Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy.

Autor:	Guzelturk B; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States., Utterback JK; Department of Chemistry, University of California, Berkeley, California 94720, United States., Coropceanu I; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States., Kamysbayev V; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States., Janke EM; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States., Zajac M; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States., Yazdani N; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States.; Department of Information Technology and Electrical Engineering, ETH Zurich, 8092 Zurich, Switzerland., Cotts BL; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States., Park S; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States., Sood A; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States., Lin MF; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Reid AH; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Kozina ME; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Shen X; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Weathersby SP; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Wood V; Department of Information Technology and Electrical Engineering, ETH Zurich, 8092 Zurich, Switzerland., Salleo A; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States., Wang X; SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States., Talapin DV; Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States., Ginsberg NS; Department of Chemistry, University of California, Berkeley, California 94720, United States.; Department of Physics, University of California, Berkeley, California 94720, United States.; Molecular Biophysics and Integrated Bioimaging Division and Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.; Kavli Energy NanoSciences Institute, Berkeley, California 94720, United States., Lindenberg AM; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States.; The PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.; Department of Photon Science, Stanford University and SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
Jazyk:	angličtina
Zdroj:	ACS nano [ACS Nano] 2020 Apr 28; Vol. 14 (4), pp. 4792-4804. Date of Electronic Publication: 2020 Mar 30.
DOI:	10.1021/acsnano.0c00673
Abstrakt:	Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. Here, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron-phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron-phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism ( i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.
Databáze:	MEDLINE
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