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Yuejun Shen

Publications and source records attributed to Yuejun Shen.

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Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics

Quantifying and minimizing dissipation in a non-equilibrium phase transition

In a finite-time continuous phase transition, topological defects emerge as the system undergoes spontaneous symmetry breaking. The Kibble-Zurek mechanism predicts how the defect density scales with the quench rate. During such processes, dissipation also arises as the system fails to adiabatically follow the control protocol near the critical point. Quantifying and minimizing this dissipation is fundamentally relevant to nonequilibrium thermodynamics and practically important for energy-efficient computing and devices. However, there are no prior experimental measurements of dissipation, or the optimization of control protocols to reduce it in many-body systems. In addition, it is an open question to what extent dissipation is correlated with the formation of defects. Here, we directly measure the dissipation generated during the voltage-driven Freedericksz transition of a liquid crystal with a sensitivity equivalent to a ~10 nanokelvin temperature rise. We observe Kibble-Zurek scaling of dissipation and its breakdown, both in quantitative agreement with existing theoretical works. We further implement a fully automated in-situ optimization approach that discovers more optimal driving protocols, reducing dissipation by a factor of three relative to a simple linear protocol.

cond-mat.stat-mech

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics

Millimeter-scale exfoliation of hBN with tunable flake thickness

As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-film exfoliation method to prepare hBN flakes with millimeter-scale dimension, near-unity yields, and tunable flake thickness distribution from 1-7 layers, a substantial improvement over scotch tape exfoliation. The single crystallinity and high quality of the exfoliated hBN are demonstrated with optical microscopy, atomic force microscopy, Raman spectroscopy, and second harmonic generation. We further explore a possible mechanism for the effectiveness and selectivity based on thin-film residual stress measurements, density functional theory calculations, and transmission electron microscopy imaging of the deposited metal films. We find that the magnitude of the residual tensile stress induced by thin film deposition plays a key role in determining exfoliated flake thickness in a manner which closely resembles 3D semiconductor spalling. Lastly, we demonstrate that our exfoliated, large-area hBN flakes can be readily incorporated as encapsulating layers for other 2D monolayers. Altogether, this method brings us one step closer to the high throughput, mass production of hBN-based 2D photonic, optoelectronic, and quantum devices.

cond-mat.mtrl-sci

Solution-phase single-particle spectroscopy for probing multi-polaronic dynamics in quantum emitters at femtosecond resolution

The development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

cond-mat.mes-hall

Photon-assisted Landau-Zener transitions in a periodically driven Rabi dimer coupled to a dissipative mode

We investigate multiple photon-assisted Landau-Zener (LZ) transitions in a hybrid circuit quantum electrodynamics device in which each of two interacting transmission-line resonators is coupled to a qubit, and the qubits are driven by periodic driving fields and also coupled to a common phonon mode. The quantum state of the entire composite system is modeled using the multi-$\rm D_2$ Ansatz in combination with the time-dependent Dirac-Frenkel variational principle. Applying a sinusoidal driving field to one of the qubits, this device is an ideal platform to study the photon-assisted LZ transitions by comparing the dynamics of the two qubits. A series of interfering photon-assisted LZ transitions take place if the photon frequency is much smaller than the driving amplitude. Once the two energy scales are comparable, independent LZ transitions arise and a transition pathway is revealed using an energy diagram. It is found that both adiabatic and nonadiabatic transitions are involved in the dynamics. Used to model environmental effects on the LZ transitions, the common phonon mode coupled to the qubits allows for more available states to facilitate the LZ transitions. An analytical formula is obtained to estimate the short-time phonon population and produces results in reasonable agreement with numerical calculations. Equipped with the knowledge of the photon-assisted LZ transitions in the system, we can precisely manipulate the qubit state and successfully generate the qubit dynamics with a square-wave pattern by applying driving fields to both qubits, opening up new venues to manipulate the states of qubits and photons in quantum information devices and quantum computers

quant-ph