Strong coupling in a microcavity containing β-carotene

Grant, Richard T.; Jayaprakash, Rahul; Coles, David M.; Musser, Andrew J.; Liberato, Simone De; Samuel, Ifor D. W.; Turnbull, Graham A.; Clark, Jenny; Lidzey, David G.

doi:10.1364/oe.26.003320

Cited by 11 publications

(10 citation statements)

References 30 publications

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“…The angle-dependent reflectivity of DBRs and microcavities was characterized on a broadband fibercoupled goniometer. The resulting reflectivity dispersions were simulated with transfer matrix methods, 65 using as inputs the normal-incidence transmission spectra of a 156-nm BODIPY-R/PS thin film (Figure 1a) and a 7-pair DBR. Following benchmarking using the steady-state reflectivity, a transfer matrix model was used to simulate pump-induced changes to the microcavity optical properties.…”

Section: Methodsmentioning

confidence: 99%

Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale

Renken

Pandya

Georgiou

et al. 2021

The Journal of Chemical Physics

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Strong light-matter coupling to form exciton-and vibropolaritons is increasingly touted as a powerful tool to alter the fundamental properties of organic materials. It is proposed that these states and their facile tunability can be used to rewrite molecular potential energy landscapes and redirect photophysical pathways, with applications from catalysis to electronic devices. Crucial to their photophysical properties is the exchange of energy between coherent, bright polaritons and incoherent dark states. One of the most potent tools to explore this interplay is transient absorption/reflectance spectroscopy. Previous studies have revealed unexpectedly long lifetimes of the coherent polariton states, for which there is no theoretical explanation. Applying these transient methods to a series of strong-coupled organic microcavities, we recover similar long-lived spectral effects. Based on transfer-matrix modelling of the transient experiment, we find that virtually the entire photoresponse results from photoexcitation effects other than the generation of polariton states. Our results suggest that the complex optical properties of polaritonic systems make them especially prone to misleading optical signatures, and that more challenging high-time-resolution measurements on high-quality microcavities are necessary to uniquely distinguish the coherent polariton dynamics.

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Section: Methodsmentioning

confidence: 99%

Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale

Renken

Pandya

Georgiou

et al. 2021

The Journal of Chemical Physics

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“…There are several widely-used technologies that ultimately base their efficiency on the rates of chemical reactions or electron transfer processes that occur in excited electronic states (e.g., sunscreens, polymers, catalysis, solar cells, OLEDs). Therefore, the ability to manipulate the rates and branching ratios of these fundamental chemical processes in a reversible manner using light-matter interaction with a vacuum field, suggests a promising route for targeted control of excited state reactivity, without exposing fragile molecular species or materials to ESC Cavity-enhanced energy transfer and conductivity in organic media [30,[137][138][139] ESC/VSC Strong coupling with biological light-harvesting systems [44,[140][141][142] ESC Cavity-modified photoisomerization and intersystem crossing [28,104,[143][144][145] ESC Strong coupling with an individual molecule in a plasmonic nanocavity [95,96,98,146] ESC Polariton-enhanced organic light emitting devices [32,35,147,148] EUSC Ultrastrong light-matter interaction with molecular ensembles [29,36,92,147,[149][150][151] VSC/VUSC Vibrational polaritons in solid phase and liquid phase Fabry-Perot cavities [38-40, 45-47, 49-54, 152] VSC Manipulation of chemical reactivity in the ground electronic state [43,55,153] ESC Cavity-controlled intramolecular electron transfer in molecular ensembles. [134,[154][155]…”

Section: A Recent Experimental Progressmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

257

248

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This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control and quantum technology.

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“… − The open Fabry–Pérot IR microcavity used in this work consists of two Au mirrors, prepared on circular CaF 2 windows ( d = 25.0 mm, 5.0 mm thickness) by a high vacuum sputtering (Leica EM MED 020). The thickness of the Au film was controlled using a quartz crystal balance as a reference during sputtering.…”

Section: Methodsmentioning

confidence: 99%

Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

et al. 2020

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The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this study, we design a voltagetunable open microcavity and we show the formation of multiple vibrational polaritons in methyl salicylate. A Rabi splitting and polariton anticrossing behavior is observed when the cavity mode hybridizes with the CO stretching vibration of methyl salicylate. Furthermore, the proposed theoretical model based on coupled harmonic oscillators reveals that the absorption of uncoupled molecules must also be considered to model the experimental spectra properly and that simultaneous coupling of multiple molecular vibrations to the same cavity mode has a significant influence on the transmission spectral profile.

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Strong coupling in a microcavity containing β-carotene

Cited by 11 publications

References 30 publications

Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale

Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale

Molecular polaritons for controlling chemistry with quantum optics

Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

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