Evidence of carrier diffusion between emission states in CdSe/ZnS core-shell quantum dots: a comprehensive investigation combining fluorescence lifetime correlation spectroscopy (FLCS) and single dot photoluminescence studies.

Autor: Acharjee D; School of Chemical Sciences, National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India. sghosh@niser.ac.in., Panda MK; School of Chemical Sciences, National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India. sghosh@niser.ac.in., Mahato AB; School of Chemical Sciences, National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India. sghosh@niser.ac.in., Das A; School of Chemical Sciences, National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India. sghosh@niser.ac.in., Ghosh S; School of Chemical Sciences, National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India. sghosh@niser.ac.in.; Center for Interdisciplinary Sciences (CIS), National Institute of Science Education and Research (NISER), An OCC of Homi Bhabha National Institute (HBNI), Khurda, Odisha 752050, India.
Jazyk: angličtina
Zdroj: Nanoscale [Nanoscale] 2024 Oct 10; Vol. 16 (39), pp. 18444-18454. Date of Electronic Publication: 2024 Oct 10.
DOI: 10.1039/d4nr02221a
Abstrakt: Investigation of carrier dynamics in CdSe/ZnS core-shell quantum dots (QDs) is performed using fluorescence-lifetime-correlation-spectroscopy (FLCS) and single-dot PL blinking studies. The origin of an emitted photon from a QD in an FLCS study is assigned to either an exciton state or trap state based on its excited state lifetime ( τ fl ). Subsequently, two intrastate autocorrelation functions (ACFs) representing the exciton and trap states and one cross-correlation function (CCF) coupling these two states are constructed. Interestingly, the timescales of carrier diffusion ( τ R ) show striking similarities across all three correlation functions, which further correlate with τ R of the conventional FCS. However, ACFs notably deviate from the CCF in their μs progression patterns, with the latter showing growth, whereas the former ones display decay. This implies inter-state carrier diffusions leading to the QD blinking. Further study of single particle PL blinking on a surface-immobilized QD indicates shallow trap states near the band edge cause the blinking at low excitation power, while trion recombination becomes an additional contributing factor at higher pump power. Overall, the results highlight not only an excellent correlation between these two techniques but also the potential of our approach for achieving an accurate and comprehensive understanding of carrier dynamics in CdSe/ZnS QDs.
Databáze: MEDLINE