Photon Recycling in CsPbBr3 All-Inorganic Perovskite Nanocrystals. 2021

Marco van der Laan, and Chris de Weerd, and Lucas Poirier, and Oscar van de Water, and Deepika Poonia, and Leyre Gomez, and Sachin Kinge, and Laurens D A Siebbeles, and A Femius Koenderink, and Tom Gregorkiewicz, and Peter Schall
Institute of Physics, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands.

Photon recycling, the iterative process of re-absorption and re-emission of photons in an absorbing medium, can play an important role in the power-conversion efficiency of photovoltaic cells. To date, several studies have proposed that this process may occur in bulk or thin films of inorganic lead-halide perovskites, but conclusive proof of the occurrence and magnitude of this effect is missing. Here, we provide clear evidence and quantitative estimation of photon recycling in CsPbBr3 nanocrystal suspensions by combining measurements of steady-state and time-resolved photoluminescence (PL) and PL quantum yield with simulations of photon diffusion through the suspension. The steady-state PL shows clear spectral modifications including red shifts and quantum yield decrease, while the time-resolved measurements show prolonged PL decay and rise times. These effects grow as the nanocrystal concentration and distance traveled through the suspension increase. Monte Carlo simulations of photons diffusing through the medium and exhibiting absorption and re-emission account quantitatively for the observed trends and show that up to five re-emission cycles are involved. We thus identify 4 quantifiable measures, PL red shift, PL QY, PL decay time, and PL rise time that together all point toward repeated, energy-directed radiative transfer between nanocrystals. These results highlight the importance of photon recycling for both optical properties and photovoltaic applications of inorganic perovskite nanocrystals.

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