arXiv subjects

Jiaojian Shi

Publications and source records attributed to Jiaojian Shi.

11 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

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↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2023

Giant room-temperature nonlinearities from a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and topological properties, such as Berry curvature and the quantum metric tensor, have stimulated great interest. Here, we report giant room-temperature nonlinearities in an emergent non-centrosymmetric two-dimensional topological material, the Janus transition metal dichalcogenides in the 1T' phase, which are synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently reveal orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities of 1T' MoSSe (e.g., > 50 times higher than 2H MoS$_2$ for 18th order harmonic generation; > 20 times higher than 2H MoS$_2$ for terahertz emission). It is elucidated that such colossal nonlinear optical responses come from topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and preludes the applications of topological materials in optoelectronics down to the monolayer limit. This two-dimensional form of topological materials also constitute a unique platform for examining origin of the anomalous high-harmonic generation, with potential applications as building blocks for scalable attosecond sources.

cond-mat.mes-hall↗

arXiv2022

Accelerating quantum materials development with advances in transmission electron microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, quantum dots, color center hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the materials detailed atomic scale structure, including atomic defects, dopants, and lattice stacking. In this review, after introduction of different classes of quantum materials and quantum excitations, we describe how progress in the field of electron microscopy, including in situ and in operando EM, can accelerate advances in quantum materials. Our review describes EM methods including: i) principles and operation modes of EM, ii) EM spectroscopies, such as electron energy loss spectroscopy, cathodoluminescence, and electron energy gain spectroscopy, iii) 4D scanning transmission electron microscopy, iv) dynamic and ultrafast EM, v) complimentary ultrafast spectroscopies, and vi) atomic electron tomography. We discuss how these methods inform structure function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable high resolution manipulation of quantum materials. Among numerous results, our review highlights how EM has enabled identification of the 3D structure of quantum defects, measuring reversible and metastable dynamics of quantum excitations, mapping exciton states and single photon emission, measuring nanoscale thermal transport and coupled excitation dynamics, and measuring the internal electric field of quantum heterointerfaces, all at the quantum materials intrinsic atomic and near atomic-length scale.

cond-mat.mtrl-sci↗

arXiv2022

Intrinsic 1T' phase induced in atomically thin 2H-MoTe$_2$ by a single terahertz pulse

Polymorphic transitions in layered transition metal dichalcogenides provide an excellent platform for discovering exotic phenomena associated with metastable states, ranging from topological phase transitions to enhanced superconductivity. In particular, the transition from 2H to 1T'-MoTe$_2$, which was thought to be induced by high-energy photon irradiation among many other means, has been intensely studied for its technological relevance in nanoscale transistors. Despite the remarkable electrical performance arising from this 2H-to-1T' transition, it remains controversial whether a crystalline 1T' phase is produced because optical signatures of this putative transition are found to be associated with the formation of elemental Te clusters instead. Here, we demonstrate the creation of an intrinsic 1T' lattice after irradiating a mono- or few-layer 2H-MoTe$_2$ with a single field-enhanced terahertz pulse, whose low photon energy limits possible structural damage by optical pulses. To visualize the temporal evolution of this irreversible transition, we further develop a single-shot terahertz pump-second harmonic probe technique, and we find that the transition out of the 2H phase occurs within 10 ns after photoexcitation. Our results not only resolve the long-standing debate over the light-induced polymorphic transition in MoTe$_2$, they also highlight the unique capability of strong-field terahertz pulses in manipulating the structure of quantum materials.

cond-mat.mes-hall↗

arXiv2021

Terahertz Field-Induced Reemergence of Quenched Photoluminescence in Quantum Dots

Continuous and concerted development of colloidal quantum-dot light-emitting diodes over the past two decades has established them as a bedrock technology for the next generation of displays. However, a fundamental issue that limits the performance of these devices is the quenching of photoluminescence due to excess charges from conductive charge transport layers. Although device designs have leveraged various workarounds, doing so often comes at the cost of limiting efficient charge injection. Here we demonstrate that high-field terahertz (THz) pulses can dramatically brighten quenched QDs on metallic surfaces, an effect which persists for minutes after THz irradiation. This phenomenon is attributed to the ability of the THz field to remove excess charges, thereby reducing trion and non-radiative Auger recombination. Our findings show that THz technologies can be used to suppress and control such undesired non-radiative decay, potentially in a variety of luminescent materials for future device applications.

cond-mat.mes-hall↗

arXiv2021

All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses

Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and mid-infrared (MIR) excitation. We show that moderate-field ultrafast MIR pulses (5.5 $μ$m, 150 fs) can switch the emission from a charged, low quantum yield 'grey' trion state to the 'bright' exciton state in CdSe/CdS core-shell quantum dots resulting in a significant reduction of the QD intensity flicker. Quantum-tunneling simulations suggest that the MIR fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced PL intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials.

cond-mat.mes-hall↗

arXiv2020

Nonlinear rotational spectroscopy reveals many-body interactions in water molecules

Because of their central importance in chemistry and biology, water molecules have been the subject of decades of intense spectroscopic investigations. Rotational spectroscopy of water vapor has yielded detailed information about the structure and dynamics of isolated water molecules as well as water dimers and clusters. Nonlinear rotational spectroscopy in the terahertz regime has been developed recently to investigate the rotational dynamics of linear and symmetric-top molecules whose rotational energy levels are regularly spaced, but it has not previously been applied to water or other lower-symmetry molecules with irregularly spaced levels. We report the use of recently developed two-dimensional terahertz rotational spectroscopy to observe high-order rotational coherences and correlations between rotational transitions that could not be observed previously. The results include two-quantum (2Q) peaks at frequencies that are shifted slightly from the sums of distinct rotational transitions on two molecules, which directly reveal the presence of previously unseen metastable water complexes with lifetimes of 100 ps or longer. Several such peaks observed at distinct 2Q frequencies indicate that the complexes have multiple preferred bimolecular geometries. Our results demonstrate sensitivity of rotational correlations measured in 2D THz spectroscopy to molecular interactions and complexation in the gas phase.

physics.chem-ph↗

arXiv2020

Room Temperature Terahertz Electroabsorption Modulation by Excitons in Monolayer Transition Metal Dichalcogenides

The interaction between off-resonant laser pulses and excitons in monolayer transition metal dichalcogenides is attracting increasing interest as a route for the valley-selective coherent control of the exciton properties. Here, we extend the classification of the known off-resonant phenomena by unveiling the impact of a strong THz field on the excitonic resonances of monolayer MoS$_2$. We observe that the THz pump pulse causes a selective modification of the coherence lifetime of the excitons, while keeping their oscillator strength and peak energy unchanged. We rationalize these results theoretically by invoking a hitherto unobserved manifestation of the Franz-Keldysh effect on an exciton resonance. As the modulation depth of the optical absorption reaches values as large as 0.05 dB/nm at room temperature, our findings open the way to the use of semiconducting transition metal dichalcogenides as compact and efficient platforms for high-speed electroabsorption devices.

cond-mat.mes-hall↗