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

Guzelturk, Burak; Utterback, James K.; Coropceanu, Igor; Kamysbayev, Vladislav; Janke, Eric M.; Zajac, Marc; Yazdani, Nuri; Cotts, Benjamin L.; Park, Suji; Sood, Aditya; Lin, Ming-Fu; Reid, Alexander H.; Kozina, Michael E.; Shen, Xiaozhe; Weathersby, Stephen P.; Wood, Vanessa; Salleo, Alberto; Wang, Xijie; Talapin, Dmitri V.; Ginsberg, Naomi S.; Lindenberg, Aaron M.

doi:10.1021/acsnano.0c00673

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

Journal Article · Wed Mar 25 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c00673· OSTI ID:1633324

^[1]; Utterback, James K. ^[2];

^[3]; Kamysbayev, Vladislav ^[3]; Janke, Eric M. ^[3]; Zajac, Marc ^[4]; Yazdani, Nuri ^[5]; Cotts, Benjamin L. ^[4]; Park, Suji ^[6];

^[6]; Lin, Ming-Fu ^[7]; Reid, Alexander H. ^[7]; Kozina, Michael E. ^[7]; Shen, Xiaozhe ^[7]; Weathersby, Stephen P. ^[7];

^[8]; Salleo, Alberto ^[4]; Wang, Xijie ^[7];

^[3];

^[9] more »

Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Univ. of California, Berkeley, CA (United States)
Univ. of Chicago, IL (United States)
Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); ETH Zurich (Switzerland)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
ETH Zurich (Switzerland)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Science

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits (PTL); SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515; SC0019140; SC0019375; AC02-05CH11231; ECCS-1542152; DMR-1420709

OSTI ID:: 1633324

Alternate ID(s):: OSTI ID: 1775377

Journal Information:: ACS Nano, Vol. 14, Issue 4; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
colloidal nanocrystals
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Title: Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

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