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Keji Lai

Publications and source records attributed to Keji Lai.

At least 37 records · Page 2Linked to original sources

Material design with the van der Waals stacking of bismuth-halide chains realizing a higher-order topological insulator

The van der Waals (vdW) materials with low dimensions have been extensively studied as a platform to generate exotic quantum properties. Advancing this view, a great deal of attention is currently paid to topological quantum materials with vdW structures. Here, we provide a new concept of designing topological materials by the vdW stacking of quantum spin Hall insulators (QSHIs). Most interestingly, a slight shift of inversion center in the unit cell caused by a modification of stacking is found to induce the topological variation from a trivial insulator to a higher-order topological insulator (HOTI). Based on that, we present the first experimental realization of a HOTI by investigating a bismuth bromide Bi4Br4 with angle-resolved photoemission spectroscopy (ARPES). The unique feature in bismuth halides capable of selecting various topology only by differently stacking chains, combined with the great advantage of the vdW structure, offers a fascinating playground for engineering topologically non-trivial edge-states toward future spintronics applications.

cond-mat.mtrl-sci↗

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↗

Nanoscale Conductivity Imaging of Correlated Electronic States in WSe2/WS2 Moiré Superlattices

We report the nanoscale conductivity imaging of correlated electronic states in angle-aligned WSe2/WS2 heterostructures using microwave impedance microscopy. The noncontact microwave probe allows us to observe the Mott insulating state with one hole per moiré unit cell that persists for temperatures up to 150 K, consistent with other characterization techniques. In addition, we identify for the first time a Mott insulating state at one electron per moiré unit cell. Appreciable inhomogeneity of the correlated states is directly visualized in the hetero-bilayer region, indicative of local disorders in the moiré superlattice potential or electrostatic doping. Our work provides important insights on 2D moiré systems down to the microscopic level.

cond-mat.mes-hall↗

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↗

Emergence of Competing Stripe Phase near the Mott Transition in Ti-doped Bilayer Calcium Ruthenates

We report the nanoscale imaging of Ti-doped bilayer calcium ruthenates during the Mott metal-insulator transition by microwave impedance microscopy. Different from a typical first-order phase transition where coexistence of the two terminal phases takes place, a new metallic stripe phase oriented along the in-plane crystalline axes emerges inside both the G-type antiferromagnetic insulating state and paramagnetic metallic state. The effect of this electronic state can be observed in macroscopic measurements, allowing us to construct a phase diagram that takes into account the energetically competing phases. Our work provides a model approach to correlate the macroscopic properties and mesoscopic phase separation in complex oxide materials.

cond-mat.str-el↗

Unexpected Giant Microwave Conductivity in a Nominally Silent BiFeO3 Domain Wall

Nanoelectronic devices based on ferroelectric domain walls (DWs), such as memories, transistors, and rectifiers, have been demonstrated in recent years. Practical high-speed electronics, on the other hand, usually demand operation frequencies in the giga-Hertz (GHz) regime, where the effect of dipolar oscillation is important. In this work, an unexpected giant GHz conductivity on the order of 103 S/m is observed in certain BiFeO3 DWs, which is about 100,000 times greater than the carrier-induced dc conductivity of the same walls. Surprisingly, the nominal configuration of the DWs precludes the ac conduction under an excitation electric field perpendicular to the surface. Theoretical analysis shows that the inclined DWs are stressed asymmetrically near the film surface, whereas the vertical walls in a control sample are not. The resultant imbalanced polarization profile can then couple to the out-of-plane microwave fields and induce power dissipation, which is confirmed by the phase-field modeling. Since the contributions from mobile-carrier conduction and bound-charge oscillation to the ac conductivity are equivalent in a microwave circuit, the research on local structural dynamics may open a new avenue to implement DW nano-devices for RF applications.

cond-mat.mtrl-sci↗

Opto-electronic properties of alpha-In2Se3: single-layer to bulk

In this work, we report linear and non-linear spectroscopic measurements of chemically-grown layered (from one to 37 quintuple layers) and bulk alpha-In2Se3 samples over a photon energy range of 1.0--4 eV, and compare with ab initio density functional theory calculations, including bandstructures and G0W0 calculations.

cond-mat.mtrl-sci↗

Coherent Acoustic Control of a Single Silicon Vacancy Spin in Diamond

Phonons are considered to be universal quantum transducers due to their ability to couple to a wide variety of quantum systems. Among these systems, solid-state point defect spins are known for being long-lived optically accessible quantum memories. Recently, it has been shown that inversion-symmetric defects in diamond, such as the negatively charged silicon vacancy center (SiV), feature spin qubits that are highly susceptible to strain. Here, we leverage this strain response to achieve coherent and low-power acoustic control of a single SiV spin, and perform acoustically driven Ramsey interferometry of a single spin. Our results demonstrate a novel and efficient method of spin control for these systems, offering a path towards strong spin-phonon coupling and phonon-mediated hybrid quantum systems.

quant-ph↗

Activation of nominally silent domain wall-localized phonons from GHz to THz frequencies

Ferroelectric domain walls (DWs) are nanoscale topological defects that can be easily tailored to create nanoscale devices. Their excitations, recently discovered to be responsible for DW GHz conductivity, hold promise for faster signal transmission and processing speed compared to the existing technology. Here we find that DW phonons disperse from GHz to THz frequencies, thus explaining the origin of the surprisingly broad GHz signature in DW conductivity. Puzzling activation of nominally silent DW sliding modes in BiFeO3 is traced back to DW tilting and resulting asymmetry in wall-localized phonons. The obtained phonon spectra and selection rules are used to simulate scanning impedance microscopy, emerging as a powerful probe in nanophononics. The results will guide experimental discovery of the predicted phonon branches and design of DW-based nanodevices.

cond-mat.mtrl-sci↗

Microwave-to-optical conversion using lithium niobate thin-film acoustic resonators

We demonstrate conversion of up to 4.5 GHz-frequency microwaves to 1500 nm-wavelength light using optomechanical interactions on suspended thin-film lithium niobate. Our method utilizes an interdigital transducer that drives a free-standing 100 $μ$m-long thin-film acoustic resonator to modulate light travelling in a Mach-Zehnder interferometer or racetrack cavity. Owing to the strong microwave-to-acoustic coupling offered by the transducer in conjunction with the strong photoelastic, piezoelectric, and electro-optic effects of lithium niobate, we achieve a half-wave voltage of $V_π$ = 4.6 V and $V_π$ = 0.77 V for the Mach-Zehnder interferometer and racetrack resonator, respectively. The acousto-optic racetrack cavity exhibits an optomechancial single-photon coupling strength of 1.1 kHz. Our integrated nanophotonic platform coherently leverages the compelling properties of lithium niobate to achieve microwave-to-optical transduction. To highlight the versatility of our system, we also demonstrate a lossless microwave photonic link, which refers to a 0 dB microwave power transmission over an optical channel.

physics.app-ph↗

Phononic band structure engineering for high-Q gigahertz surface acoustic wave resonators on lithium niobate

Phonons at gigahertz frequencies interact with electrons, photons, and atomic systems in solids, and therefore have extensive applications in signal processing, sensing, and quantum technologies. Surface acoustic wave (SAW) resonators that confine surface phonons can play a crucial role in such integrated phononic systems due to small mode size, low dissipation, and efficient electrical transduction. To date, it has been challenging to achieve high quality (Q) factor and small phonon mode size for SAW resonators at gigahertz frequencies. Here, we present a methodology to design compact high-Q SAW resonators on lithium niobate operating at gigahertz frequencies. We experimentally verify out designs and demonstrate Q factors in excess of $2\times10^4$ at room temperature ($6\times10^4$ at 4 Kelvin) and mode area as low as $1.87 λ^2$. This is achieved by phononic band structure engineering, which provides high confinement with low mechanical loss. The frequency-Q products (fQ) of our SAW resonators are greater than $10^{13}$. These high-fQ and small mode size SAW resonators could enable applications in quantum phononics and integrated hybrid systems with phonons, photons, and solid-state qubits.

cond-mat.mes-hall↗

Visualization of Local Conductance in MoS2/WSe2 Heterostructure Transistors

The vertical stacking of van der Waals (vdW) materials introduces a new degree of freedom to the research of two-dimensional (2D) systems. The interlayer coupling strongly influences the band structure of the heterostructures, resulting in novel properties that can be utilized for electronic and optoelectronic applications. Based on microwave microscopy studies, we report quantitative electrical imaging on gated molybdenum disulfide (MoS2)/tungsten diselenide (WSe2) heterostructure devices, which exhibit an intriguing anti-ambipolar effect in the transfer characteristics. Interestingly, in the region with significant source-drain current, electrons in the n-type MoS2 and holes in the p-type WSe2 segments are nearly balanced, whereas the heterostructure area is depleted of mobile charges. The configuration is analogous to the p-i-n diode, where the injected carriers dominate in the recombination current. The spatial evolution of local conductance can be ascribed to the lateral band bending and formation of depletion regions along the line of MoS2-heterostructure-WSe2. Our work vividly demonstrates the microscopic origin of novel transport behaviors, which is important for the vibrant field of vdW heterojunction research.

physics.app-ph↗

Energy-resolved Photoconductivity Mapping in a Monolayer-bilayer WSe2 Lateral Heterostructure

Vertical and lateral heterostructures of van der Waals materials provide tremendous flexibility for band structure engineering. Since electronic bands are sensitively affected by defects, strain, and interlayer coupling, the edge and heterojunction of these two-dimensional (2D) systems may exhibit novel physical properties, which can be fully revealed only by spatially resolved probes. Here, we report the spatial mapping of photoconductivity in a monolayer-bilayer WSe2 lateral heterostructure under multiple excitation lasers. As the photon energy increases, the light-induced conductivity detected by microwave impedance microscopy first appears along the hetero-interface and bilayer edge, then along the monolayer edge, inside the bilayer area, and finally in the interior of the monolayer region. The sequential emergence of mobile carriers in different sections of the sample is consistent with the theoretical calculation of local energy gaps. Quantitative analysis of the microscopy and transport data also reveals the linear dependence of photoconductivity on the laser intensity and the influence of interlayer coupling on carrier recombination. Combining theoretical modeling, atomic scale imaging, mesoscale impedance microscopy, and device-level characterization, our work suggests an exciting perspective to control the intrinsic band-gap variation in 2D heterostructures down to the few-nanometer regime.

cond-mat.mtrl-sci↗

Microwave Conductivity of Ferroelectric Domains and Domain Walls in Hexagonal Rare-earth Ferrite

We report the nanoscale electrical imaging results in hexagonal $Lu_{0.6}Sc_{0.4}FeO_3$ single crystals using conductive atomic force microscopy (C-AFM) and scanning microwave impedance microscopy (MIM). While the dc and ac response of the ferroelectric domains can be explained by the surface band bending, the drastic enhancement of domain wall (DW) ac conductivity is clearly dominated by the dielectric loss due to DW vibration rather than mobile-carrier conduction. Our work provides a unified physical picture to describe the local conductivity of ferroelectric domains and domain walls, which will be important for future incorporation of electrical conduction, structural dynamics, and multiferroicity into high-frequency nano-devices.

cond-mat.mtrl-sci↗

Visualization of Surface-acoustic-wave Potential by Transmission-mode Microwave Impedance Microscopy

Elastic waves propagating in piezoelectric materials are accompanied by a time-varying electric potential, which is of critical importance for acousto-electronic applications. The spatial mapping of such a potential at microwave frequencies is challenging since the characteristic length scale is determined by the acoustic wavelength of several micrometers. In this work, we report the visualization of surface acoustic waves (SAWs) on ferroelectric samples by transmission-mode microwave impedance microscopy (T-MIM). The SAW potential launched by the interdigital transducer is detected by the tip and demodulated by the microwave electronics as time-independent spatial patterns. Wave phenomena such as interference and diffraction are imaged and the results are in excellent agreement with the theoretical analysis. Our work opens up a new avenue to study various electromechanical systems in a spatially resolved manner.

cond-mat.mes-hall↗

Interferometric Imaging of Nonlocal Electromechanical Power Transduction in Ferroelectric Domains

The electrical generation and detection of elastic waves are the foundation for acousto-electronic and acousto-optic systems. For surface-acoustic-wave devices, micro-/nano-electromechanical systems, and phononic crystals, tailoring the spatial variation of material properties such as piezoelectric and elastic tensors may bring significant improvements to the system performance. Due to the much smaller speed of sound than speed of light in solids, it is desirable to study various electroacoustic behaviors at the mesoscopic length scale. In this work, we demonstrate the interferometric imaging of electromechanical power transduction in ferroelectric lithium niobate domain structures by microwave impedance microscopy. In sharp contrast to the traditional standing-wave patterns caused by the superposition of counter-propagating waves, the constructive and destructive fringes in microwave dissipation images exhibit an intriguing one-wavelength periodicity. We show that such unusual interference patterns, which are fundamentally different from the acoustic displacement fields, stem from the nonlocal interaction between electric fields and elastic waves. The results are corroborated by numerical simulations taking into account the sign reversal of piezoelectric tensor in oppositely polarized domains. Our work paves new ways to probe nanoscale electroacoustic phenomena in complex structures by near-field electromagnetic imaging.

cond-mat.mes-hall↗

Quantitative Measurements of Nanoscale Permittivity and Conductivity Using Tuning-fork-based Microwave Impedance Microscopy

We report quantitative measurements of nanoscale permittivity and conductivity using tuning-fork (TF) based microwave impedance microscopy (MIM). The system is operated under the driving amplitude modulation mode, which ensures satisfactory feedback stability on samples with rough surfaces. The demodulated MIM signals on a series of bulk dielectrics are in good agreement with results simulated by finite-element analysis. Using the TF-MIM, we have visualized the evolution of nanoscale conductance on back-gated $MoS_2$ field effect transistors and the results are consistent with the transport data. Our work suggests that quantitative analysis of mesoscopic electrical properties can be achieved by near-field microwave imaging with small distance modulation.

physics.app-ph↗

Direct Imaging of Sketched Conductive Nanostructures at the LaAlO3/SrTiO3 Interface

Nanoscale control of the quasi-two-dimensional electron gas at the LaAlO3/SrTiO3 (LAO/STO) interface by a conductive probe tip has triggered the development of a number of electronic devices. While the spatial distribution of the conductance is crucial for such devices, it is challenging to directly visualize the local electrical properties at the buried interface. Here we demonstrate conductivity imaging of sketched nanostructures at the LAO/STO interface by microwave impedance microscopy (MIM) with a lateral resolution on the order of 100 nm. The sheet conductance extracted from the MIM data agrees with the transport measurement. The tip-induced insulator-to-metal transition is observed above a threshold voltage of +4 V. Our work paves the way to study emergent phenomena at oxide interfaces by probing nanoscale conductance distribution.

cond-mat.mes-hall↗