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Relaxation Oscillations and Ultrafast Emission Pulses in a Disordered Expanding Polariton Condensate.

ABSTRACT: Semiconductor microcavities are often influenced by structural imperfections, which can disturb the flow and dynamics of exciton-polariton condensates. Additionally, in exciton-polariton condensates there is a variety of dynamical scenarios and instabilities, owing to the properties of the incoherent excitonic reservoir. We investigate the dynamics of an exciton-polariton condensate which emerges in semiconductor microcavity subject to disorder, which determines its spatial and temporal behaviour. Our experimental data revealed complex burst-like time evolution under non-resonant optical pulsed excitation. The temporal patterns of the condensate emission result from the intrinsic disorder and are driven by properties of the excitonic reservoir, which decay in time much slower with respect to the polariton condensate lifetime. This feature entails a relaxation oscillation in polariton condensate formation, resulting in ultrafast emission pulses of coherent polariton field. The experimental data can be well reproduced by numerical simulations, where the condensate is coupled to the excitonic reservoir described by a set of rate equations. Theory suggests the existence of slow reservoir temporarily emptied by stimulated scattering to the condensate, generating ultrashort pulses of the condensate emission.

SUBMITTER: Pieczarka M

PROVIDER: S-EPMC5540918 | biostudies-other | 2017 Aug

REPOSITORIES: biostudies-other

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Project description:When photoactive molecules interact strongly with confined light modes in optical cavities, new hybrid light-matter states form. They are known as polaritons and correspond to coherent superpositions of excitations of the molecules and of the cavity photon. The polariton energies and thus potential energy surfaces are changed with respect to the bare molecules, such that polariton formation is considered a promising paradigm for controlling photochemical reactions. To effectively manipulate photochemistry with confined light, the molecules need to remain in the polaritonic state long enough for the reaction on the modified potential energy surface to take place. To understand what determines this lifetime, we have performed atomistic molecular dynamics simulations of room-temperature ensembles of rhodamine chromophores strongly coupled to a single confined light mode with a 15 fs lifetime. We investigated three popular experimental scenarios and followed the relaxation after optically pumping (i) the lower polariton, (ii) the upper polariton, or (iii) uncoupled molecular states. The results of the simulations suggest that the lifetimes of the optically accessible lower and upper polaritons are limited by (i) ultrafast photoemission due to the low cavity lifetime and (ii) reversible population transfer into the "dark" state manifold. Dark states are superpositions of molecular excitations but with much smaller contributions from the cavity photon, decreasing their emission rates and hence increasing their lifetimes. We find that population transfer between polaritonic modes and dark states is determined by the overlap between the polaritonic and molecular absorption spectra. Importantly, excitation can also be transferred "upward" from the lower polariton into the dark-state reservoir due to the broad absorption spectra of the chromophores, contrary to the common conception of these processes as a "one-way" relaxation from the dark states down to the lower polariton. Our results thus suggest that polaritonic chemistry relying on modified dynamics taking place within the lower polariton manifold requires cavities with sufficiently long lifetimes and, at the same time, strong light-matter coupling strengths to prevent the back-transfer of excitation into the dark states.

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Relaxation Oscillations and Ultrafast Emission Pulses in a Disordered Expanding Polariton Condensate.

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