Charge Separation Dynamics in CdSe/CdS Core/Shell Nanoplatelets Addressed by Coherent Electron Spin Precession

ACS Nano. 2020 Jun 23;14(6):7237-7244. doi: 10.1021/acsnano.0c02402. Epub 2020 May 29.

Abstract

We investigate the charge separation dynamics provided by carrier surface trapping in CdSe/CdS core/shell nanoplatelets by means of a three-laser-beam pump-orientation-probe technique, detecting the electron spin coherence at room temperature. Signals with two Larmor precession frequencies are found, which strongly differ in their dynamical characteristics and dependencies on pump power and shell thickness. The electron trapping process occurs on a time scale of about 10 ns, and the charge separation induced thereby has a long lifetime of up to hundreds of microseconds. On the other hand, the hole trapping requires times from subpicoseconds to hundreds of picoseconds, and the induced charge separation has a lifetime of a few nanoseconds. With increasing CdS shell thickness the hole trapping vanishes, while the electron trapping is still detectable. These findings have important implications for understanding the photophysical processes of nanoplatelets and other colloidal nanostructures.

Keywords: carrier trapping; charge separation; electron spin coherence; nanoplatelets; ultrafast transient spectroscopy.