"Intact" Carrier-Doping by Pump-Pump-Probe Spec-troscopy in Combination with Interfacial Charge Trans-fer: A Case Study of CsPbBr3 Nanocrystals

The Journal of Physical Chemistry Letters
Junhui WangKaifeng Wu

Abstract

Carrier-doping is important for semiconductor nanocrystals (NCs) as it offers a new knob to tune their functionalities in addition to size and shape control. Also, extensive studies on NC-devices have revealed that under operating conditions NCs are often unintentionally doped with electrons or holes. Thus, it is essential to be able to controllably dope NCs and study the carrier dynamics of doped NCs. The extension of previously-reported redox-doping methods to chemically-sensitive materials, such as recently-introduced perovskite NCs, has remained challenging. Here we introduce an "intact" carrier-doping method by performing pump-pump-probe transient absorption spectroscopy on NC-acceptor complexes. The first pump pulse is used to trigger charge-transfer from the NC to the acceptor, leading to NCs doped with a band edge carrier; the following pump-probe pulses measure the dynamics of carrier-doped NCs. We performed this measurement on CsPbBr3 NCs and deduced positive and nega-tive trion lifetimes of 220±50 ps and 150±40 ps, respectively, for 10-nm-diamter NCs, both dominated by Auger recombination. It also allowed us to identify randomly-photocharged excitons in CsPbBr3 NCs as positive trions.

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Citations

Jun 18, 2021·ACS Nano·Amrita DeyLakshminarayana Polavarapu
Jul 17, 2020·Journal of the American Chemical Society·Junhui WangKaifeng Wu
Mar 1, 2019·Journal of the American Chemical Society·Xiao LuoKaifeng Wu
Apr 23, 2019·ACS Applied Materials & Interfaces·Juvinch R VicenteJixin Chen
Jun 2, 2020·Journal of the American Chemical Society·Xiao LuoKaifeng Wu
Aug 15, 2019·The Journal of Physical Chemistry Letters·Shan HeKaifeng Wu
Aug 1, 2019·The Journal of Physical Chemistry Letters·Satoshi NakaharaYoshihiko Kanemitsu

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