Excitonic spectral features in strongly coupled organic polaritons

Ćwik, Justyna Agnieszka; Kirton, Peter; Liberato, Simone De; Keeling, Jonathan

doi:10.1103/physreva.93.033840

Cited by 93 publications

(99 citation statements)

References 61 publications

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“…In Fig. 3 we display the photon transmission spectrum T (Q, E) ∝ |G C (Q, E)| 2 -note that the precise proportionality factor depends on the details of the microcavity [38,39]. When Ω E B , we see that we recover the usual polariton dispersions predicted by the two-level model, even for energies E > 0 where there is no bound exciton.…”

Section: Exact Results For a Single Exciton-polaritonmentioning

confidence: 68%

Microscopic description of exciton-polaritons in microcavities

Levinsen

Parish

2019

Phys. Rev. Research

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We investigate the microscopic description of exciton-polaritons that involves electrons, holes and photons within a two-dimensional microcavity. We show that in order to recover the simplified exciton-photon model that is typically used to describe polaritons, one must correctly define the exciton-photon detuning and exciton-photon (Rabi) coupling in terms of the bare microscopic parameters. For the case of unscreened Coulomb interactions, we find that the exciton-photon detuning is strongly shifted from its bare value in a manner akin to renormalization in quantum electrodynamics. Within the renormalized theory, we exactly solve the problem of a single exciton-polariton for the first time and obtain the full spectral response of the microcavity. In particular, we find that the electron-hole wave function of the polariton can be significantly modified by the very strong Rabi couplings achieved in current experiments. Our microscopic approach furthermore allows us to properly determine the effective interaction between identical polaritons, which goes beyond previous theoretical work. Our findings are thus important for understanding and characterizing exciton-polariton systems across the whole range of polariton densities. arXiv:1902.07966v1 [cond-mat.quant-gas]

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Section: Exact Results For a Single Exciton-polaritonmentioning

confidence: 68%

Microscopic description of exciton-polaritons in microcavities

Levinsen

Parish

2019

Phys. Rev. Research

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“…Other research directions consist in the study of the influence of the ultra‐strong coupling regime (as, e.g., ref. [] aimed at elucidating the enhancement mechanisms in Raman scattering). The ultra‐strong regime is defined by a Rabi frequency that becomes similar to the cavity mode frequency (

{normalΩ}_{0} \approx ω_{c}

).…”

Section: Quantum Mechanical Aspects Of Strong Couplingmentioning

confidence: 99%

Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach

et al. 2018

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When atoms come together and bond, these new states are called molecules and their properties determine many aspects of our daily life. Strangely enough, it is conceivable for light and molecules to bond, creating new hybrid light–matter states with far‐reaching consequences for these strongly coupled materials. Even stranger, there is no “real” light needed to obtain the effects; it simply appears from the vacuum, creating “something from nothing.” Surprisingly, the setup required to create these materials has become moderately straightforward. In its simplest form, one only needs to put a strongly absorbing material at the appropriate place between two mirrors, and quantum magic can appear. Only recently has it been discovered that strong coupling can affect a host of significant effects at a material and molecular level, which were thought to be independent of the “light” environment: phase transitions, conductivity, chemical reactions, etc. This review addresses the fundamentals of this opportunity: the quantum mechanical foundations, the relevant plasmonic and photonic structures, and a description of the various applications, connecting material chemistry with quantum information, entanglement, nonlinear optics, and chemical reactivity. Ultimately, revealing the interplay between light and matter in this new regime opens attractive avenues for various new technologies.

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“…Due to their relatively large dipole moments and large exciton binding energies, strong coupling can be achieved with organic molecules at room temperature down to the few-or even single-molecule level [4][5][6]. Strong coupling can lead to significant changes in the behavior of the coupled system, affecting properties such as the optical response [3][4][5][6][7][8][9][10][11][12], energy transport [13][14][15][16], chemical reactivity [17][18][19][20][21][22][23][24][25], and intersystem crossing [22,26,27]. However, up to now these setups did not provide direct information on the molecular dynamics.…”

Section: Introductionmentioning

confidence: 99%

Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses

et al. 2020

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Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a wavepacket in the molecule. A subsequent probe pulse can then dissociates or ionizes the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. In this work, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light-matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light-matter) potentials in the strong light-matter coupling regime as well as bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a new route towards ultrafast molecular spectroscopy with plasmonic nanocavities. :1907.12607v1 [cond-mat.mes-hall] arXiv

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Excitonic spectral features in strongly coupled organic polaritons

Cited by 93 publications

References 61 publications

Microscopic description of exciton-polaritons in microcavities

Microscopic description of exciton-polaritons in microcavities

Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach

Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses

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