DataVXChemistry of MaterialsPaper
journal article·2019-09-10Open access

Electron–Phonon Couplings Inherent in Polarons Drive Exciton Dynamics in Two-Dimensional Metal-Halide Perovskites

Félix Thouin, Ajay Ram Srimath Kandada, David A. Valverde-Chávez, Daniele Cortecchia, Ilaria Bargigia, Annamaria Petrozza, Xunmo Yang, Eric R. Bittner, Carlos Silva

Chemistry of Materials· Volume 31· Issue 17
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Source abstract

Abstract

We report on the exciton formation and relaxation dynamics following photocarrier injection in a single-layer two-dimensional lead-iodide perovskite. We probe the time evolution of four distinct exciton resonances by means of time-resolved photoluminescence and transient absorption spectroscopies and find that at 5 K a subset of excitons form on a ≲ 1 ps time scale and that these relax subsequently to lower-energy excitons on ∼5–10 ps with a marked temperature dependence over <100 K. We implement a mode projection analysis that determines the relative contribution of all observed phonons with frequency ≤ 50 cm–1 to interexciton nonadiabatic coupling, which in turn determines the rate of exciton relaxation. This analysis ranks the relative contributions of the phonons that participate in polaronic lattice distortions to the exciton interconversion dynamics and thus establishes their role in the nonadiabatic mixing of exciton states, and thus in the exciton relaxation rate.
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Research context

Electronic materials

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Quantum Dots Synthesis And Properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Physics, Georgia Institute of Technology, 837 State Street NW, Atlanta, Georgia 30332, United States

Center for Nano Science and Technology@PoliMi, Istituto Italiano di Tecnologia, via Giovanni Pascoli 70/3, 20133 Milano, Italy

School of Chemistry and Biochemistry, Georgia Institute of Technology, 901 Atlantic Drive NW, Atlanta, Georgia 30332, United States

Google, 1600 Amphitheatre Parkway, Mountain View, California 94043, United States

Department of Chemistry, University of Houston, Houston, Texas 77204, United States

Department of Physics, Durham University, South Road, Durham DH1 3LE, United Kingdom

Funding

Division of Chemistry · Welch Foundation · Leverhulme Trust · Fonds de Recherche du Qu?bec - Nature et Technologies · H2020 Marie Sklodowska-Curie Actions · Natural Sciences and Engineering Research Council of Canada · Division of Materials Research · National Science Foundation · School of Chemistry and Biochemistry and the College of Science of Georgia Institute of Technology

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