Disentangling the Electron and Hole Dynamics in Janus CdSe/PbSe Nanocrystals through Variable Pump Transient Absorption Spectroscopy

摘要： CdSe/PbSe Janus hetero-nanocrystals (HNCs) represent an interesting system where structurally immiscible CdSe and PbSe co-exist in a single structure with intermixed electronic states. Here, we have investigated the carrier dynamics in Janus CdSe/PbSe HNCs through ultrafast transient absorption spectroscopy by selectively exciting either the CdSe or the PbSe domains. Upon excitation of the CdSe domain sub-picosecond hole transfer to the hybrid interfacial PbSe states were identified. On the other hand, the transfer of hot electron from PbSe to CdSe was evident upon creation of hot electrons in PbSe domain without exciting the CdSe domain. The photo-excited hot hole also gets transferred to the hybrid interfacial states in sub-ps time (~1ps) bleaching the corresponding transition. The decay of the localized hole was found to be much slower compared to the electron which can be beneficial for carrier extraction and multiexciton generation. The finding of hot electron transfer in a single structure and slow decay of holes can thus prove to be advantageous for future design of photovoltaic devices.