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. Weathersby, Richard D. Schaller, Vanessa Wood, Xijie Wang, Jennifer A. Dionne, Dmitri V. Talapin, A. Paul Alivisatos, Alberto Salleo, Eran Rabani and Aaron M. Lindenberg ()
Additional contact information
Burak Guzelturk: Stanford University
Benjamin L. Cotts: Stanford University
Dipti Jasrasaria: University of California
John P. Philbin: University of California
David A. Hanifi: Stanford University
Brent A. Koscher: University of California
Arunima D. Balan: University of California
Ethan Curling: University of California
Marc Zajac: Stanford University
Suji Park: SLAC National Accelerator Laboratory
Nuri Yazdani: SLAC National Accelerator Laboratory
Clara Nyby: SLAC National Accelerator Laboratory
Vladislav Kamysbayev: University of Chicago
Stefan Fischer: Stanford University
Zach Nett: University of California
Xiaozhe Shen: SLAC National Accelerator Laboratory
Michael E. Kozina: SLAC National Accelerator Laboratory
Ming-Fu Lin: SLAC National Accelerator Laboratory
Alexander H. Reid: SLAC National Accelerator Laboratory
Stephen P. Weathersby: SLAC National Accelerator Laboratory
Richard D. Schaller: Argonne National Laboratory
Vanessa Wood: ETH Zurich
Xijie Wang: SLAC National Accelerator Laboratory
Jennifer A. Dionne: Stanford University
Dmitri V. Talapin: University of Chicago
A. Paul Alivisatos: University of California
Alberto Salleo: Stanford University
Eran Rabani: University of California
Aaron M. Lindenberg: Stanford University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-22116-0

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