Ultrafast Dynamics of Nonequilibrium Organic Exciton-Polariton Condensates.

Exciton-polariton condensation in organic materials, arising from the coupling of Frenkel excitons to the electromagnetic field in cavities, is a phenomenon resulting in low-threshold coherent light emission among other fascinating properties. The exact mechanisms leading to the thermalization of organic exciton-polaritons toward condensation are not yet understood, partly due to the complexity of organic molecules and partly to the canonical microcavities used in condensation studies, which limit broadband studies. Here, we exploit an entirely different cavity design, i.e., an array of plasmonic nanoparticles strongly coupled to organic molecules, to successfully measure the broadband ultrafast dynamics of the strongly coupled system. Sharp features emerge in the transient spectrum originating from the formation of a condensate with a well-defined molecular vibrational composition. These measurements represent the first direct experimental evidence that molecular vibrations drive condensation in organic systems and provide a benchmark for modeling the dynamics of organic-based exciton-polariton condensates.

Organic-Inorganic Hybrid Solution-Processed H2-Evolving Photocathodes.

Here we report for the first time an H2-evolving photocathode fabricated by a solution-processed organic-inorganic hybrid composed of CdSe and P3HT. The CdSe:P3HT (10:1 (w/w)) hybrid bulk heterojunction treated with 1,2-ethanedithiol (EDT) showed efficient water reduction and hydrogen generation. A photocurrent of -1.24 mA/cm(2) at 0 V versus reversible hydrogen electrode (V(RHE)), EQE of 15%, and an unprecedented Voc of 0.85 V(RHE) under illumination of AM1.5G (100 mW/cm(2)) in mild electrolyte were observed. Time-resolved photoluminescence (TRPL), internal quantum efficiency (IQE), and transient photocurrent measurements were carried out to clarify the carrier dynamics of the hybrids. The exciton lifetime of CdSe was reduced by one order of magnitude in the hybrid blend, which is a sign of the fast charge separation upon illumination. By comparing the current magnitude of the solid-state devices and water-splitting devices made with identical active layers, we found that the interfaces of the water-splitting devices limit the device performance. The electron/hole transport properties investigated by comparing IQE spectra upon front- and back-side illumination evidenced balanced electron/hole transport. The Faradaic efficiency is 80-100% for the hybrid photocathodes with Pt catalysts and ∼70% for the one without Pt catalysts.