4 years ago

Optical Transitions and Excitonic Properties of Ge1–xSnx Alloy Quantum Dots

Optical Transitions and Excitonic Properties of Ge1–xSnx Alloy Quantum Dots
Ümit Özgür, Shopan Hafiz, Tanner A. Nakagawara, Denis O. Demchenko, Richard J Alan Esteves, Indika U. Arachchige, Venkatesham Tallapally
Using hybrid functional calculations and experimental characterization, we analyze optical properties of 2–3 nm Ge1–xSnx alloy quantum dots, synthesized by colloidal chemistry methods. Hybrid functional theory, tuned to yield experimental bulk band structure of germanium, reproduces directly measured properties of Ge1–xSnx quantum dots, such as lattice constants, energy gaps, and absorption spectra. Time-dependent hybrid functional calculations yield optical absorption in good agreement with experiments, and allow probing the nature of the dark excitons in quantum dots. Calculations suggest a spin-forbidden dark exciton ground state, which is supported by the changes in the photoluminescence lifetimes with temperature and tin concentrations. The synthesis and theoretical understanding of Ge1–xSnx alloy quantum dots will add to the overall toolbox of low to nontoxic, silicon-compatible group IV semiconductors with potential application in visible to near-infrared optoelectronics.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b06458

DOI: 10.1021/acs.jpcc.7b06458

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