Atomic fluctuations in electronic materials revealed by dephasing

Palato, Samuel; Seiler, Hélène; Nijjar, Parmeet; Prezhdo, Oleg; Kambhampati, Patanjali

doi:10.1073/pnas.1916792117

Atomic fluctuations in electronic materials revealed by dephasing

Journal Article · Thu May 14 00:00:00 EDT 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1916792117· OSTI ID:1802659

^[1]; ^[2]; Nijjar, Parmeet ^[3]; ^[3]; ^[2]

McGill Univ., Montreal, QC (Canada); McGill University
McGill Univ., Montreal, QC (Canada)
Univ. of Southern California, Los Angeles, CA (United States)

The microscopic origin and timescale of the fluctuations of the energies of electronic states has a significant impact on the properties of interest of electronic materials, with implication in fields ranging from photovoltaic devices to quantum information processing. Spectroscopic investigations of coherent dynamics provide a direct measurement of electronic fluctuations. Modern multidimensional spectroscopy techniques allow the mapping of coherent processes along multiple time or frequency axes and thus allow unprecedented discrimination between different sources of electronic dephasing. Exploiting modern abilities in coherence mapping in both amplitude and phase, we unravel dissipative processes of electronic coherences in the model system of CdSe quantum dots (QDs). The method allows the assignment of the nature of the observed coherence as vibrational or electronic. The expected coherence maps are obtained for the coherent longitudinal optical (LO) phonon, which serves as an internal standard and confirms the sensitivity of the technique. Fast dephasing is observed between the first two exciton states, despite their shared electron state and common environment. This result is contrary to predictions of the standard effective mass model for these materials, in which the exciton levels are strongly correlated through a common size dependence. In contrast, the experiment is in agreement with ab initio molecular dynamics of a single QD. Electronic dephasing in these materials is thus dominated by the realistic electronic structure arising from fluctuations at the atomic level rather than static size distribution. The analysis of electronic dephasing thereby uniquely enables the study of electronic fluctuations in complex materials.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Southern California, Los Angeles, CA (United States)

Sponsoring Organization:: Canada Foundation for Innovation; McGill University; Natural Sciences and Engineering Research Council of Canada (NERSC); Swiss National Science Foundation; USDOE Office of Science (SC)

Grant/Contract Number:: SC0014429

OSTI ID:: 1802659

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 22 Vol. 117; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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