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

Ghosh, Arnab; Liu, Albert; Boehme, Simon C.; Brosseau, Patrick; Dirin, Dmitry N.; Kovalenko, Maksym V.; Kambhampati, Patanjali

doi:10.1021/acsnano.5c03051

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

Journal Article · Sun May 18 00:00:00 EDT 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5c03051· OSTI ID:2587789

^[1]; ^[2]; ^[3]; Brosseau, Patrick ^[1]; ^[3]; ^[3]; ^[1]

McGill Univ., Montreal, QC (Canada)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology, Dübendorf (Switzerland)

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. In conclusion, 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: European Research Council (ERC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2587789

Report Number(s):: BNL--228519-2025-JAAM

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 21 Vol. 19; ISSN 1936-0851; ISSN 1936-086X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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