DOI: 10.20350/digitalcsic/16079
title: Strong light-matter coupling in lead halide perovskite quantum dot solids [Dataset]

description: Strong coupling between lead halide perovskite materials and optical resonators enables both the polaritonic control of the photophysical properties of these emerging semiconductors and the observation of novel fundamental physical phenomena. However, the difficulty to achieve optical-quality perovskite quantum dot (PQD) films showing well-defined excitonic transitions has prevented the study of strong light-matter coupling in these materials, central to the field of optoelectronics. Herein we demonstrate the formation at room temperature of multiple cavity exciton-polaritons in metallic resonators embedding highly transparent Cesium Lead Bromide quantum dot (CsPbBr3-QD) solids, revealed by a significant reconfiguration of the absorption and emission properties of the system. Our results indicate that the effects of biexciton interaction or large polaron formation, frequently invoked to explain the properties of PQDs, are seemingly absent or compensated by other more conspicuous effects in the CsPbBr3-QD optical cavity. We observe that strong coupling enables a significant reduction of the photoemission linewidth, as well as the ultrafast modulation of the optical absorption, controllable by means of the excitation fluence. We find that the interplay of the polariton states with the large dark state reservoir play a decisive role in determining the dynamics of the emission and transient absorption properties of the hybridized light-quantum dot solid system. Our results open the route for the investigation of PQD solids as polaritonic optoelectronic materials.
description: Folder List: 1. Figure_1 - Figure1_d: Absorptance; PL (counts) dispersion QDs - Figure1_e: Absorptance; PL (counts) film QDs - Figure1_f: Absorptance cavity QDs 26º, 36º, 46º - Figure1_g: Absorptance; second derivative dispersion QDs - Figure1_h: Absorptance; second derivative film QDs - Figure1_i: Absorptance; second derivative cavity QDs 2. Figure_2 -Figure2_a_experimental_map_right: experimental dispersion A vs. k|| s-polarised -Figure2_a_theoretical_map_left: theoretical dispersion A vs. k|| s-polarised -Figure2_a_experimental_maxima: experimental A maxima s-polarised -Figure2_a_JCmodel: theoretical polaritonic dispersion from JC model s-polarised -Figure2_b_experimental_map_right: experimental dispersion A vs. k|| p-polarised -Figure2_b_theoretical_map_left: theoretical dispersion A vs. k|| p-polarised -Figure2_b_experimental_maxima: experimental A maxima p-polarised -Figure2_b_JCmodel: theoretical polaritonic dispersion from JC model p-polarised -Figure2_c: Hopfield coeffcients lower polariton -Figure2_d: Hopfield coeffcients middle polariton -Figure2_e: Hopfield coeffcients upper polariton 3. Figure_3 -Figure3_a: transient absorption map of the cavity vs. wavelength -Figure3_b: delta A at 0.4 and 10ps vs. wavelength -Figure3_c: |delta A| vs. time -Figure3_d: transient absorptance (delta A + A) of the cavity vs. wavelength -Figure3_e: deconvoluted delta A -Figure3_f: deconvoluted delta A + A -Figure3_g: dinamics of I_PIA, Area_overlap MP-LP, and energy splitting vs. time 4. Figure_4 -Figure4_a: PL of QDs film vs. angle of collection -Figure4_b: Pl of QDs cavity vs. angle of collection -Figure4_c: experimental dispersion A vs. k|| -Figure4_d: PL dispersion vs. k|| -Figure4_e_data: PL decay data vs.time of colloidal dispersion, film and cavity -Figure4_e_fits: lognormal fit of PL decay data vs.time -Figure4_f: distribution of decay rates