Journal ArticleDOI
Investigating New Reactivities Enabled by Polariton Photochemistry.
Arkajit Mandal,Pengfei Huo +1 more
TLDR
Results from direct quantum dynamics simulations reveal basic principles of polariton photochemistry as well as promising reactivities that take advantage of intrinsic quantum behaviors of photons.Abstract:
We perform quantum dynamics simulations to investigate new chemical reactivities enabled by cavity quantum electrodynamics. The quantum light–matter interactions between the molecule and the quanti...read more
Citations
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Journal ArticleDOI
Cavity frequency-dependent theory for vibrational polariton chemistry.
TL;DR: In this article, a non-Markovian rate theory was proposed to describe a single molecular system coupled to a cavity mode, and the accuracy of the rate theory by performing direct numerical calculations of the transmission coefficients with the same model of the molecule-cavity hybrid system.
Journal ArticleDOI
Polariton-Mediated Electron Transfer via Cavity Quantum Electrodynamics.
TL;DR: Theoretically, both the counter-rotating terms and the dipole self-energy in the quantum electrodynamics Hamiltonian are important for obtaining an accurate polariton eigenspectrum, hence, the polariton mediated charge transfer rate constant is found, especially in the ultra-strong coupling regime.
Journal ArticleDOI
On the origin of ground-state vacuum-field catalysis: Equilibrium consideration
TL;DR: In this article, the authors examined the effect of coupling to cavity mode(s) on the potential of mean force associated with the reaction coordinate, and found that while the PMF can be affected by the cavity environment, this effect is negligible for the usual micron-length cavities used to examine VSC situations.
Journal ArticleDOI
Resolution of Gauge Ambiguities in Molecular Cavity Quantum Electrodynamics.
Michael A. D. Taylor,Michael A. D. Taylor,Arkajit Mandal,Wanghuai Zhou,Wanghuai Zhou,Pengfei Huo +5 more
TL;DR: In this article, the Coulomb gauge and dipole gauge Hamiltonians under the electronic state truncation were resolved by constructing a unitary transformation operator that constrains all light-matter interaction terms in the same subspace.
Journal Article
Polariton-assisted Singlet Fission in acene Aggregates
TL;DR: In this article, the authors investigated the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities.
References
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Journal ArticleDOI
Coherence in Spontaneous Radiation Processes
TL;DR: In this article, the authors considered a radiating gas as a single quantum-mechanical system, and the energy levels corresponding to certain correlations between individual molecules were described, where spontaneous emission of radiation in a transition between two such levels leads to the emission of coherent radiation.
Journal ArticleDOI
Comparison of quantum and semiclassical radiation theories with application to the beam maser
E.T. Jaynes,F.W. Cummings +1 more
TL;DR: In this article, it was shown that the semiclassical theory, when extended to take into account both the effect of the field on the molecules and the effects of the molecules on the field, reproduces the same laws of energy exchange and coherence properties as the quantized field theory, even in the limit of one or a few quanta in the field mode.
Proceedings Article
Optical microcavities
TL;DR: In quantum optical devices, microcavities can coax atoms or quantum dots to emit spontaneous photons in a desired direction or can provide an environment where dissipative mechanisms such as spontaneous emission are overcome so that quantum entanglement of radiation and matter is possible.
Journal ArticleDOI
Single-molecule strong coupling at room temperature in plasmonic nanocavities
Rohit Chikkaraddy,Bart de Nijs,Felix Benz,Steven J. Barrow,Oren A. Scherman,Edina Rosta,Angela Demetriadou,P. Fox,Ortwin Hess,Jeremy J. Baumberg +9 more
TL;DR: Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.
Journal ArticleDOI
Exact Solution for an N-Molecule-Radiation-Field Hamiltonian
Michael Tavis,F.W. Cummings +1 more
TL;DR: In this article, the exact solution for a problem of identical two-level molecules interacting through a dipole coupling with a single-mode quantized radiation field at resonance is given, and approximate expressions for the eigenvectors and eigenvalues for the ground and low-lying excited states, as well as the most highly excited states are developed and compared with the exact results.