2015•Nature CommunicationsOpen access

Room-temperature exciton coherence and dephasing in two-dimensional nanostructures

Elsa Cassette, Ryan D. Pensack, Benoît Mahler, Gregory D. Scholes

Open full text 137 citations

Abstract

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.

Open-access reader

About this research paper

What this paper is about

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.

Why it matters

OpenAlex reports 137 citations for this work. Citation counts describe recorded attention and do not establish research quality.

Key contribution

A contribution statement is not available in the OpenAlex record.

Method / approach

Method details are not available in the OpenAlex metadata.

Main findings

Findings are not separately available in the OpenAlex metadata.

Limitations

Limitations are not available in the OpenAlex metadata.

Applications

Application details are not available in the OpenAlex metadata.

Available abstract

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

Related papers

Back to paper searchBrowse research topicsOriginal source
Room-temperature exciton coherence and dephasing in two-dimensional nanostructures — Research Paper | ScholarLens