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Yanhao Tang

Publications and source records attributed to Yanhao Tang.

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Gate-tunable chiral spin mode in WSe2/WS2 moir\'e superlattices

The interplay between many-body and spin-orbit effects (SOC) can lead to novel phenomena in solids. Chiral spin modes (CSM) are collective spin excitations that arise from such interplay and connect states with opposite chirality, which, however, have been rarely observed. Here, we report a gate-tunable CSM that occurs between conduction SOC-split minibands in near-0{\deg}-twisted WSe2/WS2 bilayers. This mode manifests as a sharp resonance with giant Raman efficiency in the pseudovector-symmetry channel of the Raman spectra. By varying fillings, the CSM transitions from chiral spin exciton to excitonic polaron. The spin-flip nature is directly confirmed by the Zeeman effect. Moreover, the filling dependence compellingly evidences a charge-transfer insulator at filling of one. Our results demonstrate transition-metal-dichalcogenides moir\'e superlattices as a fertile platform for exploring exotic low-lying collective excitations.

cond-mat.mes-hall

Catalogue of chiral phonon materials

Chiral phonons, circularly polarized lattice vibrations carrying intrinsic angular momentum, offer unprecedented opportunities for controlling heat flow, manipulating quantum states through spin-phonon coupling, and realizing exotic transport phenomena. Despite their fundamental importance, a universal framework for identifying and classifying these elusive excitations has remained out of reach. Here, we address this challenge by establishing a comprehensive symmetry-based theory that systematically classifies the helicity and the velocity-angular momentum tensor underlying phonon magnetization in thermal transport across all 230 crystallographic space groups. Our approach, grounded in fundamental representations of phononic angular momentum, reveals three distinct classes of crystals: achiral crystals with vanishing angular momentum, chiral crystals with s-wave helicity, and achiral crystals exhibiting higher-order helicity patterns beyond the s-wave. By performing high-throughput computations and symmetry analysis of the dynamical matrices for 11614 crystalline compounds, we identified 2738 materials exhibiting chiral phonon modes and shortlisted the 170 most promising candidates for future experimental investigation. These results are compiled into an open-access Chiral Phonon Materials Database website, enabling rapid screening for materials with desired chiral phonon properties. Our theoretical framework transcends phonons--it provides a universal paradigm for classifying chiral excitations in crystalline lattices, from magnons to electronic quasiparticles.

cond-mat.mtrl-sci

Gate-tunable hot electron extraction in a two-dimensional semiconductor heterojunction

Hot carrier solar cells (HCSCs), harvesting excess energy of the hot carriers generated by above-band-gap photoexcitation, is crucial for pushing the solar cell efficiency beyond the Shockley Queisser limit, which is challenging to realize mainly due to fast hot-carrier cooling. By performing transient reflectance spectroscopy in a MoSe2/hBN/WS2 junction, we demonstrate the gate-tunable harvest of hot electrons from MoSe2 to WS2. By spectrally distinguishing hot-electron extraction from lattice temperature increase, we find that electrostatically doped electrons in MoSe2 can boost hot-electron extraction density (n_ET) by factor up to several tens. Such enhancement arises from interaction between hot excitons and doped electrons, which converts the excess energy of hot excitons to excitations of the Fermi sea and hence generates hot electrons. Moreover, n_ET can be further enhanced by reducing the conduction band offset with external electric field. Our results provide in-depth insights into design of HCSCs with electrostatic strategies.

cond-mat.mes-hall

Frustrated magnetic interactions in a Wigner-Mott insulator

Two-dimensional semiconductor moir\'e materials have emerged as a highly controllable platform to simulate and explore quantum condensed matter. Compared to real solids, electrons in semiconductor moir\'e materials are less strongly attracted to the moir\'e lattice sites, making the nonlocal contributions to the magnetic interactions as important as the Anderson super-exchange. It provides a unique platform to study the effects of competing magnetic interactions. Here, we report the observation of strongly frustrated magnetic interactions in a Wigner-Mott insulating state at 2/3 filling of the moir\'e lattice in angle-aligned WSe2/WS2 heterobilayers. Magneto-optical measurements show that the net exchange interaction is antiferromagnetic for filling factors below 1 with a strong suppression at 2/3 filling. The suppression is lifted upon screening of the long-range Coulomb interactions and melting of the Wigner-Mott insulator by a nearby metallic gate. The results can be qualitatively captured by a honeycomb-lattice spin model with an antiferromagnetic nearest-neighbor coupling and a ferromagnetic second-neighbor coupling. Our study establishes semiconductor moir\'e materials as a model system for the lattice-spin physics and frustrated magnetism.

cond-mat.mtrl-sci

Dielectric catastrophe at the Mott and Wigner transitions in a moir\'e superlattice

The metal-insulator transition (MIT) driven by electronic correlations is a fundamental and challenging problem in condensed-matter physics. Particularly, whether such a transition can be continuous remains open. The emergence of semiconducting moir\'e materials with continuously tunable bandwidth provides an ideal platform to study interaction-driven MITs. Although a bandwidth-tuned MIT at fixed full electron filling of the moir\'e superlattice has been reported recently, that at fractional filling, which involves translational symmetry breaking of the underlying superlattice, remains elusive. Here, we demonstrate bandwidth-tuned MITs in a MoSe2/WS2 moir\'e superlattice at both integer and fractional fillings using the exciton sensing technique. The bandwidth is controlled by an out-of-plane electric field. The dielectric response is probed optically with the 2s exciton in a remote WSe2 sensor layer. The exciton spectral weight is negligible for the metallic state, consistent with a large negative dielectric constant. It continuously vanishes when the transition is approached from the insulating side, corresponding to a diverging dielectric constant or a "dielectric catastrophe". Our results support continuous interaction-driven MITs in a two-dimensional triangular lattice and stimulate future explorations of exotic quantum phases, such as quantum spin liquids, in their vicinities.

cond-mat.mtrl-sci

Charge-order-enhanced capacitance in semiconductor moir\'e superlattices

Van der Waals moir\'e materials have emerged as a highly controllable platform to study the electronic correlation phenomena. In particular, robust correlated insulating states have recently been discovered at both integer and fractional filling factors of the semiconductor moir\'e systems. Here, we reveal the thermodynamic properties of these states by measuring the gate capacitance of MoSe2/WS2 moir\'e superlattices. We observe a series of incompressible states for filling factor 0 - 8 and anomalously large capacitance (nearly 60% above the device's geometrical capacitance) in the intervening compressible regions. The anomalously large capacitance is most pronounced at small filling factor, below the melting temperature of the charge-ordered states, and for small sample-gate separation. It is a manifestation of the device-geometry-dependent Coulomb interaction between electrons and phase mixing of the charge-ordered states. We have further extracted the thermodynamic gap of the correlated insulating states and the entropy of the capacitive device. The results not only establish capacitance as a powerful probe of the correlated states in semiconductor moir\'e systems, but also demonstrate control of the extended Coulomb interaction in these materials via sample-gate coupling.

cond-mat.str-el

Direct observation of distinct minibands in moir\'e superlattices

Moir\'e superlattices comprised of stacked two-dimensional materials present a versatile platform for engineering and investigating new emergent quantum states of matter. At present, the vast majority of investigated systems have long moir\'e wavelengths, but investigating these effects at shorter, incommensurate wavelengths, and at higher energy scales, remains a challenge. Here, we employ angle-resolved photoemission spectroscopy (ARPES) with sub-micron spatial resolution to investigate a series of different moir\'e superlattices which span a wide range of wavelengths, from a short moir\'e wavelength of 0.5 nm for a graphene/WSe2 (g/WSe2) heterostructure, to a much longer wavelength of 8 nm for a WS2/WSe2 heterostructure. We observe the formation of minibands with distinct dispersions formed by the moir\'e potential in both systems. Finally, we discover that the WS2/WSe2 heterostructure can imprint a surprisingly large moir\'e potential on a third, separate layer of graphene (g/WS2/WSe2), suggesting a new avenue for engineering moir\'e superlattices in two-dimensional materials.

cond-mat.mtrl-sci

Stripe phases in WSe2/WS2 moir\'e superlattices

Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions. One representative example is the copper-oxide superconductors, where stripe order is thought to be relevant to the mechanism of high-temperature superconductivity. Identifying and studying the stripe phases in conventional strongly correlated systems are, however, challenging due to the complexity and limited tunability of these materials. Here we uncover stripe phases in WSe2/WS2 moir\'e superlattices with continuously gate-tunable charge densities by combining optical anisotropy and electronic compressibility measurements. We find strong electronic anisotropy over a large doping range peaked at 1/2 filling of the moir\'e superlattice. The 1/2-state is incompressible and assigned to a (insulating) stripe crystal phase. It can be continuously melted by thermal fluctuations around 35 K. The domain configuration revealed by wide-field imaging shows a preferential alignment along the high-symmetry axes of the moir\'e superlattice. Away from 1/2 filling, we observe additional stripe crystals at commensurate filling 1/4, 2/5 and 3/5. The anisotropy also extends into the compressible regime of the system at incommensurate fillings, indicating the presence of electronic liquid crystal states. The observed filling-dependent stripe phases agree with the theoretical phase diagram of the extended Hubbard model on a triangular lattice in the flat band limit. Our results demonstrate that two-dimensional semiconductor moir\'e superlattices are a highly tunable platform to study the stripe phases and their interplay with other symmetry breaking ground states.

cond-mat.mes-hall

Creation of moir\'e bands in a monolayer semiconductor by spatially periodic dielectric screening

Moir\'e superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moir\'e bands in a crystal through interlayer hybridization when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moir\'e bands in a monolayer semiconductor. It relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their environmental dielectric-dependent electronic band structure. We observe optical transitions between moir\'e bands in monolayer WSe$_{2}$ when it is placed close to small angle-misaligned graphene on hexagonal boron nitride. The moir\'e bands are a result of long-range Coulomb interactions, strongly gate-tunable, and can have versatile superlattice symmetries independent of the crystal lattice of the host material. Our result also demonstrates that monolayer semiconductors are sensitive local dielectric sensors.

cond-mat.mtrl-sci

Spatially mixed moir\'e excitons in two-dimensional van der Waals superlattices

Moir\'e superlattices open an unprecedented opportunity for tailoring interactions between quantum particles and their coupling to electromagnetic fields. Strong superlattice potential generates moir\'e minibands of excitons -- bound pairs of electrons and holes that reside either in a single layer (intralayer excitons) or two separate layers (interlayer excitons). The twist-angle-controlled interlayer hybridization of carriers can also mix the two types of excitons to combine the strengths of both. Here, we report a direct observation of spatially mixed moir\'e excitons in angle-aligned WSe2/WS2 and MoSe2/WS2 superlattices by optical reflectance spectroscopy. The strongly interacting interlayer and intralayer moir\'e excitons in WSe2/WS2 manifest energy level anticrossing and oscillator strength redistribution under a vertical electric field. We also observe doping-dependent exciton miniband renormalization and mixing near half filling of the first electron miniband of WS2. Our findings have significant implications for emerging correlated states in two-dimensional semiconductors, such as exciton condensates and Bose-Hubbard models, and optoelectronic applications of these materials.

cond-mat.mtrl-sci

WSe2/WS2 moir\'e superlattices: a new Hubbard model simulator

The Hubbard model, first formulated by physicist John Hubbard in the 1960s, is a simple theoretical model of interacting quantum particles in a lattice. The model is thought to capture the essential physics of high-temperature superconductors, magnetic insulators, and other complex emergent quantum many-body ground states. Although the Hubbard model is greatly simplified as a representation of most real materials, it has nevertheless proved difficult to solve accurately except in the one-dimensional case. Physical realization of the Hubbard model in two or three dimensions, which can act as quantum simulators, therefore have a vital role to play in solving the strong-correlation puzzle. Here we obtain a quantum phase diagram of the two-dimensional triangular lattice Hubbard model by studying angle-aligned WSe2/WS2 bilayers, which form moir\'e superlattices because of the difference in lattice constant between the two two-dimensional materials. We probe both charge and magnetic properties of the system by measuring the dependence of optical response on out-of-plane magnetic field, and on gate-tuned carrier density. At half filling of the first hole moir\'e superlattice band, we observe a Mott insulating state with antiferromagnetic Curie-Weiss behavior as expected for a Hubbard model in the strong interaction regime. Past half filling, our experiment suggests an antiferromagnetic to paramagnetic quantum phase transition near 0.6 filling. Our results establish a new solid-state platform based on moir\'e superlattices which can be used to simulate outstanding problems in strong correlation physics that are manifested by triangular lattice Hubbard models.

cond-mat.mtrl-sci

Long valley lifetime of dark excitons in single-layer WSe2

Single-layer transition metal dichalcogenides (TMDs) provide a promising material system to explore the electron's valley degree of freedom as a quantum information carrier. The valley degree of freedom in single-layer TMDs can be directly accessed by means of optical excitation. The rapid valley relaxation of optically excited electron-hole pairs (excitons) through the long-range electron-hole exchange interaction, however, has been a major roadblock. Theoretically such a valley relaxation does not occur for the recently discovered dark excitons, suggesting a potential route for long valley lifetimes. Here we investigate the valley dynamics of dark excitons in single-layer WSe2 by time-resolved photoluminescence spectroscopy. We develop a waveguide-based method to enable the detection of the dark exciton emission, which involves spin-forbidden optical transitions with an out-of-plane dipole moment. The valley degree of freedom of dark excitons is accessed through the valley-dependent Zeeman effect under an out-of-plane magnetic field. We find a short valley lifetime for the dark neutral exciton, likely due to the short-range electron-hole exchange, but long valley lifetimes exceeding several nanoseconds for dark charged excitons.

cond-mat.mes-hall

Optical Stark metrology of CdSe quantum dots: Reconciling the size-dependent oscillator strength with theory

The $k\cdot p$ effective mass approximation (EMA) predicts large, nearly size-independent exciton oscillator strengths in quantum confined semiconductors. Yet, experimental reports have concluded that the total oscillator strength of the lowest-energy (1S$_{3/2}$1S$_{\text{e}}$) excitons in strongly confined CdSe NQDs is small and strongly size-dependent. Using the optical Stark effect, we show that the oscillator strength of the 1S$_{3/2}$1S$_{\text{e}}$ excitonic absorption peak in CdSe NQDs follows the predictions of the EMA. These oscillator strengths enable helicity-selective unsaturated Stark shifts corresponding to femtosecond pseudo-magnetic fields exceeding 100 T.

cond-mat.mes-hall

Layer- and Frequency-Dependent Second Harmonic Generation in Reflection from GaSe Atomic Crystals

We report optical second-harmonic generation (SHG) in reflection from GaSe crystals of 1 to more than 100 layers using a fundamental picosecond pulsed pump at 1.58 eV and a supercontinuum white light pulsed laser with energies ranging from 0.85 to 1.4 eV. The measured reflected SHG signal is maximal in samples of $\sim$20 layers, decreasing in thicker samples as a result of interference. The thickness- and frequency-dependence of the SHG response of samples thicker than $\sim$7 layers can be reproduced by a second-order optical susceptibility that is the same as in bulk samples. For samples $\lesssim$7 layers, the second-order optical susceptibility is reduced compared to that in thicker samples, which is attributed to the expected bandgap increase in mono- and few-layer GaSe.

cond-mat.mes-hall

Exciton spin dynamics in GaSe

We analyze exciton spin dynamics in GaSe under nonresonant circularly polarized optical pumping with an exciton spin-flip rate-equation model. The model reproduces polarized time-dependent photoluminescence measurements in which the initial circular polarization approaches unity even when pumping with 0.15 eV excess energy. At T = 10 K, the exciton spin relaxation exhibits a biexponential decay with a sub-20 ps and a >500 ps time constants, which are also reproduced by the rate-equation model assuming distinct spin-relaxation rates for hot (nonequilibrium) and cold band-edge excitons.

cond-mat.mes-hall

Linearly polarized remote-edge luminescence in GaSe nanoslabs

We report highly linearly polarized remote luminescence that emerges at the cleaved edges of nanoscale gallium selenide slabs tens of micrometers away from the optical excitation spot. The remote-edge luminescence (REL) measured in the reflection geometry has a degree of linear polarization above 0.90, with polarization orientation pointing toward the photoexcitation spot. The REL is dominated by an index-guided optical mode that is linearly polarized along the crystalline $c$-axis. This luminescence is from out-of-plane dipoles that are converted from in-plane dipoles through a spin-flip process at the excitation spot.

cond-mat.mes-hall

Near Unity Optical Spin Polarization in GaSe Nanoslabs

We report nearly complete preservation of "spin memory" between optical absorption and photoluminescence (PL) in nanometer slabs of GaSe pumped with 0.2 eV excess energy. At cryogenic temperatures, the initial degree of circular polarization ($\rho_0$) of PL approaches unity, with the major fraction of the spin polarization decaying with a time constant $>$500 ps in sub-100-nm GaSe nanoslabs. Even at room temperature, $\rho_0$ as large as 0.7 is observed, while pumping 1 eV above the band edge yields $\rho_0$ = 0.15. Angular momentum preservation for both electrons and holes is due to the separation of the non-degenerate conduction and valence bands from other bands. In contrast to valley polarization in atomically thin TMDs, here optical spin polarization is preserved in nanoslabs of 100 layers or more of GaSe.

cond-mat.mes-hall