TY - JOUR
T1 - Nonequilibrium thermodynamics of colloidal gold nanocrystals monitored by ultrafast electron diffraction and optical scattering microscopy
AU - Guzelturk, Burak
AU - Lindenberg, Aaron M.
AU - Utterback, James K.
AU - Coropceanu, Igor
AU - Kamysbayev, Vladislav
AU - Janke, Eric M.
AU - Zajac, Marc
AU - Yazdani, Nuri
AU - Cotts, Benjamin L.
AU - Park, Suji
AU - Sood, Aditya
AU - Lin, Ming Fu
AU - Reid, Alexander H.
AU - Kozina, Michael E.
AU - Shen, Xiaozhe
AU - Weathersby, Stephen P.
AU - Wood, Vanessa
AU - Salleo, Alberto
AU - Wang, Xijie
AU - Talapin, Dmitri V.
AU - Ginsberg, Naomi S.
N1 - Funding Information:
We thank T. Giamarchi for very insightful discussions and J. White for estimating the longitudinal skyrmion correlation length in Cu2OSeO3 from small-angle neutron scattering data. We are grateful to D. Laub and B. Bártová for help with sample fabrication. This work was supported by the Swiss National Science Foundation (SNSF) through project 166298, the Sinergia network 171003 for Nanoskyrmionics and the National Center for Competence in Research 157956 on Molecular Ultrafast Science and Technology (NCCR MUST), as well as ERC project HERO. P.H. also acknowledges financial support from the Young Talent Support Plan of Xi’an Jiaotong University and the National Natural Science Foundation of China (project 11904277). L.H. and A.R. acknowledge financial support by the DFG within CRC1238 (C02) through project 277146847.
Funding Information:
The UED and stroboSCAT work is part of the “Photonics at Thermodynamic Limits” Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DESC0019140. MeV-UED is operated as part of the Linac Coherent Light Source at the SLAC National Accelerator Laboratory, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-76SF00515. We also acknowledge support for sample preparation and characterization from the Office of Basic Energy Sciences, the U.S. Department of Energy, under Award No. DE-SC0019375. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. E.J. was supported by the University of Chicago Materials Research Science and Engineering Center funded by NSF under Award No. DMR-1420709. N.Y. and V.W. acknowledge funding from Swiss National Science Foundation from the Quantum Sciences and Technology NCCR. J.K.U. acknowledges the Camille and Henry Dreyfus Foundation’s Postdoctoral Program in Environmental Chemistry. J.K.U. acknowledges Hannah Weaver and Jonathan Raybin for helpful discussions. M.Z., S.P., and A.S. acknowledge support from the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC02-76SF00515. N.S.G. and D.V.T. also acknowledge Alfred P. Sloan Research Fellowships, David and Lucile Packard Foundation Fellowships for Science and Engineering, and Camille and Henry Dreyfus Teacher-Scholar Awards.
Funding Information:
This work was supported by Institute for Basic Science under IBS-R012-D1. Hyung Taek Kim, Jae Hee Sung, and Seong Ku Lee are partially supported by GIST Research Institute(GRI) grant funded by the GIST in 2020. .
Funding Information:
The UED and stroboSCAT work is part of the ?Photonics at Thermodynamic Limits? Energy Frontier Research Center funded by the U.S. Department of Energy, O?ce of Science, O?ce of Basic Energy Sciences, under Award Number DESC0019140. MeV-UED is operated as part of the Linac Coherent Light Source at the SLAC National Accelerator Laboratory, supported by the U.S. Department of Energy, O?ce of Science, O?ce of Basic Energy Sciences, under Contract No. DE-AC02-76SF00515. We also acknowledge support for sample preparation and characterization from the O?ce of Basic Energy Sciences, the U.S. Department of Energy, under Award No. DE-SC0019375. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. E.J. was supported by the University of Chicago Materials Research Science and Engineering Center funded by NSF under Award No. DMR-1420709. N.Y. and V.W. acknowledge funding from Swiss National Science Foundation from the Quantum Sciences and Technology NCCR. J.K.U. acknowledges the Camille and Henry Dreyfus Foundation's Postdoctoral Program in Environmental Chemistry. J.K.U. acknowledges Hannah Weaver and Jonathan Raybin for helpful discussions. M.Z., S.P., and A.S. acknowledge support from the Department of Energy, O?ce of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC02-76SF00515. N.S.G. and D.V.T. also acknowledge Alfred P. Sloan Research Fellowships, David and Lucile Packard Foundation Fellowships for Science and Engineering, and Camille and Henry Dreyfus Teacher-Scholar Awards.
Funding Information:
The authors acknowledge support from the Federal State of Thuringia and the European Social Fund (ESF) Project 2018 FGR 0080
Publisher Copyright:
© 2020 American Chemical Society
PY - 2020/4/28
Y1 - 2020/4/28
N2 - 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.
AB - 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.
KW - Colloidal nanocrystals
KW - Electron−phonon coupling
KW - Hot carriers
KW - Ligands
KW - Thermal transport
KW - Time-resolved microscopy
KW - Ultrafast electron diffraction
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U2 - 10.1021/acsnano.0c00673
DO - 10.1021/acsnano.0c00673
M3 - Article
C2 - 32208676
AN - SCOPUS:85084168080
SN - 1936-0851
VL - 14
SP - 4792
EP - 4804
JO - ACS Nano
JF - ACS Nano
IS - 4
ER -