American Chemical Society
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Anomalous Emission Shift of CdSe/CdS/ZnS Quantum Dots at Cryogenic Temperatures

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journal contribution
posted on 2022-03-23, 15:36 authored by Shaojie Liu, Yufei Shu, Meiyi Zhu, Haiyan Qin, Xiaogang Peng
The band-gap energy of most bulk semiconductors tends to increase as the temperature decreases. However, non-monotonic temperature dependence of the emission energy has been observed in semiconductor quantum dots (QDs) at cryogenic temperatures. Here, using stable and highly efficient CdSe/CdS/ZnS QDs as the model system, we quantitatively reveal the origins of the anomalous emission red-shift (∼8 meV) below 40 K by correlating ensemble and single QD spectroscopy measurements. About one-quarter of the anomalous red-shift (∼2.2 meV) is caused by the temperature-dependent population of the band-edge exciton fine levels. The enhancement of electron-optical phonon coupling caused by the increasing population of dark excitons with temperature decreases contributes an ∼3.4 meV red-shift. The remaining ∼2.4 meV red-shift is attributed to temperature-dependent electron-acoustic phonon coupling.