Strong Light-matter Interaction Research Articles

Chemical applications of hybridized light-matter states (a review)

Interactions between light and matter are a fundamental part of chemical sciences responsible for basic photophysical processes such as phosphorescence and fluorescence. However, these photophysical phenomena occur in the "weak" limit of interaction between light and matter in which the photon and molecule interact with each other without the former fundamentally changing the physical properties of the latter. By constructing a Fabry-Perot cavity, which traps light of a certain frequency, then placing a molecule in a cavity that undergoes a molecular electron transition at the frequency of the trapped light, scientists can force strong light-matter interaction. This interaction occurs if the exchange between the light of the cavity mode and the molecule's excited state is faster than the decay rate of either state, forming a hybrid light-matter state known as a polariton. The photophysical properties of these polariton states have been of interest to scientists due to the possibility that they can allow for the modification of the reactivity of molecules without the addition of functional groups or modification of the surrounding environment. Of particular interest is the ability of polaritons to influence the potential energy surface of molecules, with polaritons showing the ability to both, suppress the photochemical reaction in molecules such as spiropyran and stilbene, while also enhancing the nonradiative relaxation rate of porphyrins. Due to their photonic nature, polaritons have also shown the ability to facilitate long range energy transfer processes in organic dye molecules. This review focuses on discussing these recent advances in a chemistry context as well as the optical design of cavities required to sustain polaritons.

Recent Advances in Optofluidic Laser for Biochemical Sensing

Optofluidic laser (OFL) is an emerging technology that integrates microfluidics, optical microcavity, and the liquid gain medium. Thanks to the strong light-matter interaction in the laser cavity, OFL could perform bio-chemical sensing with high performance. Here, we review the recent advances in optofluidic lasers and highlight their applications in biochemical analysis with unique properties. We introduce the physical mechanisms as well as the structure and material employed in the optofluidic laser to achieve high sensitivity, disposability, fast response and high throughput. In addition, we discuss the cross properties between these performance indicators to show how to achieve overall high performance. The effects of new materials including both gain materials and enhancer materials in laser-based sensors are briefly discussed. Furthermore, the comparison with other optical biochemical sensors and the prospects of OFLs are also given.

Molecular Chemistry in Cavity Strong Coupling.

The coherent exchange of energy between materials and optical fields leads to strong light-matter interactions and so-called polaritonic states with intriguing properties, halfway between light and matter. Two decades ago, research on these strong light-matter interactions, using optical cavity (vacuum) fields, remained for the most part the province of the physicist, with a focus on inorganic materials requiring cryogenic temperatures and carefully fabricated, high-quality optical cavities for their study. This review explores the history and recent acceleration of interest in the application of polaritonic states to molecular properties and processes. The enormous collective oscillator strength of dense films of organic molecules, aggregates, and materials allows cavity vacuum field strong coupling to be achieved at room temperature, even in rapidly fabricated, highly lossy metallic optical cavities. This has put polaritonic states and their associated coherent phenomena at the fingertips of laboratory chemists, materials scientists, and even biochemists as a potentially new tool to control molecular chemistry. The exciting phenomena that have emerged suggest that polaritonic states are of genuine relevance within the molecular and material energy landscape.

Thermo-optic coefficient of chemical vapor deposited graphene multilayers

Observation of strong inelastic light-matter interaction and large thermal conductivity of novel two-dimensional graphene has invigorated the present research. Herein, the thermo-optic coefficient of graphene multilayers is obtained from their nonlinear refraction coefficients calculated from Z-scan experiment in closed aperture geometry. The refractive optical nonlinearity was obtained employing a continuous wave He-Ne laser and occurs due to thermal lensing effect. The graphene multilayers behave as the diverging (concave) lens giving rise to self-defocusing effect leading to negative sign of refractive nonlinearity. Accordingly, a large negative thermo-optic coefficient (-2.43×10-3 K-1) inferred for the graphene multilayers suggests its utility for thermo-optic device applications.
 Keywords: Graphene, Optical Nonlinearity, Thermal lens, Self-defocusing, Thermo-optic coefficients

Investigation of CVD Growth of 2D MoS2 on MXene Structures with Photoluminescence Mapping and Fluorescence Lifetime Imaging Microscopy

Molybdenum disulfide (MoS2) and molybdenum carbide (Mo2C) are 2D materials with unique properties that make them suitable for electronic and optoelectronic applications. MoS2 is known for its high optical quantum yield and strong light–matter interaction, while Mo2C has metallic properties and is a member of the relatively new class of 2D materials called MXenes. In this research, a new heterostructure is obtained by growing MoS2 directly on Mo2C for the first time using chemical vapor deposition method. This novel hybrid structure changes the interlayer interaction and excited‐state dynamics, thereby increasing material diversity. The structure is characterized using Raman spectroscopy and atomic force microscopy, while photoluminescence (PL) and fluorescence lifetime imaging microscopy measurements are used to examine exciton motions. This study shows that the thickness of the hybrid structure is directly proportional to the frequency difference between the E2g and A1g modes, and inversely proportional to the PL intensities. The hybrid structure displays distinct exciton transitions due to the metallic effect and a longer fluorescence lifetime when compared to the bare monolayer of MoS2. The introduction of this novel hybrid structure with its optical properties holds great potential in opening up new avenues for optoelectronic device applications.

Impact of substrates and quantum effects on exciton line shapes of 2D semiconductors at room temperature

Abstract Exciton resonances in monolayer transition-metal dichalcogenides (TMDs) provide exceptionally strong light–matter interaction at room temperature. Their spectral line shape is critical in the design of a myriad of optoelectronic devices, ranging from solar cells to quantum information processing. However, disorder resulting from static inhomogeneities and dynamical fluctuations can significantly impact the line shape. Many recent works experimentally evaluate the optical properties of TMD monolayers placed on a substrate and the line shape is typically linked directly to the material’s quality. Here, we highlight that the interference of the substrate and TMD reflections can strongly influence the line shape. We further show how basic, room-temperature reflection measurements allow investigation of the quantum mechanical exciton dynamics by systematically controlling the substrate reflection with index-matching oils. By removing the substrate contribution with properly chosen oil, we can extract the excitonic decay rates including the quantum mechanical dephasing rate. The results provide valuable guidance for the engineering of exciton line shapes in layered nanophotonic systems.

Broadband plasmonic chiral meta-mirrors.

Chiral meta-mirrors provide a unique opportunity for achieving handedness-selective strong light-matter interaction at the nanometer scale. Importantly, the chiral resonances observed in chiral meta-mirrors arise from the spin-dependent resonant cavity which, however, is generally narrowband. In this paper, by exploiting a genetic algorithm (GA) based optimization method, we numerically validate a chiral meta-mirror with octave bandwidth. In particular, in the wavelength range from 1000 to 2000 nm, the proposed chiral meta-mirror strongly absorbs circularly polarized light of one handedness while highly reflecting the other. A field analysis indicates that the observed broadband chiroptical response can be attributed to the multiple chiral resonances supported by the optimized meta-mirror across the band of interest. The observed broadband chiral response confirms the potential of advanced inverse-design approaches for the creation of chiral metadevices with sophisticated functionalities. Based on the Lorentz reciprocity theorem, we show that the proposed meta-mirror can enable chiral-selective broadband second harmonic generation (SHG). Our study indicates that the application of advanced inverse-design approaches can greatly facilitate the development of metadevices with strong chiral response in both the linear and nonlinear regimes.

Van der Waals integrated plasmonic Au array for self-powered MoS2 photodetector

2D transition metal dichalcogenides such as MoS2 are promising candidates for optoelectronics because of atomically thin nature and strong light–matter interaction. However, the poor light absorption limited their photodetection performance. Surface plasma resonance (SPR) can improve light absorption, but the defects introduced during the metal deposition process limit their responsivity and response time. In this work, we transfer a plasmonic Au array onto MoS2 surface, in which van der Waals (vdWs) contact forms between defect-free Au array–MoS2 interface. The Au/MoS2 heterostructure photodetector performs 1.8 ms rising time, 186.6 A/W responsivity, and 1.41 × 1012 Jones detectivity. The damage free vdWs fabrication method also makes it possible to integrate the engineered SPR Au array with functional polymer for flexible electronics. Thus, a vdWs plasmonic Au array/MoS2/P(VDF-TrFE) photodetector with a 1.28 × 103 rectification ratio has been obtained. This approach not only optimizes the performance of the 2D optoelectronic devices but also expands the scope of its potential applications.

Self-powered photodetectors based on Er-doped MoS2 film for NIR photo-communication and laser calibration

Molybdenum disulfide (MoS2) is a promising two-dimensional material for optoelectronic applications owing to its strong light–matter interactions, high carrier mobility, and ability to combine with other materials. However, the intrinsic bandgap (1.3–1.8 eV) of MoS2 limits its applications in the near-infrared (NIR) region. Herein, a heterojunction NIR photodetector based on the Er-doped MoS2 film is developed. The photodetector presents self-powered NIR response with a fast rise/fall time of ∼9.2 μs/∼168 μs and a high detectivity of ∼3.25 × 1010 Jones at 980 nm. The high performance of the device is attributed to the improved separation of the photogenerated electron–hole pairs and the characteristic trapping capacity induced by Er dopants. Density functional theory calculations reveal that Er-doping introduces an additional energy level in the forbidden band of the MoS2:Er, and the Er-f electron orbital locates near its Fermi energy level, both of which contribute to the formation of photogenerated carriers. The MoS2:Er-based device with a 3-dB bandwidth of 5.4 kHz exhibits promising application potential in the NIR photo-communication field. Moreover, the laser calibration application of the high-performance photodetector is demonstrated. This work not only develops an effective strategy to enhance the NIR photoresponse of MoS2 films but also extends the application of MoS2-based devices.

Theory of plasmon-polaritons in binary metallic supercrystals

We present a theory of optical excitations in binary plasmonic supercrystals that are made out of two types of metal nanoparticles. Compared to monodisperse supercrystals, binary crystals have a larger number of plasmonic bands. Their dispersion is governed by the lattice symmetry, unit cell parameters, and shape and material composition of the nanoparticle building blocks. We develop a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticles, their interaction, and their coupling to photons. We show how to use group theory to analyze the plasmon- and photon-induced supercrystal states and their interaction. Plasmon-polaritons of binary metallic supercrystals are in the regime of ultrastrong and deep strong light-matter interaction; i.e., the coupling strength is on the same order as the photon energy. One consequence of the strong interaction is that quadrupolar plasmon modes and photons with energies well above the plasmon energies have to be taken into account to calculate the polariton dispersion. A cesium chloride crystal of two nanoparticles with different dipole and quadrupole energies serves as the example structure to show how the plasmon-polariton dispersion depends on the properties of the nanoparticles and supercrystal structure. The tools presented here can be used to predict and analyze any type of optically active excitation in supercrystals. The results show how to differentiate the optical properties of binary nanoparticle supercrystals into properties that inflexibly depend on lattice symmetry and properties that can be finely tuned by choosing the nanoparticle composition and shape.

Nonadiabatic dynamics near metal surface with periodic drivings: A Floquet surface hopping algorithm.

We develop a Floquet surface hopping approach to deal with nonadiabatic dynamics of molecules near metal surfaces subjected to time-periodic drivings from strong light-matter interactions. The method is based on a Floquet classical master equation (FCME) derived from a Floquet quantum master equation (FQME), followed by a Wigner transformation to treat nuclear motion classically. We then propose different trajectory surface hopping algorithms to solve the FCME. We find that a Floquet averaged surface hopping with electron density (FaSH-density) algorithm works the best as benchmarked with the FQME, capturing both the fast oscillations due to the driving and the correct steady-state observables. This method will be very useful to study strong light-matter interactions with a manifold of electronic states.

Coupled magnetic Mie resonances induced extraordinary optical transmission and its non-linear tunability

Dielectric metamaterials with low ohmic losses and resonating in the local magnetic mode are preferable for enhancing material non-linearity. Here, we propose and experimentally demonstrate broadband extraordinary electromagnetic transmission (EET) behavior, which is induced by the coupling of magnetic modes of two ceramic cuboids. It is shown that extraordinary electromagnetic transmission behavior through a perforated metal sheet with a subwavelength aperture can be achieved by exciting the first-order magnetic mode Mie resonant coupling of these cuboids. Our findings indicate that the transmission bandwidth and amplitude are dependent on the strength of coupling between the two ceramic cuboids. Additionally, we utilized non-linear effects within the dielectric cuboids to achieve tunable extraordinary electromagnetic transmission behavior. Our results are promising for developing non-linearly tunable microwave devices such as filters and modulators of their strong light-matter interactions.

Ultrafast Long-Distance Electron-Hole Plasma Expansion in GaAs Mediated by Stimulated Emission and Reabsorption of Photons.

Electron-hole plasma expansion with velocities exceeding c/50 and lasting over 10ps at 300K was evidenced by time-resolved terahertz spectroscopy. This regime, in which the carriers are driven over >30 μm is governed by stimulated emission due to low-energy electron-hole pair recombination and reabsorption of the emitted photons outside the plasma volume. At low temperatures a speed of c/10 was observed in the regime where the excitation pulse spectrally overlaps with emitted photons, leading to strong coherent light-matter interaction and optical soliton propagation effects.

Molecular Energy Transfer under the Strong Light-Matter Interaction Regime.

Research into strong light-matter interactions continues to fascinate, being spurred on by unforeseen and often spectacular experimental observations. Properties that were considered to depend exclusively on material composition have been found to be drastically altered when a material is placed inside a resonant optical cavity. This is nowhere more the case than in the field of intermolecular energy transfer, where polaritonic states formed as a result of strong light-matter interactions have been shown to promote energy transfer over distances vastly exceeding conventional limits. In this review, we provide the reader with a succinct account of the fundamental concepts of intermolecular energy transfer, and how they are modified by strong light-matter interactions. We also summarize recent experimental advances in the area, including in optoelectronic device contexts, and highlight both the potential and challenges that remain in this exciting field of research going forward.

High-performance 2D WS2 photodetector enhanced by charge-transfer doping through NH3 annealing

Transition metal dichalcogenides (TMDs) are potential candidates towards the next-generation photodetector, owing to their tunable energy bandgap and strong light–matter interaction. However, the low charge-carrier mobility and insufficient quantum efficiency of TMDs-based devices restrain their optoelectronic performances. Therefore, an effective and facile doping method needs to be developed for overcoming their poor optoelectronics properties. Here, we demonstrate a controllable nondegenerate n-doping technique for 2D TMDs materials by annealing under NH3 flow. The on/off current ratio and field-effect mobility of the device after annealing treatment increases about 2 orders of magnitude and 23 times, respectively. We attribute this remarkable doping effect to the physical adsorption and chemical adsorption of NH3 as well as the associated formation of isolated sulfur vacancies, which is dynamically activated during the annealing treatment, and further verified by the atomic-scale characterization and density functional theory calculations. The annealing temperature and time present a controllable modulation on the electron doping levels of the WS2 channel. The fabricated WS2 photodetector can operate in a broad range of visible light at room temperature. At 532 nm wavelength, the responsivity of 2.97 A/W, external quantum efficiency of 699% and specific detectivity of over 1010 Jones indicate its great potential in sensitive and power-efficient photodetectors. Our results provide an effective method to realize controllable n-doping of 2D materials, aiming for fabricating high-performance 2D photodetectors.

Sustainable chemistry with plasmonic photocatalysts

Abstract There is a pressing global need to increase the use of renewable energy sources and limit greenhouse gas emissions. Towards this goal, highly efficient and molecularly selective chemical processes that operate under mild conditions are critical. Plasmonic photocatalysis uses optically-resonant metallic nanoparticles and their resulting plasmonic, electronic, and phononic light-matter interactions to drive chemical reactions. The promise of simultaneous high-efficiency and product-selective reactions with plasmon photocatalysis provides a compelling opportunity to rethink how chemistry is achieved. Plasmonic nanoparticles serve as nanoscale ‘antennas’ that enable strong light–matter interactions, surpassing the light-harvesting capabilities one would expect purely from their size. Complex composite structures, combining engineered light harvesters with more chemically active components, are a focal point of current research endeavors. In this review, we provide an overview of recent advances in plasmonic catalysis. We start with a discussion of the relevant mechanisms in photochemical transformations and explain hot-carrier generation and distributions from several ubiquitous plasmonic antennae. Then we highlight three important types of catalytic processes for sustainable chemistry: ammonia synthesis, hydrogen production and CO2 reduction. To help elucidate the reaction mechanism, both state-of-art electromagnetic calculations and quantum mechanistic calculations are discussed. This review provides insights to better understand the mechanism of plasmonic photocatalysis with a variety of metallic and composite nanostructures toward designing and controlling improved platforms for green chemistry in the future.

Near‐Field Nano‐Optical Imaging of van der Waals Materials

Abstract2D van der Waals (vdW) materials are emerging as the next generation platform for optical and electronic devices with their wide coverage of the energy bandgaps. The strong light–matter interactions in 2D vdW layers allow for exploring novel optical and electronic phenomena such as 2D polaritons exhibiting ultrahigh field confinement, defects‐induced new quantum states, and strain‐modulated quantum confinement of 2D excitons. Far‐field optical imaging techniques are extensively used to characterize the 2D vdW materials so far, however, subdiffraction spatial resolution is required for comprehensive investigations of 2D vdW materials of which physical properties are greatly influenced by local defects and strain. This article aims to cover historical advances, fundamental principles, and distinct features of emerging near‐field optical imaging techniques: scattering‐type scanning near‐field optical microscopy, tip‐enhanced Raman spectroscopy, tip‐enhanced photoluminescence techniques, and photo‐induced force microscopy. The recent developments toward spectroscopic analysis of near‐field imaging and applications for unveiling unique properties of 2D polaritons, nanoscale defects, and mechanical strains in 2D vdW materials, are also discussed. This review article provides an understanding of emerging near‐field imaging techniques and suggests prospective applications for exploring 2D vdW materials.

An Optoelectronic Synapse Based on Two-Dimensional Violet Phosphorus Heterostructure.

Neuromorphic computing can efficiently handle data-intensive tasks and address the redundant interaction required by von Neumann architectures. Synaptic devices are essential components for neuromorphic computation. 2D phosphorene, such as violet phosphorene, show great potential in optoelectronics due to their strong light-matter interactions, while current research is mainly focused on synthesis and characterization, its application in photoelectric devices is vacant. Here, the authors combined violet phosphorene and molybdenum disulfide to demonstrate an optoelectronic synapse with a light-to-dark ratio of 106 , benefiting from a significant threshold shift due to charge transfer and trapping in the heterostructure. Remarkable synaptic properties are demonstrated, including a dynamic range (DR) of > 60dB, 128 (7-bit) distinguishable conductance states, electro-optical dependent plasticity, short-term paired-pulse facilitation, and long-term potentiation/depression. Thanks to the excellent DR and multi-states, high-precision image classification with accuracies of 95.23% and 79.65% is achieved for the MNIST and complex Fashion-MNIST datasets, which is close to the ideal device (95.47%, 79.95%). This work opens the way for the use of emerging phosphorene in optoelectronics and provides a new strategy for building synaptic devices for high-precision neuromorphic computing.

Multifunctional interface between integrated photonics and free space

The combination of photonic integrated circuits and free-space metaoptics has the ability to untie technological knots that require advanced light manipulation due to their conjoined ability to achieve strong light–matter interaction via wave-guiding light over a long distance and shape them via large space-bandwidth product. Rapid prototyping of such a compound system requires component interchangeability. This represents a functional challenge in terms of fabrication and alignment of high-performance optical systems. Here, we report a flexible and interchangeable interface between a photonic integrated circuit and the free space using an array of low-loss metaoptics and demonstrate multifunctional beam shaping at a wavelength of 780 nm. We show that robust and high-fidelity operation of the designed optical functions can be achieved without prior precise characterization of the free-space input nor stringent alignment between the photonic integrated chip and the metaoptics chip. A diffraction limited spot of ∼3 μm for a hyperboloid metalens of numerical aperture 0.15 is achieved despite an input Gaussian elliptical deformation of up to 35% and misalignments of the components of up to 20 μm. A holographic image with a peak signal-to-noise ratio of >10 dB is also reported.

Strongly enhanced light-matter coupling of monolayer WS2 from a bound state in the continuum.

Exciton-polaritons derived from the strong light-matter interaction of an optical bound state in the continuum with an excitonic resonance can inherit an ultralong radiative lifetime and significant nonlinearities, but their realization in two-dimensional semiconductors remains challenging at room temperature. Here we show strong light-matter interaction enhancement and large exciton-polariton nonlinearities at room temperature by coupling monolayer tungsten disulfide excitons to a topologically protected bound state in the continuum moulded by a one-dimensional photonic crystal, and optimizing for the electric-field strength at the monolayer position through Bloch surface wave confinement. By a structured optimization approach, the coupling with the active material is maximized here in a fully open architecture, allowing to achieve a 100 meV photonic bandgap with the bound state in the continuum in a local energy minimum and a Rabi splitting of 70 meV, which results in very high cooperativity. Our architecture paves the way to a class of polariton devices based on topologically protected and highly interacting bound states in the continuum.