Strong Light-matter Interaction Research Articles

Cavity Controlled Upconversion in CdSe Nanoplatelet Polaritons.

Exciton-polaritons provide a versatile platform for investigating quantum electrodynamics effects in chemical systems, such as polariton-altered chemical reactivity. However, using polaritons in chemical contexts will require a better understanding of their photophysical properties under ambient conditions, where chemistry is typically performed. Here, we used cavity quality factor to control strong light-matter interactions and in particular the excited state dynamics of colloidal CdSe nanoplatelets (NPLs) coupled to a Fabry-Pérot optical cavity. With increasing cavity quality factor, we observe significant population of the upper polariton (UP) state, exemplified by the rare observation of substantial UP photoluminescence (PL). Excitation of the lower polariton (LP) states results in upconverted PL emission from the UP branch due to efficient exchange of population between the LP, UP and the reservoir of dark states present in collectively coupled polaritonic systems. In addition, we measure time scales for polariton dynamics ∼100 ps, implying great potential for NPL based polariton systems to affect photochemical reaction rates. State-of-the-art quantum dynamical simulations show outstanding quantitative agreement with experiments, and thus provide important insight into polariton photophysical dynamics of collectively coupled nanocrystal-based systems. These findings represent a significant step toward the development of practical polariton photochemistry platforms.

Influence of Edges and Interlayer Electron-phonon Coupling in WS2/h-BN Heterostructure.

The semiconducting layered transition metal dichalcogenides (e.g., WS2) are excellent candidates for the realization of optoelectronic and nanophotonic applications on account of their band gap tunability, high binding energy and oscillator strength of the excitons, strong light-matter interaction, appreciable charge carrier mobility, and valleytronic properties. However, the photoluminescence (PL) emissions are reported to show a nonuniform spatial distribution, with the edges emitting features like defect-bound excitons and biexcitons at low temperatures in addition to the typical excitons and trions. The appearance of these additional PL features has been shown in the literature to have a strong dependence on the presence of S-vacancies and excess charge carriers. We demonstrate an enhancement of the defect-bound excitons and biexcitons by creating a heterostructure of WS2 with h-BN where the coupling between the charge carriers in WS2 with the polar phonons in h-BN governs the enhancement. Furthermore, we have performed a comprehensive resonant Raman study with varying polarization and magnetic field which not only confirms the presence of electron-phonon coupling in WS2/h-BN heterostructure, it further demonstrates a thermally induced differential resonance behavior with the excitonic level and the defect-induced midgap states (due to S-vacancies at the edge of WS2) exhibited by a dome-shaped behavior of the Raman intensities with temperature for the normal and defect-induced phonon modes. The defect-bound Raman modes exhibit maximum resonance at ∼240 K while normal Raman modes show at ∼280 K owing to a thermal variation of the electronic states.

Reversible modulation of superconductivity in thin-film NbSe2 via plasmon coupling

In recent years, lightwave has stood out as an ultrafast, non-contact control knob for developing compact superconducting circuitry. However, the modulation efficiency is limited by the low photoresponse of superconductors. Plasmons, with the advantages of strong light-matter interaction, present a promising route to overcome the limitations. Here we achieve effective modulation of superconductivity in thin-film NbSe2 via near-field coupling to plasmons in gold nanoparticles. Upon resonant plasmon excitation, the superconductivity of NbSe2 is substantially suppressed. The modulation factor exceeds 40% at a photon flux of 9.36 × 1013 s−1mm−2, and the effect is significantly diminished for thicker NbSe2 samples. Our observations can be theoretically interpreted by invoking the non-equilibrium electron distribution in NbSe2 driven by the plasmon-associated evanescent field. Finally, a reversible plasmon-driven superconducting switch is realized in this system. These findings highlight plasmonic tailoring of quantum states as an innovative strategy for superconducting electronics.

Wide-Dynamic-Range Control of Quantum-Electrodynamic Electron Transfer Reactions in the Weak Coupling Regime.

Catalyzing reactions effectively by vacuum fluctuations of electromagnetic fields is a significant challenge within the realm of chemistry. As opposed to most studies based on vibrational strong coupling, we introduce an innovative catalytic mechanism driven by weakly coupled polaritonic fields. Through the amalgamation of macroscopic quantum electrodynamics (QED) principles with Marcus electron transfer (ET) theory, we predict that ET reaction rates can be precisely modulated across a wide dynamic range by controlling the size and structure of nanocavities. Compared to QED-driven radiative ET rates in free space, plasmonic cavities induce substantial rate enhancements spanning the range from 103- to 10-fold. By contrast, Fabry-Perot cavities engender rate suppression spanning the range from 10-2- to 10-1-fold. This work overcomes the necessity of using strong light-matter interactions in QED chemistry, opening up a new era of manipulating QED-based chemical reactions in a wide dynamic range.

Femtosecond laser direct writing wedge metallic microcavities for terahertz sensing

Metallic resonators allow the manipulation of electromagnetic fields in subwavelength volumes for strong light-matter interaction, underpinning emerging flat-optics devices. Metamaterials designed with optimized effective mode volume (Veff) for stimulating and maximizing the utilization of high-density photons are highly desirable for sensing applications. Here, we demonstrate a bowtie-type terahertz (THz) metallic aperture metamaterial structure with low Veff for enhanced biosensing. The device leverages the inherent characteristic of the femtosecond laser fabrication process enabling wedge cavities down to 3 µm by tailoring the pulse energy, whose sensing performance is superior to trapezoidal ones. Such a substrate-free, microcavity metallic metamaterial sensor with extremely strong interactions achieves an experimentally normalized sensitivity of 0.654 RIU−1, and demonstrates the detection of L-proline down to 0.87 nmol. These findings provide new insights into the design and optimization of efficient THz metamaterials with tightly confined fields for ultrasensitive biomolecular detection.

Enhancing photoluminescence of WSe2 in vapor grown WSe2/VOCl bilayer heterojunctions via surface passivation.

Monolayer tungsten selenide (WSe2) has attracted attention due to its direct bandgap-generated strong light emission and light-matter interaction. Herein, vertical WSe2/VOCl bilayer heterojunctions with enhanced PL of WSe2 were synthesized by the vapor growth method. The morphology, crystal structure, and chemical composition of the WSe2/VOCl heterojunctions were systematically investigated, which confirmed the successful formation of the heterojunctions. The PL emission intensity of WSe2 obtained from the WSe2/VOCl heterojunction was about 2.4 times higher than that of the WSe2 monolayer, demonstrating the high optical quality of the WSe2/VOCl heterojunction, which was further confirmed by time-resolved PL measurements. The insulator top VOCl, which was deposited on the surface of the semiconductor bottom WSe2 as a surface passivation material, reducing the impurities and resulting in an atomically clean surface, successfully enhanced the PL emission of the bottom WSe2. This vertical WSe2/VOCl bilayer heterojunction with PL enhancement could provide a promising platform for optical devices.

Jaynes–Cummings model breaks down when the cavity geometry significantly reduces free-space emission

Strong coupling between a single resonator mode and a single quantum emitter is key to a plethora of experiments and applications in quantum science and technology and is commonly described by means of the Jaynes–Cummings model. Here, we show that the Jaynes–Cummings model only applies when the cavity does not significantly change the emitter’s decay rate into free-space. Most notably, the predictions made by the Jaynes–Cummings model become increasingly wrong when approaching the ideal emitter-resonator systems with no free-space decay channels. We present a Hamiltonian that provides, within the validity range of the rotating wave approximation, a correct theoretical description that applies to all regimes. As minimizing the coupling to free-space modes is paramount for many cavity-based applications, a correct description of strong light-matter interaction is therefore crucial for developing and optimizing quantum protocols.

Room-temperature strong coupling between CdSe nanoplatelets and a metal-DBR Fabry-Pérot cavity.

The generation of exciton-polaritons through strong light-matter interactions represents an emerging platform for exploring quantum phenomena. A significant challenge in colloidal nanocrystal-based polaritonic systems is the ability to operate at room temperature with high fidelity. Here, we demonstrate the generation of room-temperature exciton-polaritons through the coupling of CdSe nanoplatelets (NPLs) with a Fabry-Pérot optical cavity, leading to a Rabi splitting of 74.6meV. Quantum-classical calculations accurately predict the complex dynamics between the many dark state excitons and the optically allowed polariton states, including the experimentally observed lower polariton photoluminescence emission, and the concentration of photoluminescence intensities at higher in-plane momenta as the cavity becomes more negatively detuned. The Rabi splitting measured at 5K is similar to that at 300K, validating the feasibility of the temperature-independent operation of this polaritonic system. Overall, these results show that CdSe NPLs are an excellent material to facilitate the development of room-temperature quantum technologies.

Graphene-based polarization insensitive structure of ultra-wideband terahertz wave absorber

Graphene, a new smart material, has gained a lot of attention recently because of its tunable band structure and strong light-matter interaction. In comparison with typical absorbers, graphene absorbers have emerged as a highly attractive substitute for various types of applications. To broaden the absorption bandwidth, a two-dimensional graphene-based ultra-wideband and polarization-insensitive novel terahertz (THz) absorber with absorption over 95 % from 3.0 THz to 8.5 THz is proposed, with peak absorption of 99.9 % at 6.6 THz and average absorption of 98.4 % for the 5.5 THz bandwidth. The surface plasmon increased by the gold-graphene structure, the Mei resonance, and the interference cancellation between metasurfaces collectively contribute to the ultra-wideband absorption. To obtain nearly perfect broadband terahertz absorption, a single layer of graphene is used. The finite difference time domain (FDTD) approach is used for absorber analysis. In addition, the absorber is insensitive to the polarization angles and incidence angles of incident electromagnetic waves. The proposed graphene-based absorber dominates previously reported wideband THz absorbers in terms of over 95 % bandwidth, absorption peak value, and overall volume. This research will present a novel idea for the design of an ultra-wideband absorber, which can be considered a suitable candidate for different potential applications in terahertz imaging, sensors, photodetectors, and modulators.

Two-Dimensional GeS/SnSe2 Tunneling Photodiode with Bidirectional Photoresponse and High Polarization Sensitivity.

A two-dimensional (2D) broken-gap (type-III) p-n heterojunction has a unique charge transport mechanism because of nonoverlapping energy bands. In light of this, type-III band alignment can be used in tunneling field-effect transistors (TFETs) and Esaki diodes with tunable operation and low consumption by highlighting the advantages of tunneling mechanisms. In recent years, 2D tunneling photodiodes have gradually attracted attention for novel optoelectronic performance with a combination of strong light-matter interaction and tunable band alignment. However, an in-depth understanding of the tunneling mechanisms should be further investigated, especially for developing electronic and optoelectronic applications. Here, we report a type-III tunneling photodiode based on a 2D multilayered p-GeS/n+-SnSe2 heterostructure, which is first fabricated by the mechanical exfoliation and dry transfer method. Through the Simmons approximation, its various tunneling transport mechanisms dependent on bias and light are demonstrated as the origin of excellent bidirectional photoresponse performance. Moreover, compared to the traditional p-n photodiode, the device enables bidirectional photoresponse capability, including maximum responsivity values of 43 and 8.7 A/W at Vds = 1 and -1 V, respectively, with distinctive photoactive regions from the scanning photocurrent mapping. Noticeably, benefiting from the in-plane anisotropic structure of GeS, the device exhibits an enhanced photocurrent anisotropic ratio of 9, driven by the broader depletion region at Vds = -3 V under 635 nm irradiation. Above all, the results suggest that our designed architecture can be potentially applied to CMOS imaging sensors and polarization-sensitive photodetectors.

Floquet nonadiabatic mixed quantum-classical dynamics in periodically driven solid systems.

In this paper, we introduce the Floquet mean-field dynamics and Floquet surface hopping approaches to study the nonadiabatic dynamics in periodically driven solid systems. We demonstrate that these two approaches can be formulated in both real and reciprocal spaces. Using the two approaches, we are able to simulate the interaction between electronic carriers and phonons under periodic drivings, such as strong light-matter interactions. Employing the Holstein and Peierls models, we show that strong light-matter interactions can effectively modulate the dynamics of electronic population and mobility. Notably, our study demonstrates the feasibility and effectiveness of modeling low-momentum carriers' interactions with phonons using a truncated reciprocal space basis, an approach impractical in real space frameworks. Moreover, we reveal that even with a significant truncation, carrier populations derived from surface hopping maintain greater accuracy compared to those obtained via mean-field dynamics. These results underscore the potential of our proposed methods in advancing the understanding of carrier-phonon interactions in various periodically driven materials.

Waveguide-integrated van der Waals heterostructure photodetector on a lithium niobate on insulator platform.

Lithium niobate (LN) photonics has gained significant interest for their distinct material properties. However, achieving monolithically integrated photodetectors on lithium niobate on an insulator (LNOI) platform for communication wavelengths remains a challenge due to the large bandgap and extremely low electrical conductivity of LN material. A two-dimensional (2D) material photodetector is an ideal solution for LNOI photonics with a strong light-matter interaction and simple integration technique. In this work, a van der Waals heterostructure photodiode composed of a p-type black phosphorus layer and an n-type MoS2 layer is successfully demonstrated for photodetection at communication wavelengths on a LNOI platform. The LNOI waveguide-integrated BP-MoS2 photodetector exhibits a dark current as low as 0.21 nA and an on/off ratio exceeding 200 under zero voltage bias with an incident power of 13.93 µW. A responsivity as high as 1.46 A/W is achieved at -1 V bias with a reasonable dark current around 2.33 µA. With the advantages of high responsivity, low dark current, and simple fabrication process, it is promising for the monolithically integrated photodetector application for LNOI photonic platforms at communication wavelengths.

Eco-friendly and biocompatible gelatin plasmonic filters for UV-vis-NIR light

The quest for environmentally sustainable materials spans many fields and applications including optical materials. Here, we present the development of light filters using a gelatin-based nanocomposite. Owing to the plasmonic properties of metallic nanoparticles (NPs), strong light-matter interactions, these filters can be customized across the UV-Visible-NIR spectrum. The filters are designed for modular use, allowing for the addition or removal of desired spectral ranges. Moreover, the nanocomposites are composed of biodegradable and biocompatible materials which highlight the intersection of chemistry and ecological awareness for the exploration of new eco-friendly alternatives. These plasmonic gelatin-based filters block light due to the Localized Surface Plasmon Resonance (LSPR) of the NPs and can be tailored to meet various requirements, akin to a diner selecting options from a menu. This approach is inspired by culinary techniques, and we anticipate it will stimulate further exploration of biomaterials for applications in optics, materials science or electronics.

Highly tunable ground and excited state excitonic dipoles in multilayer 2H-MoSe2

The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb-bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe2 crystals exhibit electric-field-driven coupling with the ground (1s) and excited states (2s) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to 0.73 ± 0.01 enm), high energy tunability (up to ~200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from −4 to +14). Further, we observe the bi- and tri-layer excited state (2s) interlayer excitons and their coupling with the intralayer excitons states (1s and 2s). Our results, in good agreement with a coupled oscillator model with spin (layer)-selectivity and beyond standard density functional theory calculations, promote multilayer 2H-MoSe2 as a highly tunable platform to explore exciton-exciton interactions with strong light-matter interactions.

Photodetectors Based on ZrS3/MoS2 Heterostructures.

High-performance photodetectors with the detection capability of linearly polarized light have broad applications in both military and civilian fields. Quasi-one-dimensional ZrS3 as an emerging anisotropic two-dimensional material has come under the spotlight owing to its intriguing properties. However, the performance of the ZrS3 photodetector is seriously restricted by its low responsivity. Herein, a novel high-performance photodetector based on the van der Waals ZrS3/MoS2 heterostructure is proposed. Attributed to the charge trapping-assisted photogating effect, interlayer carrier transitions, and fast spatial separation of the photogenerated electron-hole pairs, the device displays superior photoresponse characteristics ranging from the ultraviolet to the visible spectrum in terms of high responsivity up to 212 A/W, an extraordinary external quantum efficiency of 8.5 × 104%, and a prompt rise/decay time of 0.19/0.38 ms. In addition, owing to the profound birefringence and dichroism effects in ZrS3 together with strong light-matter interactions in the heterostructure, profound linear-polarization sensitivity is demonstrated with a dichroic ratio of about 2.8. Overall, this photodetector not only is integrated with the excellent properties of ZrS3 and monolayer MoS2 but also further enhances the advantages through interlayer couplings, which demonstrate the strong potential of the ZrS3-based devices for high-performance, ultrafast, and polarization-sensitive photodetection.

Plasmon-assisted boosting of strong self-hybrid exciton–anapole coupling in bulk transition metal dichalcogenides nanoresonators

Intrinsic strong coupling between excitons and anapole mode in self-hybridizing transition metal dichalcogenide (TMD) nanostructures has recently attracted much attention for their capability of improving exciton–anapole interactions as a consequence of the nonradiative feature of anapole mode and the excellent mode overlap in the self-hybridizing geometry. Here, we propose a strategy for further enhancing exciton–anapole coupling. By embedding Au dimers as plasmonic components in slotted bulk WS2 nanodisks, a plasmon-induced electric field strength enhancement over nearly 140 times is achieved compared to that of the bulk WS2 nanodisk, boosting the strong exciton–anapole hybridization with greatly enhanced Rabi splitting up to 532 meV. Importantly, we demonstrate not only the effect of the plasmon mode on the initial Rabi phase of the anapole mode but also the great reduction of the ultrafast energy transfer time by the constructed full-quantum model. The plasmon-assisted hybrid system proposed in this paper provides a promising approach for enhancing strong light–matter interactions and may pave the way for the development of high-performance TMD-based photonic devices.

High-Q silicon microring resonator with ultrathin sub-wavelength thicknesses for sensitive gas sensing

Microring resonators, due to their ability to enable robust strong light–matter interactions within their structures, have garnered substantial interest for their utility in sensing applications, particularly in the realm of gas detection. However, there is an inherent trade-off between a microring resonator's quality factor and confinement factor in the air, making it difficult to balance them. Here, we demonstrate a novel solution with a suspended nanomembrane silicon (SNS) microring resonator. This resonator has ultrathin sub-wavelength thicknesses (0.02–0.03λ), which breaks the trade-off, offering not only a high intrinsic quality factor of 6 × 105 but also an extraordinarily large confinement factor of ∼80% in the air at mid-infrared wavelengths. As a proof-of-concept demonstration, we applied the SNS microring resonator for CO2 gas sensing, exhibiting a sensitivity over 10 times higher than conventional silicon resonators and a large dynamic sensing range spanning from 0% to 100% with a high resolution of better than 4% and chemical specificity. By virtue of its excellent properties, the SNS microring resonator has the potential to open new possibilities for the development of unprecedented nanophotonic integrated circuits, with a broad range of applications in on-chip sensing scenarios.

Ultralow-threshold dual-wavelength optical bistability from a perovskite hyperbolic metasurface and its application in a photonic neural network

In a hyperbolic metamaterial or metasurface (HMM or HMS), strong light-matter interaction occurs at the phase transition wavelength where the material behavior changes from metal to dielectric. As a result, the enhanced electric field can generate non-linear phenomena, such as optical bistability. In this work, we numerically investigate polarization-dependent dual-wavelength optical bistability from perovskite HMS consisting of alternating layers of MAPbBr3 perovskite and Au. Benefiting from the anisotropic property, the bistable operation wavelength for TE and TM polarizations are different. In particular, for TE polarization, strong light matter interaction resulting from the increment of incident light power not only shifts the phase transition wavelength but also enhances the transmission. Consequently, the bistable on-off contrast ratio is unprecedentedly enlarged. For TM polarization, strong light-matter interaction gives rise to an ultra-low bistable threshold. The proposed optical bistable states can serve as an activation function for optical neurons in a photonic neural network, with similar prediction accuracy across a variety of learning tasks as the classic activation functions ReLU and Sigmoid. Our work suggests a novel avenue towards the insertion of perovskite HMS into optical computing networks.

Topologically protected subradiant cavity polaritons through linewidth narrowing enabled by dissipationless edge states

Cavity polaritons derived from strong light–matter interaction provide a basis for efficient manipulation of quantum states via cavity field. Polaritons with narrow linewidth and long lifetime are appealing in applications, such as quantum sensing and storage. Here, we propose a prototypical arrangement to implement a whispering-gallery-mode resonator with one-dimensional topological atom mirror, which allows to boost the lifetime of cavity polaritons over an order of magnitude. This considerable enhancement attributes to the coupling of polaritonic states to dissipationless edge states protected by the topological bandgap of atom mirror that suppresses the leakage of cavity modes. When exceeding the width of Rabi splitting, topological bandgap can further reduce the dissipation from polaritonic states to bulk states, giving arise to subradiant cavity polaritons with extremely sharp linewidth. The resultant Rabi oscillation experiences decay rate lower than the free-space decay of a single quantum emitter. Inheriting from the topologically protected properties of edge states, the subradiance of cavity polaritons can be preserved in disordered atom mirror with moderate perturbations involving the atomic frequency, interaction strengths and location fluctuations. Our work opens up a new paradigm of topology-engineered quantum states with robust quantum coherence for future applications in quantum computing and network.

All-optical high-contrast femtosecond switching using nonlinearity from an epsilon-near-zero effect in plasmonic metamaterials.

Metamaterials opened a new realm to control light-matter interactions at sub-wavelength scale by engineering meta-atoms. Recently, the integration of several emerging nonlinear materials with metamaterial structures enables ultra-fast all-optical switching at the nanoscale and thus brings enormous possibilities to realize next-generation optical communication systems. This Letter presents a novel, to the best of our knowledge, design of plasmonic metamaterials for high-contrast femtosecond all-optical switching. We leverage magnetic plasmon (MP) resonance combined with the nonlinear effects of an epsilon-near-zero (ENZ)-material. The proposed design comprises a periodic array of two closely spaced Au-nanogratings deposited on an optically thick Au-substrate to excite MP-resonance. To enable a dynamically tunable resonance, the nanogrooves in meta-atoms are filled with an ENZ-material, cadmium-oxide (CdO). The intraband transition-induced optical nonlinearities in the ENZ-medium are studied using a two-temperature model. The MP-resonance ensures strong light-matter interactions enabling enhancement of the nonlinearities of the proposed structure. We observe that the pump-induced refractive index change in the CdO layer causes a redshift of the MP-resonance dip wavelength in the reflectance spectrum, leading to a high modulation depth of 0.83 at 1.55 µm. With an ultra-fast response time of 776 fs while maintaining a low pump-fluence of 75 µJ/cm2, the proposed metamaterial could help in realizing switches for next-generation optical computation systems.