Direct Detection of Long-Range Interdomain Auger Recombination in Dumbbell-Shaped Quasi-Type-II Nanoparticle

J Phys Chem Lett. 2022 Jul 28;13(29):6845-6851. doi: 10.1021/acs.jpclett.2c01077. Epub 2022 Jul 21.

Abstract

Multicarrier dynamics in heterostructured ZnS-AgInS2 (ZAIS) dumbbell-like nanoparticle (nanodumbell), which consists of two visible-light absorptive domains (ellipsoidal tip domains) directly linked to each end of a 22 nm length rod domain of the ZAIS nanodumbell with a quasi-type-II heterostructure, was investigated by femtosecond transient absorption spectroscopy under variable excitation intensities. Quantitative analysis together with the numerical simulations for the excitation intensity dependence of the dynamics revealed that only one electron-hole pair survived in the overall dumbbell as a consequence of Auger recombination, even though multiple carriers were formed on both terminal tip domains. This result strongly suggested carrier-carrier interaction between the tip domains, leading to the long-range Auger recombination via tunneling across a rod potential barrier.