Browse
Submit Data
Databases
API
Help

Dataset Information

33 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Cavity-Free Ultrastrong Light-Matter Coupling.

ABSTRACT: Strong coupling between light and matter can occur when the interaction strength between a confined electromagnetic field and a molecular resonance exceeds the losses to the environment, leading to the formation of hybrid light-matter states known as polaritons. Ultrastrong coupling occurs when the coupling strength becomes comparable to the transition energy of the system. It is widely assumed that the confined electromagnetic fields necessary for strong coupling to organic molecules can only be achieved with external structures such as Fabry-Pérot resonators, plasmonic nanostructures, or dielectric resonators. Here we show experimentally that such structures are unnecessary and that a simple dielectric film of dye molecules supports sufficiently modified vacuum electromagnetic fields to enable room-temperature ultrastrong light-matter coupling. Our results may be of use in the design of experiments to probe polaritonic chemistry and suggest that polaritonic states are perhaps easier to realize than previously thought.

SUBMITTER: Thomas PA

PROVIDER: S-EPMC8327311 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Ultrastrong coupling between nanoparticle plasmons and cavity photons at ambient conditions.

Project description:Ultrastrong coupling is a distinct regime of electromagnetic interaction that enables a rich variety of intriguing physical phenomena. Traditionally, this regime has been reached by coupling intersubband transitions of multiple quantum wells, superconducting artificial atoms, or two-dimensional electron gases to microcavity resonators. However, employing these platforms requires demanding experimental conditions such as cryogenic temperatures, strong magnetic fields, and high vacuum. Here, we use a plasmonic nanorod array positioned at the antinode of a resonant optical Fabry-Pérot microcavity to reach the ultrastrong coupling (USC) regime at ambient conditions and without the use of magnetic fields. From optical measurements we extract the value of the interaction strength over the transition energy as high as g/??~?0.55, deep in the USC regime, while the nanorod array occupies only ?4% of the cavity volume. Moreover, by comparing the resonant energies of the coupled and uncoupled systems, we indirectly observe up to ?10% modification of the ground-state energy, which is a hallmark of USC. Our results suggest that plasmon-microcavity polaritons are a promising platform for room-temperature USC realizations in the optical and infrared ranges, and may lead to the long-sought direct visualization of the vacuum energy modification.

| S-EPMC7264206 | biostudies-literature

Cavity molecular dynamics simulations of liquid water under vibrational ultrastrong coupling.

Project description:We simulate vibrational strong coupling (VSC) and vibrational ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O-H stretch mode of liquid water, the infrared spectrum shows asymmetric Rabi splitting. The lower polariton (LP) may be suppressed or enhanced relative to the upper polariton (UP) depending on the frequency of the cavity mode. Moreover, although the static properties and the translational diffusion of water are not changed under VSC or V-USC, we do find the modification of the orientational autocorrelation function of H2O molecules especially under V-USC, which could play a role in ground-state chemistry.

| S-EPMC7414078 | biostudies-literature

Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity.

Project description:Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.

| S-EPMC9151642 | biostudies-literature

Strong coupling of hybrid states of light and matter in cavity-coupled quantum dot solids.

Project description:The formation of plasmon-exciton (plexciton) polariton is a direct consequence of strong light-matter interaction, and it happens in a semiconductor-metal hybrid system. Here the formation of plasmon-exciton polaritons was observed from an AgTe/CdTe Quantum Dot (QD) solid system in the strong coupling regime. The strong coupling was achieved by increasing the oscillator strength of the excitons by forming coupled QD solids. The anti-crossing-like behaviour indicates the strong coupling between plasmonic and excitons state in AgTe/CdTe QD solids, resulting in a maximum Rabi splitting value of 225 meV at room temperature. The formation of this hybrid state of matter and its dynamics were studied through absorption, photoluminescence, and femtosecond transient studies.

| S-EPMC10551025 | biostudies-literature

Polariton Transitions in Femtosecond Transient Absorption Studies of Ultrastrong Light-Molecule Coupling.

Project description:Strong light-matter coupling is emerging as a fascinating way to tune optical properties and modify the photophysics of molecular systems. In this work, we studied a molecular chromophore under strong coupling with the optical mode of a Fabry-Perot cavity resonant to the first electronic absorption band. Using femtosecond pump-probe spectroscopy, we investigated the transient response of the cavity-coupled molecules upon photoexcitation resonant to the upper and lower polaritons. We identified an excited state absorption from upper and lower polaritons to a state at the energy of the second cavity mode. Quantum mechanical calculations of the many-molecule energy structure of cavity polaritons suggest assignment of this state as a two-particle polaritonic state with optically allowed transitions from the upper and lower polaritons. We provide new physical insight into the role of two-particle polaritonic states in explaining transient signatures in hybrid light-matter coupling systems consistent with analogous many-body systems.

| S-EPMC8154840 | biostudies-literature

Frequency conversion in ultrastrong cavity QED.

Project description:We propose a new method for frequency conversion of photons which is both versatile and deterministic. We show that a system with two resonators ultrastrongly coupled to a single qubit can be used to realise both single- and multiphoton frequency-conversion processes. The conversion can be exquisitely controlled by tuning the qubit frequency to bring the desired frequency-conversion transitions on or off resonance. Considering recent experimental advances in ultrastrong coupling for circuit QED and other systems, we believe that our scheme can be implemented using available technology.

| S-EPMC5509682 | biostudies-other

Barrier-free reverse-intersystem crossing in organic molecules by strong light-matter coupling.

Project description:Strong light-matter coupling provides the means to challenge the traditional rules of chemistry. In particular, an energy inversion of singlet and triplet excited states would be fundamentally remarkable since it would violate the classical Hund's rule. An organic chromophore possessing a lower singlet excited state can effectively harvest the dark triplet states, thus enabling 100% internal quantum efficiency in electrically pumped light-emitting diodes and lasers. Here we demonstrate unambiguously an inversion of singlet and triplet excited states of a prototype molecule by strong coupling to an optical cavity. The inversion not only implies that the polaritonic state lies at a lower energy, but also a direct energy pathway between the triplet and polaritonic states is opened. The intrinsic photophysics of reversed-intersystem crossing are thereby completely overturned from an endothermic process to an exothermic one. By doing so, we show that it is possible to break the limit of Hund's rule and manipulate the energy flow in molecular systems by strong light-matter coupling. Our results will directly promote the development of organic light-emitting diodes based on reversed-intersystem crossing. Moreover, we anticipate that it provides the pathway to the creation of electrically pumped polaritonic lasers in organic systems.

| S-EPMC8167092 | biostudies-literature

Mode-multiplexing deep-strong light-matter coupling.

Project description:Dressing electronic quantum states with virtual photons creates exotic effects ranging from vacuum-field modified transport to polaritonic chemistry, and squeezing or entanglement of modes. The established paradigm of cavity quantum electrodynamics maximizes the light-matter coupling strength ΩR/ωc , defined as the ratio of the vacuum Rabi frequency and the frequency of light, by resonant interactions. Yet, the finite oscillator strength of a single electronic excitation sets a natural limit to ΩR/ωc . Here, we enter a regime of record-strong light-matter interaction which exploits the cooperative dipole moments of multiple, highly non-resonant magnetoplasmon modes tailored by our metasurface. This creates an ultrabroadband spectrum of 20 polaritons spanning 6 optical octaves, calculated vacuum ground state populations exceeding 1 virtual excitation quantum, and coupling strengths equivalent to ΩR/ωc=3.19 . The extreme interaction drives strongly subcycle energy exchange between multiple bosonic vacuum modes akin to high-order nonlinearities, and entangles previously orthogonal electronic excitations solely via vacuum fluctuations.

| S-EPMC10901777 | biostudies-literature

Quantum topology in the ultrastrong coupling regime.

Project description:The coupling between two or more objects can generally be categorized as strong or weak. In cavity quantum electrodynamics for example, when the coupling strength is larger than the loss rate the coupling is termed strong, and otherwise it is dubbed weak. Ultrastrong coupling, where the interaction energy is of the same order of magnitude as the bare energies of the uncoupled objects, presents a new paradigm for quantum physics and beyond. As a consequence profound changes to well established phenomena occur, for instance the ground state in an ultrastrongly coupled system is not empty but hosts virtual excitations due to the existence of processes which do not conserve the total number of excitations. The implications of ultrastrong coupling for quantum topological systems, where the number of excitations are typically conserved, remain largely unknown despite the great utility of topological matter. Here we reveal how the delicate interplay between ultrastrong coupling and topological states manifests in a one-dimensional array. We study theoretically a dimerized chain of two-level systems within the ultrastrong coupling regime, where the combined saturation and counter-rotating terms in the Hamiltonian are shown to play pivotal roles in the rich, multi-excitation effective bandstructure. In particular, we uncover unusual topological edge states, we introduce a flavour of topological state which we call an anti-edge state, and we reveal the remarkable geometric-dependent renormalizations of the quantum vaccum. Taken together, our results provide a route map for experimentalists to characterize and explore a prototypical system in the emerging field of ultrastrong quantum topology.

| S-EPMC9270417 | biostudies-literature

Cavity-free plasmonic nanolasing enabled by dispersionless stopped light.

Project description:When light is brought to a standstill, its interaction with gain media increases dramatically due to a singularity in the density of optical states. Concurrently, stopped light engenders an inherent and cavity-free feedback mechanism, similar in effect to the feedback that has been demonstrated and exploited in large-scale disordered media and random lasers. Here we study the spatial, temporal and spectral signatures of lasing in planar gain-enhanced nanoplasmonic structures at near-infrared frequencies and show that the stopped-light feedback mechanism allows for nanolasing without a cavity. We reveal that in the absence of cavity-induced feedback, the subwavelength lasing mode forms dynamically as a phase-locked superposition of quasi dispersion-free waveguide modes. This mechanism proves remarkably robust against interface roughness and offers a new route towards nanolasing, the experimental realization of ultra-thin surface emitting lasers, and cavity-free active quantum plasmonics.

| S-EPMC4199200 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data