Strong Light-matter Interaction Research Articles

Interfacial-Water-Modulated Photoluminescence of Single-Layer WS2 on Mica.

Because of their bandgap tunability and strong light-matter interactions, two-dimensional (2D) semiconductors are considered promising candidates for next-generation optoelectronic devices. However, their photophysical properties are greatly affected by their surrounding environment because of their 2D nature. In this work, we report that the photoluminescence (PL) of single-layer WS2 is substantially affected by interfacial water that is inevitably present between it and the supporting mica substrates. Using PL spectroscopy and wide-field imaging, we show that the emission signals from A excitons and their negative trions decreased at distinctively different rates with increasing excitation power, which could be attributed to the more efficient annihilation between excitons than between trions. By gas-controlled PL imaging, we also prove that the interfacial water converted the trions into excitons by depleting native negative charges through an oxygen reduction reaction, which rendered the excited WS2 more susceptible to nonradiative decay via exciton-exciton annihilation. Understanding the role of nanoscopic water in complex low-dimensional materials will eventually contribute to devising their novel functions and related devices.

In-Plane and Out-of-Plane Investigation of Resonant Tunneling Polaritons in Metal-Dielectric-Metal Cavities.

Polaritons can be generated by tuning the optical transitions of a light emitter to the resonances of a photonic cavity. We show that a dye-doped cavity generates resonant tunneling polaritons with Epsilon-Near-Zero (ENZ) effective permittivity. We studied the polariton spectral dispersion in dye-doped metal-dielectric-metal (MDM) cavities as a function of the in-plane (k||) and out-of-plane (k⊥) components of the incident wavevector. The dependence on k|| was investigated through ellipsometry, revealing the ENZ modes. The k⊥ dependence was measured by varying the cavity thickness under normal incidence using a Surface Force Apparatus (SFA). Both methods revealed a large Rabi splitting well exceeding 100 meV. The SFA-based investigation highlighted the collective nature of strong coupling by producing a splitting proportional to the square root of the involved photons. This study demonstrates the possibility of generating ENZ polaritons and introduces the SFA as a powerful tool for the characterization of strong light-matter interactions.

Effective Modes for a Strongly Coupled Quantum Emitter-MoS$_{2}$ Nanodisk System

We present an effective modes theory for studying the strong light-matter interaction and better understanding the non-Markovian dynamics of a quantum emitter (QE) coupled to two-dimensional materials. Specifically, we investigate the spontaneous emission of a V-type QE in close proximity to a MoS <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"><tex-math notation="LaTeX">$_{2}$</tex-math></inline-formula> nanodisk. The non-Markovian population dynamics is observed and found linked to the initial states, indicating that the coupled system enters the strong-coupling regime. The effective modes analysis shows that though a dozen of resonant modes appear in the photonic density of states, only a few modes have significant contribution to the population dynamics. Our work demonstrates the effective modes theory as a powerful tool to explore and optimize the quantum states control of QE by two-dimensional materials.

Polaritonic Chern Insulators in Monolayer Semiconductors.

Systems with strong light-matter interaction open up new avenues for studying topological phases of matter. Examples include exciton polaritons, mixed light-matter quasiparticles, where the topology of the polaritonic band structure arises from the collective coupling between matter wave and optical fields strongly confined in periodic dielectric structures. Distinct from light-matter interaction in a uniform environment, the spatially varying nature of the optical fields leads to a fundamental modification of the well-known optical selection rules, which were derived under the plane wave approximation. Here we identify polaritonic Chern insulators by coupling valley excitons in transition metal dichalcogenides to photonic Bloch modes in a dielectric photonic crystal slab. We show that polaritonic Dirac points, which are markers for topological phase transition points, can be constructed from the collective coupling between valley excitons and photonic Dirac cones in the presence of both time-reversal and inversion symmetries. Lifting exciton valley degeneracy by breaking time-reversal symmetry leads to gapped polaritonic bands with nonzero Chern numbers. Through numerical simulations, we predict polaritonic chiral edge states residing inside the topological gaps. Our Letter paves the way for the further study of strong exciton-photon interaction in nanophotonic structures and for exploring polaritonic topological phases and their practical applications in polaritonic devices.

Toward Efficient Two-Photon Circularly Polarized Light Detection through Cooperative Strategies in Chiral Quasi-2D Perovskites.

Organic-inorganic hybrid perovskites carry unique semiconducting properties and advanced flexible crystal structures. These characteristics of organic-inorganic hybrid perovskites create a promising candidacy for circularly polarized light (CPL) detection. However, CPL detections based on chiral perovskites are limited to UV and visible wavelengths. The natural quantum well structures of layered hybrid perovskites generate strong light-matter interactions. This makes it possible to achieve near-infrared (NIR) CPL detection via two-photon absorption in the sub-wavelength region. In this study, cooperative strategies of dimension increase and mixed spacer cations are used to obtain a pair of chiral multilayered perovskites (R-β-MPA)EA2 Pb2 Br7 and (S-β-MPA)EA2 Pb2 Br7 (MPA = methylphenethylammonium and EA = ethylammonium). The distinctive bi-cations interlayer and multilayered inorganic skeletons provide enhanced photoconduction. Moreover, superior photoconduction leads to the prominent NIR CPL response with a responsivity up to 8.1 × 10-5 A W-1 . It is anticipated that this work can serve as a benchmark for the fabrication and optimization of efficient NIR CPL detection by simple chemical design.

Strong Coupling between Surface Plasmon Resonance and Exciton of Labeled Protein-Dye Complex for Immunosensing Applications.

In this study, we present an analysis of the optical response of strong coupling between SPR and labeled proteins. We demonstrate a sensing methodology that allows to evaluate the protein mass adsorbed to the gold's surface from the Rabi gap, which is a direct consequence of the strong light-matter interaction between surface plasmon polariton and dye exciton of labeled protein. The total internal reflection ellipsometry optical configuration was used for simulation of the optical response for adsorption of HSA-Alexa633 dye-labeled protein to a thin gold layer onto the glass prism. It was shown that Rabi oscillations had parabolic dependence on the number of labeled proteins attached to the sensor surface; however, for photonic-plasmonic systems in real experimental conditions, the range of the Rabi energy is rather narrow, thus it can be linearly approximated. This approach based on the strong coupling effect paves the alternative way for detection and monitoring of the interaction of the proteins on the transducer surface through the change of coupling strengths between plasmonic resonance and the protein-dye complex.

Many-Body Correlations and Exciton Complexes in CsPbBr3 Quantum Dots.

All-inorganic lead-halide perovskite (LHP) (CsPbX3 , X=Cl, Br, I) quantum dots (QDs) have emerged as a competitive platform for classical light-emitting devices (in the weak light-matter interaction regime, e.g., LEDs and laser), as well as for devices exploiting strong light-matter interaction at room temperature. Many-body interactions and quantum correlations among photogenerated exciton complexes play an essential role, for example, by determining the laser threshold, the overall brightness of LEDs, and the single-photon purity in quantum light sources. Here, by combining cryogenic single-QD photoluminescence spectroscopy with configuration-interaction (CI) calculations, the size-dependent trion and biexciton binding energies are addressed. Trion binding energies increase from 7to 17meV for QD sizes decreasing from 30to 9nm, while the biexciton binding energies increase from 15to 30meV, respectively. CI calculations quantitatively corroborate the experimental results and suggest that the effective dielectric constant for biexcitons slightly deviates from the one of the single excitons, potentially as a result of coupling to the lattice in the multiexciton regime. The findings here provide a deep insight into the multiexciton properties in all-inorganic LHP QDs, essential for classical and quantum optoelectronic devices.

Strong coupling between excitons and quasibound states in the continuum in bulk transition metal dichalcogenides

We investigate the strong coupling between the excitons and quasi-bound states in the continuum (BIC) resonance in a bulk WS$_2$ metasurface. Here we employ the bulk WS$_2$ to construct an ultrathin nanodisk metasurface, supporting the symmetry-protected magnetic dipole (MD) quasi-BIC resonance, which can self-hybridize with the excitons and lead to a strong light-matter interaction enhancement within the structure without the necessity for an external cavity. This strong coupling can be charactered by the considerable Rabi splitting of 159 meV and the clearly anti-crossing behavior appeared in the absorption spectrum. Furthermore, we analyze such light-matter coupling by constructing a Hamiltonian model including the surplus excitons, and tune the interaction from weak coupling to strong coupling regimes via the tunability radiation loss of the quasi-BIC resonance. Our results have great potential for manipulating the exciton-polaritons at room temperature, and provide a promising prospect for photonic devices that exploit strong coupling in applications.

Terahertz plasmonic frequency selection metasurface based on Na-GaAs complementary symmetrical split-rings for refractive index sensing

A Terahertz (THz) plasmonic frequency selection metasurface based on Na-GaAs complementary symmetrical split-ring (PFSM-NCSS) is demonstrated for bulk refractive index (RI) sensing. The sensing performances of the PFSM-NCSS is studied by finite element method (FEM). The results show that the PFSM-NCSS has reflection peaks at 9.25 and 4.4 THz for the TM and TE incident lights, respectively. The parameter optimizations indicate that the reflection peak moves towards lower frequency when P decreases or r increases, and shifts to higher frequency when w1 or w2 increases. The PFSM-NCSS with two loaded dielectrics has minimum relative frequency offset with various θ, which means it has good angular stability. The sensing structure based on the PFSM-NCSS has RI sensitivities of −969.8 and −651.1 GHz/RIU for the TM and TE incident lights, meanwhile DLs of 9.8 × 10−4 and 3.2 × 10−4RIU can be achieved. The PFSM-NCSS provides a feasible THz RI sensing scheme for the cost-effective, real-time biosensors and immunosensors, along with strong light–matter​ interaction, good electromagnetically induced transparency characteristics, and compatibility with the CMOS technology.

Substrate engineering of plasmonic nanocavity antenna modes.

Plasmonic nanocavities have emerged as a promising platform for next-generation spectroscopy, sensing and photonic quantum information processing technologies, benefiting from a unique confluence of nanoscale compactness and integrability, ultrafast functionality and room-temperature viability. Harnessing their unprecedented optical field confinement and enhancement properties for such diverse application domains, however, demands continued innovation in cavity design and robust strategies for engineering their plasmonic mode characteristics, with the aim of optimizing spatial and spectral matching conditions for strong light-matter interaction involving embedded quantum emitters. Adopting the canonical gold bowtie nanoantenna, we show that the complex refractive index, n + ik, of the substrate material provides additional design flexibility in tailoring the properties of plasmonic nanocavity modes, including their resonance wavelengths, hotspot locations, intracavity field polarization and radiative decay rates. In particular, we predict that highly refractive (n ≥ 4) or highly absorptive (k ≥ 4) substrates provide two complementary approaches to engineering nanocavity modes that are especially desirable for coupling two-dimensional quantum materials, featuring namely an elevated hotspot with a dominantly in-plane polarized near-field, as well as a strongly radiative character. Our study elucidates the benefits and intricacies of a largely unexplored facet of nanocavity mode manipulation, beyond the widely practiced synthetic control over the cavity topology or physical dimensions, and paves the way for plasmonic cavity quantum electrodynamics with two-dimensional excitonic matter.

Microstructured Optical Fiber-Enhanced Light-Matter Interaction Enables Highly Sensitive Exosome-Based Liquid Biopsy of Breast Cancer.

Exosome-based liquid biopsies highlight potential utility in diagnosis and determining the prognosis of patients with cancer and other diseases. However, the existing techniques are severely limited for practical applications due to the complications of high cost, low sensitivity, tedious procedures, and large sample consumption. Herein, we report a microstructured optical fiber sensor for fast, sensitive, and accurate quantification of exosomes in blood samples of breast cancer patients. Numerical simulations are applied to demonstrate that hollow-core microstructured antiresonant fibers (HARFs) can stringently confine light in the fiber core, ensuring strong light-matter interaction and thus maximumly amplifying the signal. Taking this advantage, a AuNPs-dsDNA assembly containing gold nanoparticles, a recognizing DNA aptamer, and a fluorescent reporter DNA sequence is fabricated followed by immobilization on the fiber wall to form a AuNPs-dsDNA-HARF sensor. Cancer-derived exosomes can be recognized and captured in the fiber channel and generate dose-dependent fluorescent signals for quantification. The microfiber sensor demonstrates enhanced sensitivity and specificity, enabling the detection of single digits of exosome particles at the nanoliter sample level. In addition, by tracking exosome phenotypic changes, the proposed fiber sensor can facilitate precise drug treatment monitoring. This work provides a robust platform for exosome-based biopsy for cancer diagnosis and prediction of therapeutic outcomes.

A roadmap to decipher ultrafast photophysics in two-dimensional nanomaterials.

Atomically thin two-dimensional (2D) semiconductors are extensively investigated for optoelectronic applications that require strong light-matter interactions. In view of such applications, it is essential to understand how (photo)excitation alters the non-linear optical response of these materials under high carrier density conditions. Broadband transient absorption (TA) spectroscopy is by now a widely used tool to study the semiconductor physics in such highly excited systems. However, the complex interplay between different many-body interactions in 2D materials produces highly congested spectral information and an ensuing non-trivial non-linear photo-response, thereby masking the desired intrinsic photophysics. Herein, we outline a concise roadmap for analyzing such congested datasets based on examples of TA analysis of various 2D materials. In particular, we emphasize the synergy between an initial qualitative understanding of the transient photo-response based on line shapes and their derivatives and a consequent quantitative spectral deconvolution backed by such insights.

Design and numerical simulation of a sensitive plasmonic-based nanosensor utilizing MoS2 monolayer and graphene

In this paper, a Kretschmann structure with a graphene-MoS2 hybrid layer has been used to design a sensitive biosensor for the detection of biomolecules. Here, by using a silicon layer, the sensitivity of the nanosensor is increased. Such a result is obtained from strong light-matter interaction between graphene and semiconductor layer. As a result, by changing the active metal and adding an additional silicon layer at a wavelength of 670 nm to access higher sensitivity and lower FWHM for the effective biosensor eventually we reach a sensitivity equal to 192°/RIU. The designed structure is investigated by numerical analysis and using the FDTD method, we numerically extract the optical characteristics of the surface plasmon polariton sensor. The detection range for the proposed structure is obtained with a refractive index of 0.005. Also, the basic parameters of the sensor to achieve the best conditions have been calculated and evaluated. In addition, the overall size of the sensor is 1112 nm × 2000 nm.

Floquet engineering in quantum materials

Floquet engineering based on the strong light-matter interaction is expected to drive quantum materials into nonequilibrium states on an ultrafast timescale, thereby engineering their electronic structure and physical properties, and achieving novel physical effects which have no counterpart in equilibrium states. In recent years, Floquet engineering has attracted a lot of research interest, and there have been numerous rich theoretical predictions. In addition, important experimental research progress has also been made in several representative materials such as topological insulators, graphene, and black phosphorus. Herein, we briefly introduce the important theoretical and experimental progress in this field, and prospect the research future, experimental challenges, and development directions.

Nonlinearity in optomechanical microresonators –phenomena, applications, and future

Optomechanical microresonators have received considerable attention in recent years because of their ability to realize strong light-matter interactions in both classical and quantum regimes and support various applications, e.g., sensing and constructing optical devices. Light-matter interactions in optomechanical microresonators enable a variety of nonlinear phenomena, which can significantly enhance the precision of sensing, the efficiency of communication, and the capabilities of quantum information processing, such as quantum state reconstruction. In this perspective, we first summarize optomechanical nonlinear phenomena in classical regimes (e.g., bistability, chaos, solitons) and quantum regimes (e.g., phonon lasing, optomechanically induced transparency). In addition, the application progress of nonlinear optomechanical effects in classical and quantum systems is reviewed, including high-sensitivity measurement, quantum state reconstruction, photon blockade, and microwave-optical conversion, etc. Finally, we provide new insights into future developments.

2D Nb&lt;sub&gt;2&lt;/sub&gt;CT&lt;sub&gt;&lt;i&gt;x&lt;/i&gt;&lt;/sub&gt; MXene/MoS&lt;sub&gt;2&lt;/sub&gt; heterostructure construction for nonlinear optical absorption modulation

Two-dimensional (2D) nonlinear optical mediums with high and tunable light modulation capability can significantly stimulate the development of ultrathin, compact, and integrated optoelectronics devices and photonic elements. 2D carbides and nitrides of transition metals (MXenes) are a new class of 2D materials with excellent intrinsic and strong light-matter interaction characteristics. However, the current understanding of their photo-physical properties and strategies for improving optical performance is insufficient. To address this issue, we rationally designed and <italic>in situ</italic> synthesized a 2D Nb₂C/MoS₂ heterostructure that outperforms pristine Nb₂C in both linear and nonlinear optical performance. Excellent agreement between experimental and theoretical results demonstrated that the Nb₂C/MoS₂ inherited the preponderance of Nb₂C and MoS₂ in absorption at different wavelengths, resulting in the broadband enhanced optical absorption characteristics. In addition to linear optical modulation, we also achieved stronger near infrared nonlinear optical modulation, with a nonlinear absorption coefficient of Nb₂C/MoS₂ being more than two times that of the pristine Nb₂C. These results were supported by the band alinement model which was determined by the X-ray photoelectron spectroscopy (XPS) experiment and first-principal theory calculation. The presented facile synthesis approach and robust light modulation strategy pave the way for broadband optoelectronic devices and optical modulators.

Strong quenching of dye fluorescence in monomeric perylene orange/TMDC hybrid structures.

Hybrid structures with an interface between two different materials with properly aligned energy levels facilitate photo-induced charge separation to be exploited in optoelectronic applications. Particularly, the combination of 2D transition metal dichalcogenides (TMDCs) and dye molecules offers strong light-matter interaction, tailorable band level alignments, and high fluorescence quantum yields. In this work, we aim at the charge or energy transfer-related quenching of the fluorescence of the dye perylene orange (PO) when isolated molecules are brought onto monolayer TMDCs via thermal vapor deposition. Here, micro-photoluminescence spectroscopy revealed a strong intensity drop of the PO fluorescence. For the TMDC emission, in contrast, we observed a relative growth of the trion versus exciton contribution. In addition, fluorescence imaging lifetime microscopy quantified the intensity quenching to a factor of about 103 and demonstrated a drastic lifetime reduction from 3 ns to values much shorter than the 100 ps width of the instrument response function. From the ratio of the intensity quenching that is attributed to hole or energy transfer from dye to semiconductor, we deduce a time constant of several picoseconds at most, pointing to an efficient charge separation suitable for optoelectronic devices.

Shining light on the microscopic resonant mechanism responsible for cavity-mediated chemical reactivity

Strong light–matter interaction in cavity environments is emerging as a promising approach to control chemical reactions in a non-intrusive and efficient manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating a chemical reaction has, however, remained unclear, hampering progress in this frontier area of research. We leverage quantum-electrodynamical density-functional theory to unveil the microscopic mechanism behind the experimentally observed reduced reaction rate under cavity induced resonant vibrational strong light-matter coupling. We observe multiple resonances and obtain the thus far theoretically elusive but experimentally critical resonant feature for a single strongly coupled molecule undergoing the reaction. While we describe only a single mode and do not explicitly account for collective coupling or intermolecular interactions, the qualitative agreement with experimental measurements suggests that our conclusions can be largely abstracted towards the experimental realization. Specifically, we find that the cavity mode acts as mediator between different vibrational modes. In effect, vibrational energy localized in single bonds that are critical for the reaction is redistributed differently which ultimately inhibits the reaction.

Room-temperature coherent optical manipulation of hole spins in solution-grown perovskite quantum dots

Manipulation of solid-state spin coherence is an important paradigm for quantum information processing. Current systems either operate at very low temperatures or are difficult to scale up. Developing low-cost, scalable materials whose spins can be coherently manipulated at room temperature is thus highly attractive for a sustainable future of quantum information science. Here we report ambient-condition all-optical initialization, manipulation and readout of hole spins in an ensemble of solution-grown CsPbBr3 perovskite quantum dots with a single hole in each dot. The hole spins are initialized by sub-picosecond electron scavenging following circularly polarized femtosecond-pulse excitation. A transverse magnetic field induces spin precession, and a second off-resonance femtosecond-pulse coherently rotates hole spins via strong light-matter interaction. These operations accomplish near-complete quantum-state control, with a coherent rotation angle close to the π radian, of hole spins at room temperature.

Two-dimensional optoelectronic devices for silicon photonic integration

With the unprecedented increasing demand for extremely fast processing speed and huge data capacity, traditional silicon-based information technology is becoming saturated due to the encountered bottlenecks of Moore's Law. New material systems and new device architectures are considered promising strategies for this challenge. Two-dimensional (2D) materials are layered materials and garnered persistent attention in recent years owing to their advantages in ultrathin body, strong light-matter interaction, flexible integration, and ultrabroad operation wavelength range. To this end, the integration of 2D materials into silicon-based platforms opens a new path for silicon photonic integration. In this work, a comprehensive review is given of the recent signs of progress related to 2D material integrated optoelectronic devices and their potential applications in silicon photonics. Firstly, the basic optical properties of 2D materials and heterostructures are summarized in the first part. Then, the state-of-the-art three typical 2D optoelectronic devices for silicon photonic applications are reviewed in detail. Finally, the perspective and challenges for the aim of 3D monolithic heterogeneous integration of these 2D optoelectronic devices are discussed.