Optical Response of Monolayer CdTe/CdS Quantum Dots to X-rays and Gamma-rays

TL;DR

This study examines how X-ray and gamma-ray irradiation affect the optical properties of monolayer CdTe/CdS quantum dots embedded in silica, revealing irradiation-induced changes and potential for optical dosimeter applications.

Contribution

It provides new insights into the effects of high-energy radiation on quantum dot optical properties and demonstrates methods for reversing irradiation-induced photodarkening.

Findings

X-ray irradiation causes exponential decrease in emission intensity and blue-shift.

Gamma-ray irradiation results in significant photodarkening without blue-shift.

Surface re-passivation can partially or fully reverse irradiation effects.

Abstract

We investigate the influence of X-ray and gamma-ray irradiation on the photophysical properties of sub-monolayer CdTe/CdS quantum dots (QDs) immobilized in porous silica (PSiO2) scaffolds. The highly luminescent QD-PSiO2 thin films allow for straightforward monitoring of the optical properties of the QDs through continuous wave and time-resolved photoluminescence spectroscopy. The PSiO2 host matrix itself does not modify the QD properties. X-ray irradiation of the QD-PSiO2 films in air leads to an exponential decrease in QD emission intensity, an exponential blue-shift in peak emission energy, and substantially faster exciton decay rates with increasing exposure doses from 2.2 Mrad(SiO2) to 6.6 Mrad(SiO2). Gamma-ray irradiation of a QD-PSiO2 thin film at a total exposure dose of 700 krad(SiO2) in a nitrogen environment results in over 80% QD photodarkening but no concurrent blue-shift in peak emission energy due to a lack of photo-oxidative effects. Near-complete and partial reversal of irradiation-induced photodarkening was demonstrated on X-ray and gamma-ray irradiated samples, respectively, through the use of a surface re-passivating solution, suggesting that there are different contributing mechanisms responsible for photodarkening under different irradiation energies. This work contributes to improving the reliability and robustness of QD based heterogeneous devices that are exposed to high risk, high energy environments with the possibility of also developing QD-based large area, low-cost, re-useable, and flexible optical dosimeters.