Energy Gap Tuning and Carrier Dynamics in Colloidal Ge1-xSnx Quantum Dots

Optical transition energies and carrier dynamics in colloidally synthesized 2.0 +/- 0.8 nm Ge1-xSnx quantum dots (x = 0.055-0.236) having visible luminescence were investigated using steady-state and time-resolved photoluminescence (PL) spectroscopy supported by first-principles calculations. By changing Sn content from x = 0.055 to 0.236, experimentally determined HOMO LUMO gap at 15 K was tuned from 1.88 to 1.61 eV. Considering the size and compositional variations, these values were consistent with theoretically calculated ones. At 15 K, time resolved PL revealed slow decay of luminescence (3-27 mu s), likely due to the recombination of spin-forbidden dark excitons and recombination of carriers trapped at surface states. Increasing Sn concentration to 23.6% led to 1 order of magnitude faster recombination. At 295 K, PL decays were 3 orders of magnitude faster (9-28 ns) owing to the thermal activation of bright excitons and carrier detrapping from surface states.