Hot Carrier Dynamics in Perovskite Nanocrystal Solids: Role of the Cold Carriers, Nanoconfinement, and the Surface

Nano Letters
Thomas R HopperArtem A Bakulin

Abstract

Carrier cooling is of widespread interest in the field of semiconductor science. It is linked to carrier-carrier and carrier-phonon coupling and has profound implications for the photovoltaic performance of materials. Recent transient optical studies have shown that a high carrier density in lead-halide perovskites (LHPs) can reduce the cooling rate through a "phonon bottleneck". However, the role of carrier-carrier interactions, and the material properties that control cooling in LHPs, is still disputed. To address these factors, we utilize ultrafast "pump-push-probe" spectroscopy on LHP nanocrystal (NC) films. We find that the addition of cold carriers to LHP NCs increases the cooling rate, competing with the phonon bottleneck. By comparing different NCs and bulk samples, we deduce that the cooling behavior is intrinsic to the LHP composition and independent of the NC size or surface. This can be contrasted with other colloidal nanomaterials, where confinement and trapping considerably influence the cooling dynamics.

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Citations

Aug 19, 2020·Physical Chemistry Chemical Physics : PCCP·Thomas R HopperArtem A Bakulin
Jun 3, 2020·Nature Communications·Marcello RighettoTze Chien Sum
Jun 3, 2021·Journal of the American Chemical Society·Oliviero CannelliGiulia F Mancini
Jun 18, 2021·ACS Nano·Amrita DeyLakshminarayana Polavarapu
Sep 10, 2020·The Journal of Physical Chemistry Letters·La Moyne Tyler MixDmitry A Yarotski
Sep 10, 2020·ACS Omega·Dolf TimmermanYasufumi Fujiwara
Jan 9, 2021·Nano Letters·Yocefu HattoriJacinto Sá
Sep 4, 2021·The Journal of Physical Chemistry Letters·Xijia ZhengArtem A Bakulin

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