arXiv subjects

Xiaoqin Li

Publications and source records attributed to Xiaoqin Li.

At least 37 records · Page 2Linked to original sources

arXiv2022

Confined monolayer Ag as a large gap 2D semiconductor and its momentum resolved excited states

2D materials have intriguing quantum phenomena that are distinctively different from their bulk counterparts. Recently, epitaxially synthesized wafer-scale 2D metals, composed of elemental atoms, are attracting attention not only for their potential applications but also for exotic quantum effects such as superconductivity. By mapping momentum-resolved electronic states using time-resolved and angle-resolved photoemission spectroscopy (ARPES), we reveal that monolayer Ag confined between bilayer graphene and SiC is a large gap (> 1 eV) 2D semiconductor, consistent with GW-corrected density functional theory. The measured valence band dispersion matches the DFT-GW quasiparticle band. However, the conduction band dispersion shows an anomalously large effective mass of 2.4 m0. Possible mechanisms for this large enhancement in the apparent mass are discussed.

cond-mat.mtrl-sci↗

arXiv2022

Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe$_2$ bilayers

While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ valley to other lower energy $Γ$ and $Λ$ valleys in the bilayer. Our combined experimental and theoretical studies unequivocally establish different microscopic mechanisms that determine exciton quantum dynamics in TMDC monolayers and bilayers. Understanding exciton quantum dynamics provides critical guidance to manipulation of spin/valley degrees of freedom in TMDC bilayers.

cond-mat.mes-hall↗

arXiv2022

Strong bulk Dzyaloshinskii-Moriya interaction in composition-uniform centrosymmetric magnetic single layers

Dzyaloshinskii-Moriya interaction (DMI) is the key ingredient of chiral spintronic phenomena and the emerging technologies based on such phenomena. A nonzero DMI usually occurs at magnetic interfaces or within non-centrosymmetric single crystals. Here, we report the observation of a strong unexpected DMI within a centrosymmetric polycrystalline ferromagnet that has neither a crystal inversion symmetry breaking nor a composition gradient. This DMI is a bulk effect, increases with the thickness of the magnetic layer, and is insensitive to the symmetry of the interfaces or the neighboring materials. We observe a total DMI strength that is a factor of >2 greater than the highest interfacial DMI in the literature. This DMI most likely arises from the strong spin-orbit coupling, strong orbital hybridization, and a "hidden" long-range asymmetry in the material. Our discovery of the strong unconventional bulk DMI in centrosymmetric, composition-uniform magnetic single layers provide fundamental building blocks for the emerging field of spintronics and will stimulate the exploitation of unconventional spin-orbit phenomena in a wide range of materials.

cond-mat.mtrl-sci↗

arXiv2022

Quantitative determination of interlayer electronic coupling at various critical points in bilayer MoS2

Tailoring interlayer coupling has emerged as a powerful tool to tune the electronic structure of van der Waals (vdW) bilayers. One example is the usage of the moire pattern to create controllable two-dimensional electronic superlattices through the configurational dependence of interlayer electronic couplings. This approach has led to some remarkable discoveries in twisted graphene bilayers, and transition metal dichalcogenide (TMD) homo- and hetero-bilayers. However, a largely unexplored factor is the interlayer distance, d, which can impact the interlayer coupling strength exponentially. In this letter, we quantitatively determine the coupling strengths as a function of interlayer spacing at various critical points of the Brillouin zone in bilayer MoS2. The exponential dependence of the coupling parameter on the gap distance is demonstrated. Most significantly, we achieved a 280% enhancement of K-valley coupling strength with an 8% reduction of the vdW gap, pointing to a new strategy in designing a novel electronic system in vdW bilayers.

cond-mat.mtrl-sci↗

arXiv2022

All Electrical Control and Temperature Dependence of the Spin and Valley Hall Effect in Monolayer WSe2 Transistors

Heavy metal-based two-dimensional van der Waals materials have a large, coupled spin and valley Hall effect (SVHE) that has potential use in spintronics and valleytronics. Optical measurements of the SVHE have largely been performed below 30 K and understanding of the SVHE-induced spin/valley polarizations that can be electrically generated is limited. Here, we study the SVHE in monolayer p-type tungsten diselenide (WSe2). Kerr rotation (KR) measurements show the spatial distribution of the SVHE at different temperatures, its persistence up to 160 K, and that it can be electrically modulated via gate and drain bias. A spin/valley drift and diffusion model together with reflection spectra data is used to interpret the KR data and predict a lower-bound spin/valley lifetime of 4.1 ns below 90 K and 0.26 ns at 160 K. The excess spin and valley per unit length along the edge is calculated to be 109 per micron at 45 K, which corresponds to a spin/valley polarization on the edge of 6%. These results are important steps towards practical use of the SVHE.

cond-mat.mes-hall↗

arXiv2021

Superior Photo-carrier Diffusion Dynamics in Organic-inorganic Hybrid Perovskites Revealed by Spatiotemporal Conductivity Imaging

The outstanding performance of organic-inorganic metal trihalide solar cells benefits from the exceptional photo-physical properties of both electrons and holes in the material. Here, we directly probe the free-carrier dynamics in Cs-doped FAPbI3 thin films by spatiotemporal photoconductivity imaging. Using charge transport layers to selectively quench one type of carriers, we show that the two relaxation times on the order of 1 microsecond and 10 microseconds correspond to the lifetimes of electrons and holes in FACsPbI3, respectively. Strikingly, the diffusion mapping indicates that the difference in electron/hole lifetimes is largely compensated by their disparate mobility. Consequently, the long diffusion lengths (3 ~ 5 micrometers) of both carriers are comparable to each other, a feature closely related to the unique charge trapping and de-trapping processes in hybrid trihalide perovskites. Our results unveil the origin of superior diffusion dynamics in this material, crucially important for solar-cell applications.

cond-mat.mes-hall↗

arXiv2021

Interfacial Dzyaloshinskii-Moriya interaction and spin-orbit torque in Au1-xPtx/Co bilayers with varying interfacial spin-orbit coupling

The quantitative roles of the interfacial spin-orbit coupling (SOC) in Dzyaloshinskii-Moriya interaction (DMI) and dampinglike spin-orbit torque (τDL) have remained unsettled after a decade of intensive study. Here, we report a conclusive experiment evidence that, because of the critical role of the interfacial orbital hybridization, the interfacial DMI is not necessarily a linear function of the interfacial SOC, e.g. at Au1-xPtx/Co interfaces where the interfacial SOC can be tuned significantly via strongly composition (x)-dependent spin-orbit proximity effect without varying the bulk SOC and the electronegativity of the Au1-xPtx layer. We also find that τDL in the Au1-xPtx/Co bilayers varies distinctly from the interfacial SOC as a function of x, indicating no important τDL contribution from the interfacial Rashba-Edelstein effect.

cond-mat.mtrl-sci↗

arXiv2021

Spin-Phonon Interaction in Yttrium Iron Garnet

Spin-phonon interaction is an important channel for spin and energy relaxation in magnetic insulators. Understanding this interaction is critical for developing magnetic insulator-based spintronic devices. Quantifying this interaction in yttrium iron garnet (YIG), one of the most extensively investigated magnetic insulators, remains challenging because of the large number of atoms in a unit cell. Here, we report temperature-dependent and polarization-resolved Raman measurements in a YIG bulk crystal. We first classify the phonon modes based on their symmetry. We then develop a modified mean-field theory and define a symmetry-adapted parameter to quantify spin-phonon interaction in a phonon-mode specific way for the first time in YIG. Based on this improved mean-field theory, we discover a positive correlation between the spin-phonon interaction strength and the phonon frequency.

cond-mat.mes-hall↗

arXiv2021

Twist Angle Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in $\text{MoSe}_{\text{2}}$/$\text{WSe}_{\text{2}}$ twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1$^\circ$ to 3.5$^\circ$. Using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of "twistronics".

cond-mat.mes-hall↗

arXiv2020

Momentum resolved ground/excited states and the ultra-fast excited state dynamics of monolayer MoS2

The emergence of transition metal dichalcogenides (TMD) as crystalline atomically thin semiconductors has created a tremendous amount of scientific and technological interest. Many novel device concepts have been proposed and realized (1-3). Nonetheless, progress in k-space investigations of ground/excited state electronic structures has been slow due to the challenge to create large scale, laterally homogeneous samples. Taking advantage of recent advancements in chemical vapor deposition, here we create a wafer-size MoS2 monolayer with well-aligned lateral orientation for advanced electron spectroscopy studies (4-6). Low energy electron diffraction and scanning tunneling microscopy (STM) demonstrate atomically clean surfaces with in-plane crystalline orientation. The ground state and excited state electronic structures are probed using scanning tunneling spectroscopy (STS), angle-resolved photoemission (ARPES) and time-resolved (tr-)ARPES. In addition to mapping out the momentum-space quasiparticle band structure in the valence and conduction bands, we unveil ultrafast excited state dynamics, including inter- and intra-valley carrier scattering and a rapid downward energy shift by ~ 0.2eV lower than the initial free carrier state at Sigma point.

cond-mat.mes-hall↗

arXiv2020

Dimensional crossover in spin Hall oscillators

Auto-oscillations of magnetization driven by direct spin current have been previously observed in multiple quasi-zero-dimensional (0D) ferromagnetic systems such as nanomagnets and nanocontacts. Recently, it was shown that pure spin Hall current can excite coherent auto-oscillatory dynamics in quasi-one-dimensional (1D) ferromagnetic nanowires but not in quasi-two-dimensional (2D) ferromagnetic films. Here we study the 1D to 2D dimensional crossover of current-driven magnetization dynamics in wire-based Pt/$\mathrm{Ni}_{80}\mathrm{Fe}_{20}$ bilayer spin Hall oscillators via varying the wire width. We find that increasing the wire width results in an increase of the number of excited auto-oscillatory modes accompanied by a decrease of the amplitude and coherence of each mode. We also observe a crossover from a hard to a soft onset of the auto-oscillations with increasing the wire width. The amplitude of auto-oscillations rapidly decreases with increasing temperature suggesting that interactions of the phase-coherent auto-oscillatory modes with incoherent thermal magnons plays an important role in suppression of the auto-oscillatory dynamics. Our measurements set the upper limit on the dimensions of an individual spin Hall oscillator and elucidate the mechanisms leading to suppression of coherent auto-oscillations with increasing oscillator size.

cond-mat.mes-hall↗

arXiv2020

Directivity modulation of exciton emission using single dielectric nanospheres

Coupling emitters with nanoresonators is an effective strategy to control light emission at the subwavelength scale with high efficiency. Low-loss dielectric nanoantennas hold particular promise for this purpose, owing to their strong Mie resonances. Herein, we explore a highly miniaturized platform for the control of emission based on individual subwavelength Si nanospheres (SiNSs) to modulate the directional excitation and exciton emission of two-dimensional transition metal dichalcogenides (2D TMDs). A modified Mie theory for dipole-sphere hybrid systems is derived to instruct the optimal design for desirable modulation performance. Controllable forward-to-backward intensity ratios are experimentally validated in 532 nm laser excitation and 635 nm exciton emission from a monolayer WS2. Versatile light emission control along all device orientations is achieved for different emitters and excitation wavelengths, benefiting from the facile size control and isotropic shape of SiNSs. Simultaneous modulation of excitation and emission via a single SiNS at visible wavelengths significantly improves the efficiency and directivity of TMD exciton emission and leads to the potential of multifunctional integrated photonics. Overall, our work opens promising opportunities for nanophotonics and polaritonic systems, enabling efficient manipulation, enhancement and reconfigurability of light-matter interactions.

physics.optics↗

arXiv2020

Phonon Renormalization in Reconstructed MoS$_2$ Moiré Superlattices

In moiré crystals formed by stacking van der Waals (vdW) materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS$_2$ twisted bilayers, adding a new perspective to moiré physics. Over a range of small twist angles, the phonon spectra evolve rapidly due to ultra-strong coupling between different phonon modes and atomic reconstructions of the moiré pattern. We develop a new low-energy continuum model for phonons that overcomes the outstanding challenge of calculating properties of large moiré supercells and successfully captures essential experimental observations. Remarkably, simple optical spectroscopy experiments can provide information on strain and lattice distortions in moiré crystals with nanometer-size supercells. The newly developed theory promotes a comprehensive and unified understanding of structural, optical, and electronic properties of moiré superlattices.

cond-mat.mes-hall↗

arXiv2020

Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors

Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of the momentum forbidden dark excitons, and study their properties, including their near-degeneracy with bright excitons and their formation pathways in the energy-momentum landscape. These dark excitons dominate the excited state distribution - a surprising finding that highlights their importance in atomically thin semiconductors.

cond-mat.mtrl-sci↗

arXiv2020

Chiral symmetry breaking for deterministic switching of perpendicular magnetization by spin-orbit torque

Symmetry breaking is a characteristic to determine which branch of a bifurcation system follows upon crossing a critical point. Specifically, in spin-orbit torque (SOT) devices, a fundamental question arises: how to break the symmetry of the perpendicular magnetic moment by the in-plane spin polarization? Here, we show that the chiral symmetry breaking by the DMI can induce the deterministic SOT switching of the perpendicular magnetization. By introducing a gradient of saturation magnetization or magnetic anisotropy, non-collinear spin textures are formed by the gradient of effective SOT strength, and thus the chiral symmetry of the SOT-induced spin textures is broken by the DMI, resulting in the deterministic magnetization switching. We introduce a strategy to induce an out-of-plane (z) gradient of magnetic properties, as a practical solution for the wafer-scale manufacture of SOT devices.

cond-mat.mes-hall↗

arXiv2020

Unveiling Defect-Mediated Carrier Dynamics in Monolayer Semiconductors by Spatiotemporal Microwave Imaging

The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals respectively. Time-resolved experiments indicate that the critical process for photo-excited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the photoconductivity is stronger in CVD samples than exfoliated monolayers with a lower defect density. Our work reveals the intrinsic time and length scales of electrical response to photo-excitation in van der Waals materials, which is essential for their applications in novel optoelectronic devices.

cond-mat.mes-hall↗

arXiv2019

Moiré Potential Impedes Interlayer Exciton Diffusion in van der Waals Heterostructures

The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moiré superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moiré crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the moiré period reduces at a larger twist angle, excitons can tunnel between supercells and diffuse over a longer lifetime. The diffusion length should be the longest in commensurate heterostructures where the moiré superlattice is completely absent. In this study, we experimentally demonstrate that the moiré potential impedes interlayer exciton diffusion by comparing a number of WSe2/MoSe2 heterostructures prepared with chemical vapor deposition and mechanical stacking with accurately controlled twist angles. Our results provide critical guidance to developing 'twistronic' devices that explore the moiré superlattice to engineer material properties.

cond-mat.mes-hall↗

arXiv2019

Modulated Interlayer Exciton Properties in a Two-Dimensional Moire Crystal

Twisted van der Waals heterostructures and the corresponding superlattices, moire superlattices, are remarkable new material platforms, in which electron interactions and excited-state properties can be engineered. Particularly, the band offsets between adjacent layers can separate excited electrons and holes, forming interlayer excitons that exhibit unique optical properties. In this work, we employ the first-principles GW-Bethe-Salpeter Equation (BSE) method to calculate quasiparticle band gaps, interlayer excitons, and their modulated excited-state properties in twisted MoSe2/WSe2 bilayers that are of broad interest currently. In addition to achieving good agreements with the measured interlayer exciton energies, we predict a more than 100-meV lateral quantum confinement on quasiparticle energies and interlayer exciton energies, guiding the effort on searching for localized quantum emitters and simulating the Hubbard model in two-dimensional twisted structures. Moreover, we find that the optical dipole oscillator strength and radiative lifetime of interlayer excitons are modulated by a few orders of magnitude across moire supercells, highlighting the potential of using moire crystals to engineer exciton properties for optoelectronic applications.

cond-mat.mes-hall↗