Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Burak Guzelturk, Benjamin L. Cotts, Dipti Jasrasaria, John P. Philbin, David A. Hanifi, Brent A. Koscher, Arunima D. Balan, Ethan Curling, Marc Zajac, Suji Park, Nuri Yazdani, Clara Nyby, Vladislav Kamysbayev, Stefan Fischer, Zach Nett, Xiaozhe Shen, Michael E. Kozina, Ming Fu Lin, Alexander H. Reid, Stephen P. WeathersbyRichard D. Schaller, Vanessa Wood, Xijie Wang, Jennifer A. Dionne, Dmitri V. Talapin, A. Paul Alivisatos, Alberto Salleo, Eran Rabani, Aaron M. Lindenberg

Research output: Contribution to journalArticlepeer-review

Abstract

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

Original languageEnglish
Article number1860
JournalNature communications
Volume12
Issue number1
DOIs
Publication statusPublished - Dec 2021

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

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