Simulating anharmonic vibrational polaritons beyond the long wavelength approximation DOI
Dipti Jasrasaria, Arkajit Mandal, David R. Reichman

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(1)

Published: Jan. 2, 2025

In this work, we investigate anharmonic vibrational polaritons formed due to strong light–matter interactions in an optical cavity between radiation modes and vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of interactions, where spatially localized couple vibrations. Within theoretical framework, employ self-consistent phonon theory dynamical mean-field efficiently simulate momentum-resolved vibrational-polariton spectra, including effects anharmonicity. Numerical simulations model systems demonstrate accuracy applicability our approach.

Language: Английский

Extracting accurate light–matter couplings from disordered polaritons DOI Creative Commons

Kai Schwennicke,

Noel C. Giebink, Joel Yuen-Zhou

et al.

Nanophotonics, Journal Year: 2024, Volume and Issue: 13(14), P. 2469 - 2478

Published: April 12, 2024

The vacuum Rabi splitting (VRS) in molecular polaritons stands as a fundamental measure of collective light-matter coupling. Despite its significance, the impact disorder on VRS is not fully understood yet. This study delves into complexities amidst various distributions and degrees disorder. Our analysis provides precise analytical expressions for linear absorption, transmission, reflection spectra, along with "sum" rule, offering straightforward protocol extracting accurate coupling values from experimental data. Importantly, our cautions against directly translating large to onset ultrastrong regime. Furthermore, rectangular disorder, we witness emergence narrow side bands alongside broad central peak, indicating an extended coherence lifetime even presence substantial These findings only enhance understanding disordered systems but also open avenues achieving prolonged lifetimes between cavity molecules via interplay

Language: Английский

Citations

12
Cavity-enhanced energy transport in molecular systems DOI
Gal Sandik, Johannes Feist, F. J. Garcı́a-Vidal

et al.

Nature Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 9, 2024

Language: Английский

Citations

12
Photochemical initiation of polariton-mediated exciton propagation DOI Creative Commons
Ilia Sokolovskii, Gerrit Groenhof

Nanophotonics, Journal Year: 2024, Volume and Issue: 13(14), P. 2687 - 2694

Published: Jan. 16, 2024

Abstract Placing a material inside an optical cavity can enhance transport of excitation energy by hybridizing excitons with confined light modes into polaritons, which have dispersion that provides these light–matter quasi-particles low effective masses and very high group velocities. While in experiments, polariton propagation is typically initiated laser pulses, tuned to be resonant either the polaritonic branches are delocalized over many molecules, or uncoupled higher-energy electronic excited state localized on single molecule, practical implementations polariton-mediated exciton devices would require operation under low-intensity incoherent conditions. Here, we propose initiate photo-acid, upon absorption photon spectral range not strongly reflected mirrors, undergoes ultra-fast excited-state proton transfer red-shifted photo-product couple collectively large number suitable dye molecules cavity. By means atomistic molecular dynamics simulations demonstrate cascading from photo-excited donor coupled acceptor-cavity states via photo-chemical reaction indeed induce long-range transport.

Language: Английский

Citations

10
Thermal disorder prevents the suppression of ultra-fast photochemistry in the strong light-matter coupling regime DOI Creative Commons
Arpan Dutta, Ville Tiainen, Ilia Sokolovskii

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Aug. 4, 2024

Strong coupling between molecules and confined light modes of optical cavities to form polaritons can alter photochemistry, but the origin this effect remains largely unknown. While theoretical models suggest a suppression photochemistry due formation new polaritonic potential energy surfaces, many these do not account for energetic disorder among molecules, which is unavoidable at ambient conditions. Here, we combine simulations experiments show that an ultra-fast photochemical reaction such thermal prevents modification surface radiative decay lossy cavity modes. We also excitation spectrum under strong product bare absorption molecule-cavity system, suggesting act as gateways channeling into molecule, then reacts normally. Our results therefore imply provides means tune action rather than change reaction. The aim chemistry control reactions by placing inside cavities. authors directly possible disorder, in real experiments, mostly channel molecular excitations.

Language: Английский

Citations

9
Simulating anharmonic vibrational polaritons beyond the long wavelength approximation DOI
Dipti Jasrasaria, Arkajit Mandal, David R. Reichman

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(1)

Published: Jan. 2, 2025

In this work, we investigate anharmonic vibrational polaritons formed due to strong light–matter interactions in an optical cavity between radiation modes and vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of interactions, where spatially localized couple vibrations. Within theoretical framework, employ self-consistent phonon theory dynamical mean-field efficiently simulate momentum-resolved vibrational-polariton spectra, including effects anharmonicity. Numerical simulations model systems demonstrate accuracy applicability our approach.

Language: Английский

Citations

1