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Ultrafast polariton population build-up mediated by molecular phonons in organic microcavities
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Image of FIG. 1.

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FIG. 1.

(Color online) (a) A schematic of the organic microcavity structure containing J-aggregates dispersed in matrix. (b) Upper and lower polariton branches and uncoupled exciton reservoir states. Population of lower polariton states occurs through resonant coupling of exciton reservoir via molecular phonons in accordance with the J-aggregate Raman spectrum.

Image of FIG. 2.

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FIG. 2.

(Color online) Normalized contour plots of the angular PL intensity for two different detunings. Upper panel: experimental lower polariton branch PL images. Lower panel: modelled steady state polariton emission. Dashed lines indicate the bare cavity mode dispersions and exciton reservoir energy.

Image of FIG. 3.

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FIG. 3.

(Color online) (a) Temporal changes in probe transmission reflecting real polariton population at vibronic resonance of 1.968 eV; measured (circles) and modelled (solid line). (b) Experimental (solid lines) and modelled (dashed lines) angle integrated PL intensity for different exciton-cavity mode detunings showing peaked emission when resonance condition is met. (c) Measured and modelled ER to LP rise time values at different energies. J-aggregate Raman spectra are superimposed for comparison confirming fast build-up time at resonances.

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/content/aip/journal/apl/99/14/10.1063/1.3645633
2011-10-03
2014-04-21

Abstract

A key prerequisite for low-threshold polariton lasing in organic or inorganic microcavity systems is the efficient population of the lower polariton ground state. Here, we report the observation of a resonant phonon-mediated relaxation process which gives rise to nonthermal polariton population with sub 100 fs build-up times. This mechanism is manifested by discrete maxima of the angular-resolved photoluminescence intensity, with corresponding shortening of the photoluminescence rise time at respective phononresonances. The realization of enhanced relaxation rates in disordered J-aggregate systems is important for developing room temperature organic laser sources with less fabrication complexity than their crystalline counterparts.

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Scitation: Ultrafast polariton population build-up mediated by molecular phonons in organic microcavities
http://aip.metastore.ingenta.com/content/aip/journal/apl/99/14/10.1063/1.3645633
10.1063/1.3645633
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