arXiv subjects

Qihua Xiong

Publications and source records attributed to Qihua Xiong.

At least 19 recordsLinked to original sources

arXiv2026

Electrically reconfigurable dipolar polaritons with highly tunable nonlinearity in a homobilayer microcavity

Active control over optical nonlinearity in solid-state systems is central to unlocking exotic many-body phenomena and photonic devices. While exciton-polaritons in transition metal dichalcogenides (TMDs) offer a promising platform, their practical utility is impeded by fixed interactions and a trade-off between nonlinearity and oscillator strength. Here, we report electrically tunable dipolar polaritons in a dual-gated bilayer MoS2 microcavity, demonstrating in situ reshaping of the dispersion and modulation of the light-matter coupling strength via the quantum-confined Stark effect. Crucially, this electrical control yields a seven-fold enhancement of the polariton-polariton interaction strength. This enhancement arises from the combined tuning of the effective exciton-exciton interaction and the excitonic Hopfield coefficient. In addition, electrostatic doping provides an independent knob to continuously drive a strong-to-weak coupling crossover. Our findings establish dual-gated TMD homobilayer as a versatile platform for on-chip, dynamically reconfigurable nonlinear light-matter physics.

physics.optics↗

arXiv2026

Self-Trapping Enabled Highly Bright Momentum-Indirect Interlayer Excitons

Interlayer excitons in two dimensional material heterostructures exhibit large exciton binding energies and long lifetimes, making them ideal platforms for studying excitonic devices and many body quantum phenomena. However, the spatially separated electron and hole nature of IXs reduces their oscillator strength by two orders of magnitude compared to intralayer excitons. Achieving high efficiency IX emission remains challenging and requires optimal material selection with appropriate momentum matching and meticulous device fabrication. Here we demonstrate a highly bright momentum indirect IX emission within heterostructures formed between 2D perovskites and monolayer transition metal dichalcogenides. The quantum yield of IX emission reaches 35.2% on average, over 50 times higher than that of the corresponding constituent TMD monolayer, with the highest value exceeding 60%. Notably, the radiative recombination efficiency of this momentum indirect IX exceeds that of momentum direct IXs in monolayer TMD-based heterostructures by two orders of magnitude. We suggest that the remarkably bright IX emission in our heterostructure originates from IX self trapping, induced by strong exciton phonon coupling arising from the soft lattice nature of the 2D perovskite. Our findings provide new insights into achieving high IX emission efficiency and open new avenues for exploring long lifetime excitonic devices.

cond-mat.mes-hall↗

arXiv2026

High-energy electronic excitations in La3Ni2O7 by time-resolved optical spectroscopy

Recently, high-temperature superconductivity has been established in bilayer La3Ni2O7, which exhibits a density-wave (DW) transition at ~ 150 K under ambient pressure. The DW order is believed to be linked to superconductivity, as it is suppressed upon the emergence of superconductivity at high pressures. Here, we explore the ultrafast dynamics of high-energy electronic excitations from 10 K to room temperature under ambient pressure using time-resolved optical spectroscopy. Two high-energy electronic excitations at ~1.8 and ~ 2.4 eV, arising from distinct interband transitions, are identified. They exhibit different DW gaps of approximately 54 and 67 meV, respectively, along with relaxation dynamics that can be well described by the Rothwarf-Taylor model. In addition, we observe four coherent Raman-active phonon modes that exhibit distinct coupling with different electronic excitations. The phonon softening with increasing temperature can be well described between ~100 K and room temperature by a semi-quantitative model, which includes thermal expansion and anharmonic phonon-phonon coupling. At cryogenic temperatures, deviations from the measured temperature-dependent phonon frequencies and the model fits suggest an additional contribution from electron-phonon coupling. Our study provides direct evidence of the complex gap structure and phonon dynamics in this material, offering critical insights into the DW mechanism and many-body effects.

cond-mat.supr-con↗

arXiv2025

Low-frequency interlayer phonon dynamics and photoinduced terahertz absorption in black phosphorus

The strong interlayer coupling in black phosphorus (BP), arising from wavefunction overlap between layers, is critical for understanding its electronic and optical properties. Here, we utilize terahertz (THz) spectroscopy to study phonon dynamics in BP. We identify two peaks at 6 and 8.5 meV in steady-state THz spectra, which are attributed to low-frequency interlayer phonon modes. Both modes exhibit anharmonic phonon coupling behavior below 150 K, manifesting as temperature-dependent red-shifts. Using time-resolved THz spectroscopy, we observe significantly increased THz absorption under photoexcitation, arising from the transient enhancements of the extended Drude component and the oscillator strengths of interlayer phonons in non-equilibrium. These findings highlight the critical role of interlayer phonon dynamics in understanding many-body physics in BP.

cond-mat.str-el↗

arXiv2025

Intrinsic exciton transport and recombination in single-crystal lead bromide perovskite

Photogenerated carrier transport and recombination in metal halide perovskites are critical to device performance. Despite considerable efforts, sample quality issues and measurement techniques have limited the access to their intrinsic physics. Here, by utilizing high-purity CsPbBr3 single crystals and contact-free transient grating spectroscopy, we directly monitor exciton diffusive transport from 26 to 300 K. As the temperature (T) increases, the carrier mobility (μ) decreases rapidly below 100 K wtih a μ~T^{-3.0} scaling, and then follows a more gradual μ~T^{-1.7} trend at higher temperatures. First-principles calculations perfectly reproduce this experimental trend and reveal that optical phonon scattering governs carrier mobility shifts over the entire temperature range, with a single longitudinal optical mode dominating room-temperature transport. Time-resolved photoluminescence further identifies a substantial increase in exciton radiative lifetime with temperature, attributed to increased exciton population in momentum-dark states caused by phonon scattering. Our findings unambiguously resolve previous theory-experiment discrepancies, providing benchmarks for future optoelectronic design.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast Chirality-dependent Dynamics from Helicity-resolved Transient Absorption Spectroscopy

Chirality, a pervasive phenomenon in nature, is widely studied across diverse fields including the origins of life, chemical catalysis, drug discovery, and physical optoelectronics. The investigations of natural chiral materials have been constrained by their intrinsically weak chiral effects. Recently, significant progress has been made in the fabrication and assembly of low-dimensional micro and nanoscale chiral materials and their architectures, leading to the discovery of novel optoelectronic phenomena such as circularly polarized light emission, spin and charge flip, advocating great potential for applications in quantum information, quantum computing, and biosensing. Despite these advancements, the fundamental mechanisms underlying the generation, propagation, and amplification of chirality in low-dimensional chiral materials and architectures remain largely unexplored. To tackle these challenges, we focus on employing ultrafast spectroscopy to investigate the dynamics of chirality evolution, with the aim of attaining a more profound understanding of the microscopic mechanisms governing chirality generation and amplification. This review thus provides a comprehensive overview of the chiral micro-/nano-materials, including two-dimensional transition metal dichalcogenides (TMDs), chiral halide perovskites, and chiral metasurfaces, with a particular emphasis on the physical mechanism. This review further explores the advancements made by ultrafast chiral spectroscopy research, thereby paving the way for innovative devices in chiral photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2024

Quantum Interference and Optical Tuning of Self-Trapped Exciton State in Double Halide Perovskite

Self-trapped excitons (STEs), renowned for their unique radiative properties, have been harnessed in diverse photonic devices. Yet, a full comprehension and manipulation of STEs remain elusive. In this study, we present novel experimental and theoretical evidence of the hybrid nature and optical tuning of the STEs state in Cs2Ag0.4Na0.6InCl6. The detection of Fano resonance in the laser energy-dependent Raman and photoluminescence spectra indicates the emergence of an exciton-phonon hybrid state, a result of the robust quantum interference between the discrete phonon and continuous exciton states. Moreover, we showcase the ability to continuously adjust this hybrid state with the energy and intensity of the laser field. These significant findings lay the foundation for a comprehensive understanding of the nature of STE and its potential for state control.

cond-mat.mtrl-sci↗

arXiv2024

Room temperature spin-layer locking of exciton-polariton nonlinearities

Recent advancements in transition metal dichalcogenides (TMDs) have unveiled exceptional optical and electronic characteristics, opened up new opportunities, and provided a unique platform for exploring light-matter interactions under the strong coupling regime. The exploitation of exciton-polaritons, with their peculiar hybrid light-matter properties, for the development of spintronic customizable devices that enhance both the information capacity and functionality at ambient temperatures is often suggested as a promising route. However, although TMD polaritons have shown promising potential, the microscopic mechanisms leading to nonlinearities in TMD polaritons are complex and their spin-anisotropy, a crucial requirement for many proposed polaritonic devices, has been missing. Here, we demonstrate the absence of spin-anisotropic interaction in a monolayer WS2 microcavity (at room temperature) and show how spin-dependent interactions can be controlled and spin anisotropy recovered by engineering double WS2 layer structures with varied interlayer spacing. We attribute this phenomenon to a distinctive feature in exciton-polariton physics: layer-dependent polariton-phonon coupling. We use theoretical calculations of the phonon electrostatic potentials finding a drastically different coupling strength for single and double monolayer samples and discuss qualitatively how this explains the observed spin-anisotropic response. This is further consistent with experiments on multi WS2 layer samples and the identification of a critical separation distance, above which an effective single monolayer spin-anisotropic response is recovered, both in experiment and theory. Our work lays the groundwork for the development of spin-optronic polaritonic devices at room temperature.

physics.optics↗

arXiv2024

Observation of perovskite topological valley exciton-polaritons at room temperature

Topological exciton-polaritons are a burgeoning class of topological photonic systems distinguished by their hybrid nature as part-light, part-matter quasiparticles. Their further control over novel valley degree of freedom (DOF) has offered considerable potential for developing active topological optical devices towards information processing. However, the experimental demonstration of propagating topological exciton-polaritons with valley DOF remains elusive at room temperature. Here, employing a two-dimensional (2D) valley-Hall perovskite lattice, we report the experimental observation of valley-polarized topological exciton-polaritons and their valley-dependent propagations at room temperature. The 2D valley-Hall perovskite lattice consists of two mutually inverted honeycomb lattices with broken inversion symmetry. By measuring their band structure with angle-resolved photoluminescence spectra, we experimentally verify the existence of valley-polarized polaritonic topological kink states with a large gap opening of ~ 9 meV in the bearded interface at room temperature. Moreover, these valley-polarized states exhibit counter-propagating behaviors under a resonant excitation at room temperature. Our results not only expand the landscape of realizing topological exciton-polaritons, but also pave the way for the development of topological valleytronic devices employing exciton-polaritons with valley DOF at room temperature

physics.optics↗

arXiv2024

Exciton polariton critical non-Hermitian skin effect with spin-momentum-locked gains

The critical skin effect, an intriguing phenomenon in non-Hermitian systems, displays sensitivity to system size and manifests distinct dynamical behaviors. In this work, we propose a novel scheme to achieve the critical non-Hermitian skin effect of exciton polaritons in an elongated microcavity system. We show that by utilising longitudinal-transverse spin splitting and spin-momentum-locked gain, a critical non-Hermitian skin effect can be achieved in a continuous system without the need of an underlying lattice. We find that a phase transition can be induced by changing the cavity detuning with respect to the exciton energy. We identify a measurable order parameter associated with this phase transition and demonstrate the corresponding critical behavior. Our work offers a flexible approach to manipulate non-Hermitian phases of exciton polaritons, thereby expanding the potential applications of polaritonic devices.

physics.optics↗

arXiv2024

Three-dimensional hidden phase probed by in-plane magnetotransport in kagome metal CsV$_3$Sb$_5$ thin flakes

Transition metal compounds with kagome structure have been found to exhibit a variety of exotic structural, electronic, and magnetic orders. These orders are competing with energies very close to each other, resulting in complex phase transitions. Some of the phases are easily observable, such as the charge density wave (CDW) and the superconducting phase, while others are more challenging to identify and characterize. Here we present magneto-transport evidence of a new phase below ~35 K in the kagome topological metal CsV$_3$Sb$_5$ (CVS) thin flakes between the CDW and the superconducting transition temperatures. This phase is characterized by six-fold rotational symmetry in the in-plane magnetoresistance (MR) and is connected to the orbital current order in CVS. Furthermore, the phase is characterized by a large in-plane negative magnetoresistance, which suggests the existence of a three-dimensional, magnetic field-tunable orbital current ordered phase. Our results highlight the potential of magneto-transport to reveal the interactions between exotic quantum states of matter and to uncover the symmetry of such hidden phases.

cond-mat.str-el↗

arXiv2024

Ultrafast Photocurrent Hysteresis in Photoferroelectric α-In2Se3

The photon-electron interactions are generally volatile and the intricate multiphysics details of photoexcited carrier dynamics are not yet distinguished. How to nonvolatile control the physical state through all-optical means and clarify the intricate physical processes has been a long-term goal pursued in polar materials. Photoferroelectric α-In2Se3 holds the great potential for capturing multimodal nonvolatile states due to the spontaneous reversible in-plane and out-of-plane polarizations and its tunable light-matter interactions arising from the electronic degree of freedom. Here we uncover a nonvolatile zero-bias ultrafast photocurrent hysteresis response with an all-optical scheme, diagnosed by in-plane and out-of-plane terahertz waves emitted from the photoferroelectric α-In2Se3. The mechanism of such ultrafast photocurrent hysteresis emerges as a result of anomalous bulk linear and circular photovoltaic effect synchronously driven by local polarization rearrangement. Utilizing anisotropic ferroelectric kinetics-induced relative phase between the in-plane and out-of-plane directions, we further show flexibly selective chirality, tunable rotational angle, and optimizable ellipticity of terahertz wave polarizations. Our finding offers a promising avenue towards direct ultrafast nonvolatile processing of photocurrent signals through an all-optical scheme.

physics.optics↗

arXiv2024

Anomalous Quantum Propagation of Microcavity Exciton Polaritons

Here, we explore the quantum propagation of exciton polaritons in semiconductor microcavities, exhibiting intriguing effects such as interactions, decay, and disorder scatterings. Our investigation uncovers anomalies in their quantum propagation, deviating from predictions based on existing theories. By applying scaling theory, we elucidate the true nature of exciton polariton propagation, unveiling a localization phase that characteristically differs from Anderson localization. Our numerical results agree with the self-consistent theory developed for exciton polariton condensates, incorporating non-linearity and finite lifetime.

cond-mat.mes-hall↗

arXiv2024

Impact of bright-dark exciton thermal population mixing on the brightness of CsPbBr$_3$ nanocrystals

Understanding the interplay between bright and dark exciton states is crucial for deciphering the luminescence properties of low-dimensional materials. The origin of the outstanding brightness of lead halide perovskites remains elusive. Here, we analyse temperature-dependent time-resolved photoluminescence to investigate the population mixing between bright and dark exciton sublevels in individual CsPbBr$_3$ nanocrystals in the intermediate confinement regime. We extract bright and dark exciton decay rates, and show quantitatively that the decay dynamics can only be reproduced with second-order phonon transitions. Furthermore, we find that any exciton sublevel ordering is compatible with the most likely population transfer mechanism. The remarkable brightness of lead halide perovskite nanocrystals rather stems from a reduced asymmetry between bright-to-dark and dark-to-bright conversion originating from the peculiar second-order phonon-assisted transitions that freeze bright-dark conversion at low temperature together with the very fast radiative recombination and favourable degeneracy of the bright exciton state.

cond-mat.mes-hall↗

arXiv2024

Estimating many properties of a quantum state via quantum reservoir processing

Estimating properties of a quantum state is an indispensable task in various applications of quantum information processing. To predict properties in the post-processing stage, it is inherent to first perceive the quantum state with a measurement protocol and store the information acquired. In this work, we propose a general framework for constructing classical approximations of arbitrary quantum states with quantum reservoirs. A key advantage of our method is that only a single local measurement setting is required for estimating arbitrary properties, while most of the previous methods need exponentially increasing number of measurement settings. To estimate $M$ properties simultaneously, the size of the classical approximation scales as $\ln M$ . Moreover, this estimation scheme is extendable to higher-dimensional systems and hybrid systems with non-identical local dimensions, which makes it exceptionally generic. We support our theoretical findings with extensive numerical simulations.

quant-ph↗

arXiv2024

Room-temperature continuous-wave pumped exciton polariton condensation in a perovskite microcavity

Microcavity exciton polaritons (polaritons) as part-light part-matter quasiparticles, garner significant attention for non-equilibrium Bose-Einstein condensation at elevated temperatures. Recently, halide perovskites have emerged as promising room-temperature polaritonic platforms thanks to their large exciton binding energies and superior optical properties. However, currently, inducing room-temperature non-equilibrium polariton condensation in perovskite microcavities requires optical pulsed excitations with high excitation densities. Herein, we demonstrate continuous-wave optically pumped polariton condensation with an exceptionally low threshold of ~0.6 W cm-2 and a narrow linewidth of ~1 meV. Polariton condensation is unambiguously demonstrated by characterizing the nonlinear behavior and coherence properties. We also identify a microscopic mechanism involving the potential landscape in the perovskite microcavity, where numerous discretized energy levels arising from the hybridization of adjacent potential minima enhance the polariton relaxation, facilitating polariton condensate formation. Our findings lay the foundation for the next-generation energy-efficient polaritonic devices operating at room temperature.

physics.optics↗

arXiv2024

Direct evidence of interfacial coherent electron-phonon coupling in single-unit-cell FeSe film on Nb-doped SrTiO3

The interface-enhanced superconductivity in monolayer iron selenide (FeSe) films on SrTiO3 has been actively pursued in the past decade. Although a synergistic effect between interfacial charge transfer and interfacial electron-phonon coupling (EPC) is proposed to be responsible for the mechanism, the microscopic nature of the interfacial EPC in the enhancement of superconductivity remains highly controversial. Herein we experimentally reveal that a coherent optical phonon mode at 4.2 THz from the SrTiO3 substrate couples to FeSe electrons and modulates the quasiparticle relaxations using ultrafast pump-probe spectroscopy. This mode originates from the antiferrodistortive (AFD) transition in SrTiO3 and is significantly stronger in the presence of monolayer FeSe than that in purely FeTe-capped Nb-doped SrTiO3. Pump fluence and temperature-dependent spectroscopy measurements suggest that SrTiO3 substrate facilitates the stabilization of FeSe structure and possibly prevents the occurrence of nematic phase transition, supporting that SrTiO3 substrate modifies the electronic structure of monolayer FeSe through a strong interfacial EPC strength as large as 0.77. Our results provide unprecedented direct evidence that the strong coupling of SrTiO3 coherent phonon to FeSe electrons is indeed responsible for the high-temperature superconductivity in monolayer FeSe and SrTiO3 heterostructure.

cond-mat.supr-con↗

arXiv2023

Bulk photovoltaic effect in two-dimensional ferroelectric semiconductor $α$-In$_2$Se$_3$

Bulk photovoltaic effect, which arises from crystal symmetry-driven charge carrier separation, is an intriguing physical phenomenon that has attracted extensive interest in photovoltaic application due to its junction-free photovoltaic and potential to surpass Shockley-Queisser limit. Whereas conventional ferroelectric materials mostly suffer from extremely low photocurrent density and weak photovoltaic response at visible light wavelengths. Emerging two-dimensional ferroelectric semiconductors with coupled visible light absorption and spontaneous polarization characteristics are a promising alternative for making functional photoferroelectrics. Herein, we report the experimental demonstration of the bulk photovoltaic effect behavior based on the 2D ferroelectric semiconductor {$α$-InSe caused by an out-of-plane polarization induced depolarization field. The {$α$-InSe device exhibits enhanced bulk photovoltaic response in the visible light spectrum owing to its narrow bandgap. It was demonstrated that the generated photovoltaic current density was nearly two orders of magnitude greater than conventional bulk ferroelectric materials. These findings highlight the potential of 2D ferroelectric semiconductor materials for bulk photovoltaic applications in a broad spectral region.

cond-mat.mtrl-sci↗