Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals.

Autor: Guzelturk B; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA. burakg@anl.gov.; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. burakg@anl.gov.; X-ray Science Division, Argonne National Laboratory, Lemont, IL, USA. burakg@anl.gov., Cotts BL; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA., Jasrasaria D; Department of Chemistry, University of California, Berkeley, CA, USA., Philbin JP; Department of Chemistry, University of California, Berkeley, CA, USA., Hanifi DA; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.; Department of Chemistry, University of California, Berkeley, CA, USA., Koscher BA; Department of Chemistry, University of California, Berkeley, CA, USA.; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA., Balan AD; Department of Chemistry, University of California, Berkeley, CA, USA.; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA., Curling E; Department of Chemistry, University of California, Berkeley, CA, USA., Zajac M; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA., Park S; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Yazdani N; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.; Department of Information Technology and Electrical Engineering, ETH Zurich, Zurich, Switzerland., Nyby C; The PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Kamysbayev V; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, IL, USA., Fischer S; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA., Nett Z; Department of Chemistry, University of California, Berkeley, CA, USA., Shen X; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Kozina ME; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Lin MF; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Reid AH; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Weathersby SP; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Schaller RD; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA.; Department of Chemistry, Northwestern University, Evanston, IL, USA., Wood V; Department of Information Technology and Electrical Engineering, ETH Zurich, Zurich, Switzerland., Wang X; SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Dionne JA; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA., Talapin DV; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, IL, USA.; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA., Alivisatos AP; Department of Chemistry, University of California, Berkeley, CA, USA.; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.; Department of Materials Science and Engineering, University of California, Berkeley, CA, USA.; Kavli Energy NanoScience Institute, Berkeley, CA, USA., Salleo A; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA., Rabani E; Department of Chemistry, University of California, Berkeley, CA, USA.; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.; The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv, Israel., Lindenberg AM; Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA. aaronl@stanford.edu.; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. aaronl@stanford.edu.; The PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA, USA. aaronl@stanford.edu.; Department of Photon Science, Stanford University and SLAC National Accelerator Laboratory, Menlo Park, CA, USA. aaronl@stanford.edu.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2021 Mar 25; Vol. 12 (1), pp. 1860. Date of Electronic Publication: 2021 Mar 25.
DOI: 10.1038/s41467-021-22116-0
Abstrakt: 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.
Databáze: MEDLINE
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