Theoretical Model for Luminescence Broadening and Anomalous Carrier Dynamics in Chalcopyrite Quantum Dots

Mukherjee, A and Mondal, P and Pandey, A and Narayan, A (2021) Theoretical Model for Luminescence Broadening and Anomalous Carrier Dynamics in Chalcopyrite Quantum Dots. In: Journal of Physical Chemistry C .

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Abstract

We present a theoretical approach to understanding the role of defect states in hole localization in chalcopyrite quantum dots. The total energy of the electron-phonon coupled system is modeled using harmonic oscillators. The model successfully explains results from a number of separate experimental studies using a single set of parameters. The hole transfer rate from the valence band to a defect state is calculated to be 3.3 ps. Our analysis, in conjunction with the emission line width and the Stokes shift observed in these quantum dots, suggests that along with the vibronic coupling, the copper d-orbital participation to the valence band needs to be considered. In addition, we explain the radiative lifetime observed in these systems in terms of fine-structure. We furthermore study the temporal evolution of spontaneous emission rates in these quantum dots. Our results (change of radiative lifetime over �10 ps) match extremely well with the experimentally reported values (�15 ps). © 2021 American Chemical Society.

Item Type:	Journal Article
Publication:	Journal of Physical Chemistry C
Publisher:	American Chemical Society
Additional Information:	The copyright for this article belongs to American Chemical Society
Keywords:	Copper compounds; Defects; Nanocrystals; Phonons; Valence bands, Harmonic oscillators; Hole transfer rate; Radiative lifetime; Single set of parameters; Spontaneous emission rates; Temporal evolution; Theoretical approach; Theoretical modeling, Semiconductor quantum dots
Department/Centre:	Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited:	03 Dec 2021 06:48
Last Modified:	03 Dec 2021 06:48
URI:	http://eprints.iisc.ac.in/id/eprint/70100

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