Extended Data Fig. 3: Atomistic insight into electronic wavefunction delocalization and dephasing in CsPbBr3 quantum dots via ab initio molecular dynamics at the DFT level of theory.
From: Single-photon superradiance in individual caesium lead halide quantum dots
a, The HOMO wavefunction delocalizes across the quantum dot and increases in size as the quantum dot diameter increases from 1.8 nm to 5.4 nm. b, Representative snapshot of the HOMO density at 3 K (left) and 150 K (right) projected onto the y-z plane. c, Time-averaged inverse participation ratio (IPR; degree of localization) of the HOMO density obtained at various temperatures, revealing thermally induced localization of the HOMO density. Simulations performed in the canonical ensemble (NVT, blue) and the microcanonical ensemble (NVE, red) return the similar localization. Error bars indicate 95% confidence intervals. d, Temperature-dependence of the time-averaged root-mean-squared displacement of the HOMO density center from the QD center, showing thermally induced dynamic spatial fluctuations. Error bars indicate 95% confidence intervals. e–g, Phonon-induced electronic dephasing in CsPbBr3 QDs: the dephasing function D(t) related to the HOMO at (e) 3 K and (f) 150 K, respectively, is obtained from the temporal fluctuations of the HOMO energy (see insets). g, The extracted pure-dephasing time τ2* strongly decreases with increasing temperature.
