD-grown hBN is strongly dependent on the type of bombarding particles (ions, neutrons, and electrons) and irradiation conditions. In contrast to suspended hBN, defect formation in substrate-supported hBN is more complex due to the uncontrollable generation of secondary particles from the substrate, and the outcome strongly depends on the thickness of the hBN. We identify different defect types by correlating spectroscopic and optically detected magnetic resonance features, distinguishing boron vacancies (formed by light ions and neutrons) from other optically active defects emitting at 650 nm assigned to anti-site nitrogen vacancy (NBVN) and reveal the presence of additional dark paramagnetic defects that influence spin-lattice relaxation time (T1) and zero-field splitting parameters, all of which strongly depend on the defect density. These results underscore the potential for precisely engineered defect formation in large-scale CVD-grown hBN, paving the way for the scalable fabrication of quantum photonic devices.

cond-mat.mtrl-sci

Telecom-wavelength Single-photon Emitters in Multi-layer InSe

The development of robust and efficient single photon emitters (SPEs) at telecom wavelengths is critical for advancements in quantum information science. Two-dimensional (2D) materials have recently emerged as promising sources for SPEs, owing to their high photon extraction efficiency, facile coupling to external fields, and seamless integration into photonic circuits. In this study, we demonstrate the creation of SPEs emitting in the 1000 to 1550 nm near-infrared range by coupling 2D indium selenide (InSe) with strain-inducing nanopillar arrays. The emission wavelength exhibits a strong dependence on the number of layers. Hanbury Brown and Twiss experiments conducted at 10 K reveal clear photon antibunching, confirming the single-photon nature of the emissions. Density-functional-theory calculations and scanning-tunneling-microscopy analyses provide insights into the electronic structures and defect states, elucidating the origins of the SPEs. Our findings highlight the potential of multilayer 2D metal monochalcogenides for creating SPEs across a broad spectral range, paving the way for their integration into quantum communication technologies.

physics.optics

Thickness-Dependent Polaron Crossover in Tellurene

Polarons, quasiparticles arising from electron-phonon coupling, are crucial in understanding material properties such as high-temperature superconductivity and colossal magnetoresistance. However, scarce studies have been performed to investigate the formation of polarons in low-dimensional materials with phonon polarity and electronic structure transitions. In this work, we studied polarons of tellurene that are composed of chiral chains of tellurium atoms. The frequency and linewidth of the A1 phonon, which becomes increasingly polar for thinner tellurene, exhibit an abrupt change when the thickness of tellurene is below 10 nm. Meanwhile, the field effect mobility of tellurene drops rapidly as the thickness is smaller than 10 nm. These phonon and transport signatures, combined with the calculated phonon polarity and band structure, suggest a crossover from large polarons for bulk tellurium to small polarons for few-layer tellurene. Effective field theory considers the phonon renormalization in the strong coupling (small polaron) regime, and semi-quantitatively reproduces the observed phonon hardening and broadening effects in few-layer tellurene. This polaron crossover stems from the quasi-1D nature of tellurene where modulation of the interchain distance reduces the dielectric screening and promotes electron-phonon coupling. Our work provides valuable insights into the influence of polarons on phononic, electronic, and structural properties in low-dimensional materials.

cond-mat.mtrl-sci

Nanoscale imaging of He-ion irradiation effects on amorphous TaO$_x$ toward electroforming-free neuromorphic functions

Resistive switching in thin films has been widely studied in a broad range of materials. Yet the mechanisms behind electroresistive switching have been persistently difficult to decipher and control, in part due to their non-equilibrium nature. Here, we demonstrate new experimental approaches that can probe resistive switching phenomena, utilizing amorphous TaO$_x$ as a model material system. Specifically, we apply Scanning Microwave Impedance Microscopy (sMIM) and cathodoluminescence (CL) microscopy as direct probes of conductance and electronic structure, respectively. These methods provide direct evidence of the electronic state of TaO$_x$ despite its amorphous nature. For example CL identifies characteristic impurity levels in TaO$_x$, in agreement with first principles calculations. We applied these methods to investigate He-ion-beam irradiation as a path to activate conductivity of materials and enable electroforming-free control over resistive switching. However, we find that even though He-ions begin to modify the nature of bonds even at the lowest doses, the films conductive properties exhibit remarkable stability with large displacement damage and they are driven to metallic states only at the limit of structural decomposition. Finally, we show that electroforming in a nanoscale junction can be carried out with a dissipated power of < 20 nW, a much smaller value compared to earlier studies and one that minimizes irreversible structural modifications of the films. The multimodal approach described here provides a new framework toward the theory/experiment guided design and optimization of electroresistive materials.

cond-mat.mtrl-sci

Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit

Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can only provide a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopies supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 nm to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ~ 100 nm spectral range and two-orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to the observed CL photon superbunching. Also, the measured GaSe SPE photophysics after electron beam exposure shows the excellent stability of these SPEs. We anticipate this insight into nanoscale strain control of two-dimensional SPEs will guide the development of truly deterministic quantum photonics.

physics.optics

Descriptor-Enabled Rational Design of High-Entropy Materials Over Vast Chemical Spaces

The practically unlimited high-dimensional composition space of high-entropy materials (HEMs) has emerged as an exciting platform for functional materials design and discovery. However, the identification of stable and synthesizable HEMs and robust design rules remains a daunting challenge due to the difficulty in determining composition/structure-specific enthalpy and entropy contributions to the stability and formation of HEMs. In this work, using first-principles calculations, we find that (i) the stability and miscibility of HEMs strongly depend on the formation enthalpy of the HEM relative to the most stable completing phase rather than on the conventionally-viewed enthalpies of mixing over all possible competing phases, and (ii) the entropy forming ability of a HEM can be measured from the defect formation energy spectrum of tens of substitutional defects in ordered binary compounds, involving no sampling over numerous alloy configurations. Based on these findings, we propose a highly predictive Mixed Enthalpy-Entropy Descriptor (MEED), which enables the rational high-throughput first-principles design and screening of new HEMs over large chemical spaces. Applying the MEED to two structurally distinct material systems (i.e., 3D rocksalt carbides and 2D layered sulfides), not only all experimentally reported HEMs within each system are successfully identified, but a universal cutoff criterion for assessing their relative synthesizability also revealed. In addition, tens of new high entropy carbides and 2D high-entropy sulfides are also predicted. They have the potential for a wide variety of applications such as coating in aerospace devices, energy conversion and storage, and flexible electronics.

cond-mat.mtrl-sci

Deterministic Localization of Strain-induced Single-photon Emitters in Multilayer GaSe

Nanoscale strain has emerged as a powerful tool for controlling single-photon emitters (SPEs) in atomically thin transition metal dichalcogenides (TMDCs)(1, 2). However, quantum emitters in monolayer TMDCs are typically unstable in ambient conditions. Multilayer two-dimensional (2D) TMDCs could be a solution, but they suffer from low quantum efficiency, resulting in low brightness of the SPEs. Here, we report the deterministic spatial localization of strain-induced single-photon emitters in multilayer GaSe by nanopillar arrays. The strain-controlled quantum confinement effect introduces well-isolated sub-bandgap photoluminescence and corresponding suppression of the broad band edge photoluminescence. Clear photon-antibunching behavior is observed from the quantum dot-like GaSe sub-bandgap exciton emission at 3.5 Kelvin. The strain-dependent confinement potential and the brightness are found to be strongly correlated, suggesting a promising route for tuning and controlling SPEs. The comprehensive investigations of strain-engineered GaSe SPEs provide a solid foundation for the development of 2D devices for quantum photonic technologies.

cond-mat.mtrl-sci

Nano-imaging of the edge-dependent optical polarization anisotropy of black phosphorus

The electronic structure and functionality of 2D materials is highly sensitive to structural morphology, opening the possibility for manipulating material properties, but also making predictable and reproducible functionality challenging. Black phosphorus (BP), a corrugated orthorhombic 2D material, has in-plane optical absorption anisotropy critical for applications such as directional photonics, plasmonics, and waveguides. Here, we use polarization-dependent photoemission electron microscopy to visualize the anisotropic optical absorption of BP with 54 nm spatial resolution. We find the edges of BP flakes have a shift in their optical polarization anisotropy from the flake interior due to the 1D confinement and symmetry reduction at flake edges that alter the electronic charge distributions and transition dipole moments of edge electronic states, confirmed with first-principles calculations. These results uncover previously hidden modification of the polarization-dependent absorbance at the edges of BP, highlighting the opportunity for selective excitation of edge states of 2D materials with polarized light.

cond-mat.mes-hall

Phonon Chirality Induced by Vibronic-Orbital Coupling

The notion that phonons can carry pseudo-angular momentum has become popular in the last decade, with recent research efforts highlighting phonon chirality, Berry curvature of phonon band structure, and the phonon Hall effect. When a phonon is resonantly coupled to a crystal electric field excitation, a so-called vibronic bound state forms. Here, we observe angular momentum transfer of $δ$Jz = $\pm$1$\hbar$ between phonons and an orbital state in a vibronic bound state of a candidate quantum spin liquid. This observation has profound implications for the engineering of phonon band structure topology through chiral quasiparticle interactions.

cond-mat.mes-hall

The Role of the Third Dimension in Searching Majorana Fermions in $α$-RuCl$_3$ via Phonons

Understanding phonons in $α$-RuCl$_3$ is critical to analyze the controversy around the observation of the half-integer thermal quantum Hall effect. While many studies have focused on the magnetic excitations in $α$-RuCl$_3$, its vibrational excitation spectrum has remained relatively unexplored. We investigate the phonon structure of $α$-RuCl$_3$ via inelastic neutron scattering experiments and density functional theory calculations. Our results show excellent agreement between experiment and first principles calculations. After validating our theoretical model, we extrapolate the low energy phonon properties. We find that the phonons in $α$-RuCl$_3$ that either propagate or vibrate in the out-of-plane direction have significantly reduced velocities, and therefore have the potential to dominate the observability of the elusive half integer plateaus in the thermal Hall conductance. In addition, we use low-energy interlayer phonons to resolve the low temperature stacking structure of our large crystal of $α$-RuCl$_3$, which we find to be consistent with that of the $R\bar{3}$ space group, in agreement with neutron diffraction.

cond-mat.str-el

Low-frequency Raman signature of Ag-intercalated few-layer MoS$_2$

Density functional theory based calculations and experimental analysis on a limited number of real samples are performed to study how the presence of silver intercalated in the van der Waals gap of few-layer MoS$_2$ affects the low-frequency Raman active modes of this material. Silver is found to predominantly affect the breathing-like and shear-like vibrational modes of MoS$_2$. These modes correspond to quasi-rigid movements of each individual layer with a restoring force (and, in turn, frequency) that is determined by modulations in the weak interlayer interactions. Noticeable red-shifts with increasing Ag concentration are found for all low-frequency modes. This finding indicates the potential for low-frequency vibrations as useful gauges for practical determination of silver concentration using low-frequency Raman spectroscopy. This work also describes a semi-classical linear chain model that allows to extrapolate results to a large number of layers. Further, first-principles calculations show how Raman spectroscopy can be used to characterize the quality of the two-dimensional interface between MoS$_2$ and a silver substrate.

cond-mat.mes-hall

Nearly-Resonant Crystalline-Phononic Coupling in Quantum Spin Liquid Candidate CsYbSe$_2$

CsYbSe$_2$, a recently identified quantum spin liquid (QSL) candidate, exhibits strong crystal electric field (CEF) excitations. Here, we identify phonon and CEF modes with Raman spectroscopy and observe strong CEF-phonon mixing resulting in a vibronic bound state. Complex, mesoscale interplay between phonon modes and CEF modes is observed in real space, and an unexpected nearly resonant condition is satisfied, yielding up to fifth-order combination modes, with a total of 17 modes identified in the spectra. This study paves the way to coherent control of possible QSL ground states with optically accessible CEF-phonon manifolds and mesoscale engineering of CEF-phonon interactions.

cond-mat.str-el

Floquet band engineering and topological phase transitions in 1T' transition metal dichalcogenides

Using ab initio tight-binding approaches, we investigate Floquet band engineering of the 1T' phase of transition metal dichalcogenides (MX2, M = W, Mo and X = Te, Se, S) monolayers under the irradiation with circularly polarized light. Our first principles calculations demonstrate that light can induce important transitions in the topological phases of this emerging materials family. For example, upon irradiation, Te-based MX2 undergoes a phase transition from quantum spin Hall (QSH) semimetal to time-reversal symmetry broken QSH insulator with a nontrivial band gap of up to 92.5 meV. On the other hand, Se- and S-based MX2 undergoes the topological phase transition from the QSH effect to the quantum anomalous Hall (QAH) effect and into trivial phases with increasing light intensity. From a general perspective, our work brings further insight into non-equilibrium topological systems.

cond-mat.mtrl-sci