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Qiuyang Li

Publications and source records attributed to Qiuyang Li.

15 recordsLinked to original sources

Janus Dipoles: Fundamentals, Realizations, and Emerging Applications

The Janus dipole - featuring orthogonally oriented electric and magnetic dipoles with a 90-degree phase difference - has emerged as a powerful paradigm for wave manipulation. Unlike traditional Huygens dipoles used for directional control, this unique configuration exhibits strongly asymmetric, face-selective near-field behavior while maintaining a quasi-isotropic far-field radiation pattern. These remarkable properties make the Janus dipole an essential platform for directional wave shaping, with wide-ranging applications in on-chip photonics, quantum interactions, and wireless power transfer. This review systematically traces the rapid development of the Janus dipole from its foundational theoretical inception to its diverse implementation platforms across optical, microwave, and acoustic frequencies. In this paper, we explore the governing principles, classify realization strategies into passive Janus dipoles, active Janus dipoles, and advanced near-field coupling control, and highlight emerging frontiers. By bridging foundational electrodynamics with advanced device engineering, this paper serves as an essential reference and roadmap for researchers designing next-generation, highly integrated, and compact wave-manipulation systems.

physics.app-ph

Magneto-Moiré Excitons in Twisted Bilayer CrSBr

Moiré superlattices in van der Waals materials have revolutionized the study of electronic and excitonic systems by creating periodic electrostatic potentials. Extending this concept to magnetic materials promises new pathways in merging spintronics with photonics. While moiré magnetism has been revealed with near-field probes and nonlinear optical techniques, the coupling of these magnetic textures to optical excitations - magneto-moiré excitons - remains unexplored. Here, we report the observation of magneto-moiré excitons in twisted bilayer CrSBr, correlated with moiré spin textures that emerge below a critical twist angle of ~2°. The nanoscale moiré spin texture imprints distinct signatures onto the optical spectrum, shifting the exciton energy via a periodic magnetic exchange field. First-principles calculations corroborate that these signatures arise from one-dimensional spin textures governed by the balance of exchange interactions and domain wall energy. Our results demonstrate that moiré magnetism can be used to engineer nanoscale excitonic energy landscapes, providing a new platform for magneto-optical sensing, quantum transduction, and control of non-collinear magnetism and topology through light.

cond-mat.mes-hall

Enhanced second-harmonic generation from WS$_2$/ReSe$_2$ heterostructure

Van der Waals stacking presents new opportunities for nonlinear optics with its remarkable tunability and scalability. However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this letter, we report an anisotropic enhancement of second-harmonic generation (SHG) from a WS$_2$/ReSe$_2$ heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.

cond-mat.mtrl-sci

Determining the complex second-order optical susceptibility in macroscale van der Waals heterobilayers

We report on the experimental characterization of the second-order susceptibility in MoSe$_2$/WS$_2$ heterobilayers, including their hidden complex phases. To this end, we developed a heterodyne-detection scheme for second-harmonic generation and applied it to macroscale heterobilayer samples prepared using the gold-tape exfoliation method. The heterodyne scheme enabled us to distinguish the relative orientation of the crystal domains, and further, it allowed us to characterize the complex phases of the susceptibility relative to a reference quartz sample. By comparing the results from the monolayer regions and the heterobilayer region over several hundred microns of the sample area, we determined that the contribution of interlayer effects to second-harmonic generation is within the experimental uncertainty arising from the sample inhomogeneity. The results here provide fundamental quantitative information necessary for the precise design of nanophotonic systems based on stacking engineering.

cond-mat.mtrl-sci

2D material exciton-polariton transport on 2D photonic crystals

Transport of elementary excitations is a fundamental property of 2D semiconductors, important for wide-ranging emergent phenomena and device applications. While exciton transport reported in 2D materials barely exceeds 1-2 $μ$m, coherent coupling of excitons with photons to form polaritons allows not only greatly enhanced transport length, but also the potential to leverage photonic mode engineering for novel transport properties. However, conventional vertical cavity or waveguide polaritons are difficult to tune or integrate into photonic circuits. Here, we report the transport of transition-metal dichalcogenide polaritons in slab 2D photonic crystals that are highly versatile for tuning, mode-engineering and integration. We show an order-of-magnitude enhancement of the transport length compared to that of bare excitons. We further show the dependence of transport on the polariton dispersion and population dynamics, which we control by varying the photonic crystal design and pumping intensity. Stimulated relaxation observed in the system suggests the potential for forming superfluid polaritons with frictionless transport. These results demonstrate the 2D photonic crystal polariton system as a versatile platform to enhance and manipulate energy transport for novel photonic technologies.

physics.optics

Twist Engineering of Anisotropic Excitonic and Optical Properties of a Two-Dimensional Magnetic Semiconductor

Two dimensional (2D) van der Waals (vdW) magnetic semiconductors are a new class of quantum materials for studying the emergent physics of excitons and spins in the 2D limit. Twist engineering provides a powerful tool to manipulate the fundamental properties of 2D vdW materials. Here, we show that twist engineering of the anisotropic ferromagnetic monolayer semiconductor, CrSBr, leads to bilayer magnetic semiconductors with continuously tunable magnetic moment, dielectric anisotropy, exciton energy and linear dichroism. We furthermore provide a model for exciton energy in the media with tunable anisotropy. These results advance fundamental studies on 2D vdW materials and open doors to applications to nano-optics, twistronics, and spintronics.

cond-mat.mes-hall

Unveiling Ultrafast Spin-Valley Dynamics and Phonon-Mediated Charge Transfer in MoSe$_{2}$/WSe$_{2}$ Heterostructures

We use helicity-resolved ultrafast transient absorption spectroscopy to study spin-valley polarization dynamics in a vertically stacked MoSe$_{2}$/WSe$_{2}$ heterostructure. The experimental findings reveal details of interlayer charge transfer on ultrafast timescales, showing that the spin-valley polarized state of photoexcited carriers is conserved during the charge transfer and formation of interlayer excitons. Our results confirm that phonon scattering mediates the interlayer charge transfer process, while a high phonon population at elevated temperatures causes a significant decrease in spin-valley selective charge transfer. Moreover, the experimental findings demonstrate the possibility that interlayer excitons and their spin-valley polarization can be probed in the optical response of intralayer excitons. These findings pave the way for ultrafast detection, control, and manipulation of spin-valley polarized excitons in transition metal dichalcogenide-based 2D heterostructures.

physics.app-ph

Large Exciton Binding Energy in the Bulk van der Waals Magnet CrSBr

Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid state systems. Excitons and their associated many-body physics are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an exceptionally large exciton binding energy in single crystals of the bulk van der Waals antiferromagnet CrSBr. Utilizing state-of-the-art angle-resolved photoemission spectroscopy and self-consistent ab-initio GW calculations, we present direct spectroscopic evidence that robust electronic and structural anisotropy can significantly amplify the exciton binding energy within bulk crystals. Furthermore, the application of a vertical electric field enables broad tunability of the optical and electronic properties. Our results indicate that CrSBr is a promising material for the study of the role of anisotropy in strongly interacting bulk systems and for the development of exciton-based optoelectronics.

cond-mat.mtrl-sci

Magnetic Exciton-Polariton with Strongly Coupled Atomic and Photonic Anisotropies

Anisotropy plays a key role in science and engineering. However, the interplay between the material and engineered photonic anisotropies has hardly been explored due to the vastly different length scales. Here we demonstrate a matter-light hybrid system, exciton-polaritons in a 2D antiferromagnet, CrSBr, coupled with an anisotropic photonic crystal (PC) cavity, where the spin, atomic lattice, and photonic lattices anisotropies are strongly correlated, giving rise to unusual properties of the hybrid system and new possibilities of tuning. We show exceptionally strong coupling between engineered anisotropic optical modes and anisotropic excitons in CrSBr, which is stable against excitation densities a few orders of magnitude higher than polaritons in isotropic materials. Moreover, the polaritons feature a highly anisotropic polarization tunable by tens of degrees by controlling the matter-light coupling via, for instance, spatial alignment between the material and photonic lattices, magnetic field, temperature, cavity detuning and cavity quality-factors. The demonstrated system provides a prototype where atomic- and photonic-scale orders strongly couple, opening opportunities of photonic engineering of quantum materials and novel photonic devices, such as compact, on-chip polarized light source and polariton laser.

physics.optics

Dimensionality crossover to 2D vestigial nematicity from 3D zigzag antiferromagnetism in an XY-type honeycomb van der Waals magnet

Fluctuations and disorder effects are substantially enhanced in reduced dimensionalities. While they are mostly considered as the foe for long-range orders, fluctuations and disorders can also stimulate the emergence of novel phases of matter, for example, vestigial orders. Taking 2D magnetism as a platform, existing efforts have been focused on maintaining 2D long-range magnetic orders by suppressing fluctuations, whereas the other side, exploiting fluctuations for realizing new 2D magnetic phases, remains as an uncharted territory. Here, using a combination of NV spin relaxometry, optical spectroscopy, and Monte Carlo simulations, we report, in an XY-type honeycomb magnet NiPS3, the phase transition from the zigzag AFM order in 3D bulk to a new Z3 vestigial Potts-nematicity in 2D few layers. Spin fluctuations are shown to significantly enhance over the GHz-THz range as the layer number of NiPS3 reduces, using the NV spin relaxometry and the optical Raman quasi-elastic scattering. As a result, the Raman signatures of the zigzag AFM for bulk NiPS3, a zone-folded phonon at ~30cm-1 from the broken translational symmetry (PBTS) and a degeneracy lift of two phonons at ~180cm-1 for the broken 3-fold rotational symmetry (PBRS), evolve into the disappearance of PBTS and the survival of PBRS in few-layer NiPS3, with a critical thickness of ~10nm. The optical linear dichroism microscopy images all three nematic domain states in a single few-layer NiPS3 flake. The large-scale Monte Carlo simulations for bilayer NiPS3 model confirms the absence of long-range zigzag AFM order but the formation of the Z3 vestigial Potts-nematic phase, corroborating with the experimental finding. Our results demonstrate the positivity of strong fluctuations in creating new phases of matter after destroying more conventional ones, and offer an unprecedented pathway for developing novel 2D phases.

cond-mat.mtrl-sci

Time-domain observation of interlayer exciton formation and thermalization in a MoSe$_2$/WSe$_2$ heterostructure

Vertical heterostructures (HS) of transition metal dichalcogenides (TMDs) host interlayer excitons (ILX), with electrons and holes residing in different layers. With respect to their intralayer counterparts, ILX feature much longer lifetimes and diffusion lengths, paving the way to excitonic optoelectronic devices operating at room temperature. While the recombination dynamics of ILX has been intensively studied, the formation process and its underlying physical mechanisms are still largely unexplored. Here we use ultrafast transient absorption spectroscopy with a white-light probe, spanning both intralayer and interlayer exciton resonances, to simultaneously capture and time-resolve interlayer charge transfer and ILX formation dynamics in a MoSe$_2$/WSe$_2$ HS. We find that the ILX formation timescale is nearly an order of magnitude (~1 ps) longer than the interlayer charge transfer time (~100 fs). Microscopic calculations attribute the relative delay to an interplay between a phonon-assisted interlayer exciton cascade and subsequent cooling processes, and excitonic wave-function overlap. Our results provide an explanation to the efficient photocurrent generation observed in optoelectronic devices based on TMD HS, as the ILX have an opportunity to dissociate during their thermalization process.

cond-mat.mtrl-sci

Dynamic screening of quasiparticles in WS$_2$ monolayers

We unravel the influence of quasiparticle screening in the non-equilibrium exciton dynamics of monolayer WS$_2$. We report pump photon energy-dependent exciton blue and red-shifts from time-resolved-reflectance contrast measurements. Based on a phenomenological model, we isolate the effective impact of excitons and free carriers on the renormalization of the quasi-free particle band gap, exciton binding energy and linewidth broadening. By this, our work does not only provide a comprehensive picture of the competing phenomena governing the exciton dynamics in WS$_2$ upon photoexcitation, but also demonstrates that exciton and carrier contributions to dynamic screening of the Coulomb interaction differ significantly.

cond-mat.mes-hall

Near-Infrared plasmon induced hot electron extraction evidence in an indium tin oxide nanoparticle / monolayer molybdenum disulphide heterostructure

In this work, we observe plasmon induced hot electron extraction in a heterojunction between indium tin oxide nanocrystals and monolayer molybdenum disulphide. We study the sample with ultrafast differential transmission exciting the sample at 1750 nm where the intense localized plasmon surface resonance of the indium tin oxide nanocrystals is and where the monolayer molybdenum disulphide does not absorb light. With the excitation at 1750 nm we observe the excitonic features of molybdenum disulphide in the visible range, close to the exciton of molybdenum disulphide. Such phenomenon can be ascribed to a charge transfer between indium tin oxide nanocrystals and monolayer molybdenum disulphide upon plasmon excitation. These results are a first step towards the implementation of near infrared plasmonic materials for photoconversion.

physics.optics

Direct view of phonon dynamics in atomically thin MoS$_{2}$

Transition metal dichalcogenide monolayers and heterostructures are highly tunable material systems that provide excellent models for physical phenomena at the two-dimensional (2D) limit. While most studies to date have focused on electrons and electron-hole pairs, phonons also play essential roles. Here, we apply ultrafast electron diffraction and diffuse scattering to directly quantify, with time and momentum resolution, electron-phonon coupling (EPC) in monolayer molybdenum disulfide (MoS$_{2}$) and phonon transport from the monolayer to a silicon nitride (Si$_3$N$_4$) substrate. Optically generated hot carriers result in a profoundly anisotropic distribution of phonons in the monolayer on the $\sim$ 5 ps time scale. A quantitative comparison with ab-initio ultrafast dynamics simulations reveals the essential role of dielectric screening in weakening EPC. Thermal transport from the monolayer to the substrate occurs with the phonon system far from equilibrium. While screening in 2D is known to strongly affect equilibrium properties, our findings extend this understanding to the dynamic regime.

cond-mat.mtrl-sci

Direct determination of momentum resolved electron transfer in the photo-excited MoS2/WS2 van der Waals heterobilayer by TR-ARPES

Photo-induced charge separation in transition metal dichalcogenide heterobilayers is being explored for moiré excitons, spin-valley polarization, and quantum phases of excitons/electrons. While different momentum spaces may be critically involved in charge separation dynamics, little is known directly from experiments. Here we determine momentum-resolved electron dynamics in the WS2/MoS2 heterobilayer using time and angle resolved photoemission spectroscopy (TR-ARPES). Upon photoexcitation in the K valleys, we detect electrons in M/2, M, and Q valleys/points on time scales as short as ~70 fs, followed by dynamic equilibration in K and Q valleys in ~400 fs. The interlayer charge transfer is accompanied by momentum-specific band renormalization. These findings reveal the essential role of phonon scattering, the coexistence of direct and indirect interlayer excitons, and constraints on spin-valley polarization.

cond-mat.mes-hall