Correlated Lattice Fluctuations in CsPbBr₃ Quantum Dots Give Rise to Long-Lived Electronic Coherence.

Abstract

Electronic coherence is central to numerous areas of science, from quantum biology to quantum materials. In quantum materials, lead-halide perovskite (LHP) quantum dots (QDs) have been shown to support electronic coherence through observation of coherent single-photon emission and superfluorescence arising from spatial coherence at low temperatures. In contrast, direct measurement of temporal coherence between exciton states has been lacking. Here, we employ coherent multi-dimensional spectroscopy to observe an electronic coherence between exciton states in CsPbBr₃ QDs that is long-lived at room temperature, surviving nearly three times longer than the electronic dephasing time. This observation of a long-lived electronic coherence at room temperature points to nearly perfectly correlated lattice fluctuations for each excitonic state in the superposition. These experiments reveal that the properties of LHP QDs extend to lattice dynamics that give rise to correlated fluctuations in the basis exciton states, a process that may next be optimized by design.