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.

Charge trapping can lead to severe nonradiative losses in colloidal semiconductor nanocrystals (NCs). The authors report femtosecond electron diffraction measurements on photoexcited NCs to reveal atomic-scale insights into how localization of charges at trap sites induce surface deformations.

Details

Title
Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals
Author
Guzelturk Burak 1   VIAFID ORCID Logo  ; Cotts, Benjamin L 2   VIAFID ORCID Logo  ; Jasrasaria Dipti 3   VIAFID ORCID Logo  ; Philbin, John P 3   VIAFID ORCID Logo  ; Hanifi, David A 4 ; Koscher, Brent A 5 ; Balan, Arunima D 5 ; Curling Ethan 3 ; Zajac, Marc 2 ; Park, Suji 6 ; Yazdani Nuri 7 ; Nyby Clara 8 ; Kamysbayev Vladislav 9 ; Fischer, Stefan 2 ; Nett Zach 3 ; Shen Xiaozhe 10   VIAFID ORCID Logo  ; Kozina, Michael E 10 ; Ming-Fu, Lin 10   VIAFID ORCID Logo  ; Reid, Alexander H 10   VIAFID ORCID Logo  ; Weathersby, Stephen P 10 ; Schaller, Richard D 11   VIAFID ORCID Logo  ; Wood, Vanessa 12   VIAFID ORCID Logo  ; Wang, Xijie 10   VIAFID ORCID Logo  ; Dionne, Jennifer A 2   VIAFID ORCID Logo  ; Talapin, Dmitri V 13   VIAFID ORCID Logo  ; Paul, Alivisatos A 14 ; Salleo Alberto 2   VIAFID ORCID Logo  ; Rabani Eran 15 ; Lindenberg, Aaron M 16   VIAFID ORCID Logo 

1  Stanford University, Department of Materials Science and Engineering, Stanford, USA (GRID:grid.168010.e) (ISNI:0000000419368956); SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771); Argonne National Laboratory, X-ray Science Division, Lemont, USA (GRID:grid.187073.a) (ISNI:0000 0001 1939 4845) 
2  Stanford University, Department of Materials Science and Engineering, Stanford, USA (GRID:grid.168010.e) (ISNI:0000000419368956) 
3  University of California, Department of Chemistry, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878) 
4  Stanford University, Department of Materials Science and Engineering, Stanford, USA (GRID:grid.168010.e) (ISNI:0000000419368956); University of California, Department of Chemistry, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878) 
5  University of California, Department of Chemistry, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878); Lawrence Berkeley National Laboratory, Materials Sciences Division, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551) 
6  SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771) 
7  SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771); ETH Zurich, Department of Information Technology and Electrical Engineering, Zurich, Switzerland (GRID:grid.5801.c) (ISNI:0000 0001 2156 2780) 
8  SLAC National Accelerator Laboratory, The PULSE Institute for Ultrafast Energy Science, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771) 
9  University of Chicago, Department of Chemistry and James Franck Institute, Chicago, USA (GRID:grid.170205.1) (ISNI:0000 0004 1936 7822) 
10  SLAC National Accelerator Laboratory, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771) 
11  Argonne National Laboratory, Center for Nanoscale Materials, Lemont, USA (GRID:grid.187073.a) (ISNI:0000 0001 1939 4845); Northwestern University, Department of Chemistry, Evanston, USA (GRID:grid.16753.36) (ISNI:0000 0001 2299 3507) 
12  ETH Zurich, Department of Information Technology and Electrical Engineering, Zurich, Switzerland (GRID:grid.5801.c) (ISNI:0000 0001 2156 2780) 
13  University of Chicago, Department of Chemistry and James Franck Institute, Chicago, USA (GRID:grid.170205.1) (ISNI:0000 0004 1936 7822); Argonne National Laboratory, Center for Nanoscale Materials, Lemont, USA (GRID:grid.187073.a) (ISNI:0000 0001 1939 4845) 
14  University of California, Department of Chemistry, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878); Lawrence Berkeley National Laboratory, Materials Sciences Division, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); University of California, Department of Materials Science and Engineering, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878); Kavli Energy NanoScience Institute, Berkeley, USA (GRID:grid.494610.e) (ISNI:0000 0004 4914 3563) 
15  University of California, Department of Chemistry, Berkeley, USA (GRID:grid.47840.3f) (ISNI:0000 0001 2181 7878); Lawrence Berkeley National Laboratory, Materials Sciences Division, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); Tel Aviv University, The Sackler Center for Computational Molecular and Materials Science, Tel Aviv, Israel (GRID:grid.12136.37) (ISNI:0000 0004 1937 0546) 
16  Stanford University, Department of Materials Science and Engineering, Stanford, USA (GRID:grid.168010.e) (ISNI:0000000419368956); SLAC National Accelerator Laboratory, Stanford Institute for Materials and Energy Sciences, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771); SLAC National Accelerator Laboratory, The PULSE Institute for Ultrafast Energy Science, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771); Stanford University and SLAC National Accelerator Laboratory, Department of Photon Science, Menlo Park, USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771) 
Publication year
2021
Publication date
2021
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
DOI
https://doi.org/10.1038/s41467-021-22116-0
ProQuest document ID
2505253363
Copyright
© This is a U.S. government work and not under copyright protection in the U.S.; foreign copyright protection may apply 2021. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.