Intrinsically Slow Cooling of Hot Electrons in CdSe Nanocrystals Compared to CdS

Coley-O’Rourke, Matthew J.; Hou, Bokang; Sherman, Skylar J.; Dukovic, Gordana; Rabani, Eran

doi:10.1021/acs.nanolett.4c04912

Intrinsically Slow Cooling of Hot Electrons in CdSe Nanocrystals Compared to CdS

Journal Article · Wed Dec 18 04:00:00 EST 2024 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.4c04912· OSTI ID:2546954

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University of California, Berkeley, CA (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of Colorado, Boulder, CO (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tel Aviv Univ. (Israel)

The utilization of excited charge carriers in semiconductor nanocrystals (NCs) for optoelectronic technologies has been a long-standing goal in the field of nanoscience. Experimental efforts to extend the lifetime of excited carriers have therefore been a principal focus. To understand the limits of these lifetimes, in this work, we theoretically study the time scales of pure electron relaxation in negatively charged NCs composed of two prototypical materials: CdSe and CdS. We find that hot electrons in CdSe have lifetimes that are 5 to 6 orders of magnitude longer than in CdS when the relaxation is governed only by the intrinsic properties of the materials. Although these two materials are known to have somewhat different electronic structure, we elucidate how this enormous difference in lifetimes arises from relatively small quantitative differences in electronic energy gaps and phonon frequencies, as well as the crucial role of Fröhlich-type electron–phonon couplings.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC)

Grant/Contract Number:: AC02-05CH11231; SC0022088

OSTI ID:: 2546954

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 1 Vol. 25; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Intrinsically Slow Cooling of Hot Electrons in CdSe Nanocrystals Compared to CdS

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