skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Dissociation slowdown by collective optical response under strong coupling conditions
We consider an ensemble of diatomic molecules resonantly coupled to an optical cavity under strong coupling conditions at normal incidence. Photodissociation dynamics is examined via direct numerical integration of the coupled Maxwell–Schrödinger equations with molecular rovibrational degrees of freedom explicitly taken into account. It is shown that the dissociation is significantly affected (slowed down) when the system is driven at its polaritonic frequencies. The observed effect is demonstrated to be of transient nature and has no classical analog. An intuitive explanation of the dissociation slowdown at polaritonic frequencies is proposed.  more » « less
Award ID(s):
1953701
PAR ID:
10398376
Author(s) / Creator(s):
; ;
Publisher / Repository:
American Institute of Physics
Date Published:
Journal Name:
The Journal of Chemical Physics
Volume:
158
Issue:
8
ISSN:
0021-9606
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Ultralow-threshold coherent light emitters can be achieved through lasing from exciton-polariton condensates, but this generally requires sophisticated device structures and cryogenic temperatures. Polaritonic nanolasers operating at room temperature lie on the crucial path of related research, not only for the exploration of polariton physics at the nanoscale but also for potential applications in quantum information systems, all-optical logic gates, and ultralow-threshold lasers. However, at present, progress toward room temperature polariton nanolasers has been limited by the thermal instability of excitons and the inherently low quality factors of nanocavities. Here, we demonstrate room temperature polaritonic nanolasers by designing wide-gap semiconductor heterostructure nanocavities to produce thermally stable excitons coupled with nanocavity photons. The resulting mixed states of exciton polaritons with Rabi frequencies of approximately 370 meV enable persistent polariton lasing up to room temperature, facilitating the realization of miniaturized and integrated polariton systems. 
    more » « less
  2. Abstract Cavity-modified chemistry uses strong light-matter interactions to modify the electronic properties of molecules in order to enable new physical phenomena such as novel reaction pathways. As cavity chemistry often involves critical regions where configurations become nearly degenerate, the ability to treat multireference problems is crucial to understanding polaritonic systems. In this Letter, we show through the use of a unitary ansatz derived from the anti-Hermitian contracted Schrödinger equation that cavity-modified systems with strong correlation, such as the deformation of rectangular H4coupled to a cavity mode, can be solved efficiently and accurately on a quantum device. In contrast, while our quantum algorithm can be made formally exact, classical-computing methods as well as other quantum-computing algorithms often yield answers that are both quantitatively and qualitatively incorrect. Additionally, we demonstrate the current feasibility of the algorithm on near intermediate-scale quantum hardware by computing the dissociation curve of H2strongly coupled to a bosonic bath. 
    more » « less
  3. Abstract Integrated photonics has been a promising platform for analog quantum simulation of condensed matter phenomena in strongly correlated systems. To that end, we explore the implementation of all-photonic quantum simulators in coupled cavity arrays with integrated ensembles of spectrally disordered emitters. Our model is reflective of color center ensembles integrated into photonic crystal cavity arrays. Using the Quantum Master equation and the Effective Hamiltonian approaches, we study energy band formation and wavefunction properties in the open quantum Tavis–Cummings–Hubbard framework. We find conditions for polariton creation and (de)localization under experimentally relevant values of disorder in emitter frequencies, cavity resonance frequencies, and emitter-cavity coupling rates. To quantify these properties, we introduce two metrics, the polaritonic and nodal participation ratios, that characterize the light-matter hybridization and the node delocalization of the wavefunction, respectively. These new metrics combined with the Effective Hamiltonian approach prove to be a powerful toolbox for cavity quantum electrodynamical engineering of solid-state systems. 
    more » « less
  4. Abstract The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics. 
    more » « less
  5. Vibrational and electronic strong coupling of light with molecular excitations has shown promise for modifying chemical reaction rates. However, the Tavis–Cummings model often used to model such polaritonic chemistry considers only a single discrete cavity mode coupled with the molecular modes, while experimental systems generally consist of a larger number of molecules in cavities with a continuum of modes. Here, we model the polaritonic effects of multimode cavities of arbitrary dimensions and filled with a large number of molecules. We obtain the dependence of the effects on the dimensionality of the cavity, the molecular oscillator strength, and molecular concentration. Combining our model with the transition state theory, we show that polaritonic effects can be altered by a few orders of magnitude compared to including only a single cavity mode, and that the effect is stronger with a larger molecular dipole moment and molecular concentration. However, the change remains negligibly small for realistic chemical systems due to the large number of dark states. 
    more » « less