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Results for “cavity polaritons”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Magnetically Tunable Polariton Cavities in van der Waals Heterostructures

Nanophotonic cavities are the foundation for a broad spectrum of applications, including quantum sensing, on-chip communication, and cavity quantum electrodynamics. In van der Waals (vdW) materials, these cavities can harness polaritons, which are quasiparticles emerging from photon interactions with excitons, plasmons, or phonons that are confined in microscopic sample flakes. Hybrid phonon–plasmon cavities leverage the long lifetimes of phonons and good tunability of plasmons, but their reconfigurability remains fundamentally limited. Here, in this work, we introduce a magnetic-field-tuning mechanism for polaritonic cavities in a vdW heterostructure. Specifically, we demonstrate that the primary Landau transition in magnetized charge-neutral graphene can be harvested for controlling polaritonic cavity modes in a graphene-based phononic heterostructure. Additionally, we predict a magnetic-field-induced topological transition in the polariton isofrequency contour, causing a nontrivial cavity mode profile redistribution. Our study underscores the versatility of Landau-based nanophotonic cavities, offering new paradigms for the design and manipulation of light–matter interactions at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Mid-Infrared Intersubband Cavity Polaritons in Flexible Single Quantum Well

Strong and ultrastrong coupling between intersubband transitions in quantum wells and cavity photons have been realized in mid-infrared and terahertz spectral regions. However, most previous works employed a large number of quantum wells on rigid substrates to achieve coupling strengths reaching the strong or ultrastrong coupling regime. In this work, we experimentally demonstrate ultrastrong coupling between the intersubband transition in a single quantum well and the resonant mode of photonic nanocavity at room temperature. We also observe strong coupling between the nanocavity resonance and the second-order intersubband transition in a single quantum well. Furthermore, we implement for the first time such intersubband cavity polariton systems on soft and flexible substrates and demonstrate that bending of the single quantum well does not significantly affect the characteristics of the cavity polaritons. Here this work paves the way to broaden the range of potential applications of intersubband cavity polaritons including soft and wearable photonics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Deciphering between enhanced light emission and absorption in multi-mode porphyrin cavity polariton samples

Abstract It remains unclear how the collective strong coupling of cavity-confined photons to the electronic transitions of molecular chromophore leverages the distinct properties of the polaritonic constituents for future technologies. In this study, we design, fabricate, and characterize multiple types of Fabry-Pérot (FP) mirco-resonators containing copper(II) tetraphenyl porphyrin (CuTPP) to show how cavity polariton formation affects radiative relaxation processes in the presence of substantial non-Condon vibronic coupling between two of this molecule’s excited electronic states. Unlike the prototypical enhancement of Q state radiative relaxation of CuTPP in a FP resonator incapable of forming polaritons, we find the light emission processes in multimode cavity polariton samples become enhanced for cavity-exciton energy differences near those of vibrations known to mediate non-Condon vibronic coupling. We propose the value of this detuning is consistent with radiative relaxation of Herzberg-Teller polaritons into collective molecular states coupled to the cavity photon coherently. We contrast the feature stemming from light emission from the HT polariton state with those that occur due to polariton-enhanced light absorption. Our results demonstrate the landscape of molecular and photonic interactions enabled by cavity polariton formation using complex chromophores and how researchers can design resonators to leverage these interactions to characterize and control polaritonic properties.

Odewale, Elizabeth O.↗
DOE OSTI2026

Scattering theory of frequency-entangled biphoton states facilitated by cavity polaritons

The use of quantum light to probe exciton properties in semiconductor and molecular nanostructures typically occurs in the low-intensity regime. A substantial enhancement of exciton-photon coupling can be achieved with photonic cavities, where excitons hybridize with cavity modes to form polariton states. Here, to provide a theoretical framework for interpreting emerging experimental efforts in this direction, we develop a scattering theory describing the interaction of frequency-entangled photon pairs with cavity polariton and bipolariton states under various coupling regimes. Employing the Tavis-Cummings model in combination with our scattering approach, we present a quantitative analysis of how the interaction of the entangled photon pair with the polariton or bipolariton modifies its joint spectral amplitude (JSA). Specifically, we examine the effects of the cavity-mode steady-state population, exciton-cavity coupling strength, and different forms of the input photon JSA. Our results show that the entanglement entropy of the scattered photons is highly sensitive to the interplay between the input JSA and the spectral line shapes of the polariton resonances, emphasizing the cavity filtering effects. We suggest that biphoton-scattering quantum light spectroscopy best serves as a sensitive probe of polariton and bipolariton states in the photon-vacuum cavity state. Our approach is not only robust to various regimes of cavity-exciton coupling, but also amenable to extensions beyond the Tavis-Cummings model, enabling the representation of a broad class of molecular systems and solid state quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

In this study, the “particle in a box” idea, which was broadly developed in semiconductor quantum dot research, was extended into mid-infrared (IR) cavity modes by applying lateral confinement in an optical cavity. The discrete cavity modes hybridized with molecular vibrational modes, resulting in a quartet of polariton states that can support multiple coherence states in the IR regime. We applied tailored pump pulse sequences to selectively prepare these coherences and verified the multi-coherence existence. The simulation based on Lindblad equation showed that because the quartet of polariton states resided in the same cavity, they were specifically robust toward decoherence caused by fluctuations in space. The multiple robust coherences paved the way for entangled states and coherent interactions between cavity polaritons, which would be critical for advancing polariton-based quantum information technology.

2D IR↗
DOE OSTI2021

Ultrafast thermal modification of strong coupling in an organic microcavity

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical responses can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron–phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the cavity polaritons to be promising as sensitive probes of non-equilibrium phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Stabilizing Ultrathin CsPbBr 3 Nanoplatelet Films for Deterministic Strong Light-Matter Coupling

While the excitons in perovskite nanomaterials possess interesting properties central to their use in optoelectronic technologies, their instability limits real world applicability. In this study, we describe a method to stabilize the structures of cesium lead bromide (CsPbBr 3 ) nanoplatelets (NPLs) in spin-casted films. We apply this method to design, fabricate, and characterize exciton cavity polaritons formed from these nanomaterials. These studies show that we can form exciton cavity polaritons from CsPbBr 3 in precisely designed Fabry−Perot microresonators and suggest that the structures of these materials can be stabilized toward their use in other solution-processed optoelectronic devices.

cavities↗
DOE OSTI2024

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero‐Bicrystal

Abstract Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO 3 ) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO 3 ‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along “forbidden” directions are also investigated in microscale bicrystals, which arise from the finite in‐plane dimension of the synthesized MoO 3 micro‐ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub‐wavelength mid‐infrared light‐matter interactions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unzipping hBN with ultrashort mid-infrared pulses

Manipulating the nanostructure of materials is critical for numerous applications in electronics, magnetics, and photonics. However, conventional methods such as lithography and laser writing require cleanroom facilities or leave residue. We describe an approach to creating atomically sharp line defects in hexagonal boron nitride (hBN) at room temperature by direct optical phonon excitation with a mid-infrared pulsed laser from free space. We term this phenomenon “unzipping” to describe the rapid formation and growth of a crack tens of nanometers wide from a point within the laser-driven region. Formation of these features is attributed to the large atomic displacement and high local bond strain produced by strongly driving the crystal at a natural resonance. This process occurs only via coherent phonon excitation and is highly sensitive to the relative orientation of the crystal axes and the laser polarization. Its cleanliness, directionality, and sharpness enable applications such as polariton cavities, phonon-wave coupling, and in situ flake cleaving.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Quantitative modeling of gate-tunable cavity exciton-polaritons in transition-metal dichalcogenides

We performed a comprehensive real-space simulation study of propagative exciton-polaritons (EPs) of tungsten disulfide (WS 2 ) inside a Fabry–Pérot cavity. Through our simulations, we were able to construct the dispersion relation and determine the propagation length (L p ) of EPs, both of which show sensitive dependence on the applied gate voltage. We found that L p increases at higher gate voltages when excited at the exciton energy but shows opposite gate dependence at the trion energy. These observations are direct evidence of the coupling between the cavity mode with excitons and trions of WS 2 . Furthermore, we demonstrate a proof-of-concept device based on the tunable cavity EPs of WS 2 , which is promising for application as photonic transistors, modulators, or electrical-to-optical converters. Furthermore, our work unveils the real-space transport properties of gate-tunable cavity EPs and paves the way for future applications of EPs in nanophotonic devices and circuits.

42 ENGINEERING↗
DOE OSTI2023

Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics

When molecules are coupled to an optical cavity, new light–matter hybrid states, so-called polaritons, are formed due to quantum light–matter interactions. With the experimental demonstrations of modifying chemical reactivities by forming polaritons under strong light–matter interactions, theorists have been encouraged to develop new methods to simulate these systems and discover new strategies to tune and control reactions. This review summarizes some of these exciting theoretical advances in polariton chemistry, in methods ranging from the fundamental framework to computational techniques and applications spanning from photochemistry to vibrational strong coupling. Even though the theory of quantum light–matter interactions goes back to the midtwentieth century, the gaps in the knowledge of molecular quantum electrodynamics (QED) have only recently been filled. We review recent advances made in resolving gauge ambiguities, the correct form of different QED Hamiltonians under different gauges, and their connections to various quantum optics models. Then, we review recently developed ab initio QED approaches which can accurately describe polariton states in a realistic molecule–cavity hybrid system. We then discuss applications using these method advancements. We review advancements in polariton photochemistry where the cavity is made resonant to electronic transitions to control molecular nonadiabatic excited state dynamics and enable new photochemical reactivities. When the cavity resonance is tuned to the molecular vibrations instead, ground-state chemical reaction modifications have been demonstrated experimentally, though its mechanistic principle remains unclear. We present some recent theoretical progress in resolving this mystery. Finally, we review the recent advances in understanding the collective coupling regime between light and matter, where many molecules can collectively couple to a single cavity mode or many cavity modes. We also lay out the current challenges in theory to explain the observed experimental results. We hope that this review will serve as a useful document for anyone who wants to become familiar with the context of polariton chemistry and molecular cavity QED and thus significantly benefit the entire community.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Comparing Exciton-Polariton Couplings in Two-Dimensional MoS2 Cavities

Exciton-polaritons (EPs) are an emerging approach to achieve strong light-matter coupling and robust quantum phenomena, with application to areas such as photonic neuromorphic computing for instance reservoir computing. 2D transition metal dichalcogenides (TMDs) are promising candidates to host EPs due to their potential for strong coupling as evidenced by large Rabi splitting energies, which in the case of few-layer MoS2 has been demonstrated to reach 293 meV when coupled to the C exciton, placing it in the ultrastrong coupling regime, at room temperature. Here we examine how the Rabi splitting of CVD-grown monolayer MoS2 in a cavity can be optimized by tuning two variables: cavity geometry (thickness of silver and dielectric spacers) and the targeted exciton for coupling (A at about 1.9 eV, B at about 2.06 eV, or C at about 2.9 eV). With the cavity geometry, there is a tradeoff between optical field confinement and transmission. With the targeted exciton, there may be a tradeoff between Rabi splitting and lifetime. Transfer matrix simulations are used to inform how thick the cavity layers need to be, and at what angle measurements should be performed, to achieve Rabi splitting at a certain exciton energy. Experimentally, the Rabi splitting is measured by placing the cavity at a specified angle and measuring the optical reflectance and transmittance. By fitting the data, we find Rabi splittings of 124 meV, 194 meV, and 288 meV for the A, B, and C excitons, respectively, which places them in the strong, and on the edge of the ultrastrong, coupling regime.

exciton-polaritons↗
DOE OSTI2020

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities

Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. In this study, we critically assess an experimental approach using near-field imaging to probe HCP in Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212) in the presence of graphene surface plasmon polaritons (SPP). Our simulations show that inherently weak HCP features in the near-field can be strongly enhanced when coupled to graphene SPP in layered graphene/hexagonal boron nitride (hBN)/Bi-2212 heterostructures. This enhancement arises from our multilayered structures effectively acting as plasmonic cavities capable of altering collective modes of a layered superconductor by modifying its electromagnetic environment. The degree of enhancement can be selectively controlled by tuning the insulating spacer thickness with atomic precision. Finally, we verify the expected renormalization of room-temperature graphene SPP using near-field infrared imaging. Our modeling, augmented with data, attests to the validity of our approach for probing HCP modes in cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗