Room-temperature exciton coherence and dephasing in two-dimensional nanostructures
Elsa Cassette, Ryan D. Pensack, Benoît Mahler, Gregory D. Scholes
Abstract
Open-access reader
Elsa Cassette, Ryan D. Pensack, Benoît Mahler, Gregory D. Scholes
Abstract
Open-access reader
Electronic coherence has attracted considerable attention for its possible role in dynamical processes in molecular systems. However, its detection is challenged by inhomogeneous line broadening and interference with vibrational coherences. In particular, reports of ‘persistent’ coherent exciton superpositions at room temperature remain controversial, as the related transitions give typically shorter optical dephasing times of about 10–20 fs. To rationalize these reported long-lived coherences, several models have been proposed, involving strong correlation in the mechanisms of decoherence or that electronic coherences may be sustained by resonant vibrational modes. Here we report a decisive example of electronic coherence occurring in a chemical system in a ‘warm and wet’ (room-temperature solution) environment, colloidal semiconductor nanoplatelets, where details are not obscured by vibrational coherences nor ensemble dephasing. Comparing the exciton and optical coherence times evidences a partial correlation of fluctuations underlying dephasing and allows us to elucidate decoherence mechanisms occurring in these samples. Evidence for exciton coherence in photosynthetic complexes raises questions about whether quantum processes can play a role in biological environments, which are warm and wet. Cassette et al. now demonstrate long-lived electronic coherence in colloidal nanoplatelets in solution and at room temperature.
OpenAlex reports 137 citations for this work. Citation counts describe recorded attention and do not establish research quality.
A contribution statement is not available in the OpenAlex record.
Method details are not available in the OpenAlex metadata.
Findings are not separately available in the OpenAlex metadata.
Limitations are not available in the OpenAlex metadata.
Application details are not available in the OpenAlex metadata.
Electronic coherence has attracted considerable attention for its possible role in dynamical processes in molecular systems. However, its detection is challenged by inhomogeneous line broadening and interference with vibrational coherences. In particular, reports of ‘persistent’ coherent exciton superpositions at room temperature remain controversial, as the related transitions give typically shorter optical dephasing times of about 10–20 fs. To rationalize these reported long-lived coherences, several models have been proposed, involving strong correlation in the mechanisms of decoherence or that electronic coherences may be sustained by resonant vibrational modes. Here we report a decisive example of electronic coherence occurring in a chemical system in a ‘warm and wet’ (room-temperature solution) environment, colloidal semiconductor nanoplatelets, where details are not obscured by vibrational coherences nor ensemble dephasing. Comparing the exciton and optical coherence times evidences a partial correlation of fluctuations underlying dephasing and allows us to elucidate decoherence mechanisms occurring in these samples. Evidence for exciton coherence in photosynthetic complexes raises questions about whether quantum processes can play a role in biological environments, which are warm and wet. Cassette et al. now demonstrate long-lived electronic coherence in colloidal nanoplatelets in solution and at room temperature.
Key concepts: Dephasing, Quantum decoherence, Coherence (philosophical gambling strategy), Exciton, Coherence time, Physics, Condensed matter physics, Semiconductor