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Spatiotemporal Temperature and Pressure in Thermoplasmonic Gold Nanosphere-Water Systems

Lindley, Sarah A. and An, Qi and Goddard, William A., III and Cooper, Jason K. (2021) Spatiotemporal Temperature and Pressure in Thermoplasmonic Gold Nanosphere-Water Systems. ACS Nano, 15 (4). pp. 6276-6288. ISSN 1936-0851. doi:10.1021/acsnano.0c09804.

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We offer a detailed investigation of the photophysical properties of plasmonic solid and hollow gold nanospheres suspended in water by combining ultrafast transient absorption (TA) spectroscopy with molecular dynamics (MD) simulations. TA reveals that hollow gold nanospheres (HGNs) exhibit faster excited state relaxation and larger amplitude acoustic phonon modes than solid gold nanoparticles of the same outer diameter. MD simulation carried out on full scale nanoparticle–water models (over 10 million atoms) to simulate the temporal evolution (0–100 ps) of the thermally excited particles (1000 or 1250 K) provides atomic-scale resolution of the spatiotemporal temperature and pressure maps, as well as visualization of the lattice vibrational modes. For the 1000 K HGN, temperatures upward of 500 K in the vicinity of the shell surface were observed, along with pressures up to several hundred MPa in the inner cavity, revealing potential use as a photoinduced nanoreactor. Our approach of combining TA and MD provides a path to better understanding how thermal–structural properties (such as expansion and contraction) and thermal–optical properties (such as modulated dielectrics) manifest themselves as TA signatures. The detailed picture of heat transfer at interfaces should help guide nanoparticle design for a wide range of applications that rely on photothermal conversion, including photothermal coupling agents for nanoparticle-mediated photothermal therapy and photocatalysts for light-driven chemical reactions.

Item Type:Article
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URLURL TypeDescription
An, Qi0000-0003-4838-6232
Goddard, William A., III0000-0003-0097-5716
Cooper, Jason K.0000-0002-7953-4229
Additional Information:© 2021 American Chemical Society. Received: November 23, 2020; Accepted: February 17, 2021; Published: February 23, 2021. We acknowledge T. Yuzvinsky and the W.M. Keck Center for Nanoscale Optofluidics at University of California Santa Cruz for use of the FEI Quanta 3D dual beam microscope for SEM particle screening. We also acknowledge T. Yuzvinsky for fruitful discussion. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. We acknowledge support from the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under award no. DE-SC0004993. Calculations were performed using the Cori cluster at the National Energy Research Scientific Computing Center (NERSC) at the LBNL supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Q.A. received support from American Chemical Society Petroleum Research Fund (PRF# 58754-DNI6). Author Contributions: S.A.L. and Q.A. contributed equally. The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05CH11231
Department of Energy (DOE)DE-SC0004993
American Chemical Society Petroleum Research Fund58754-DNI6
Subject Keywords:thermoplasmonics, transient absorption spectroscopy, molecular dynamics, hollow gold nanospheres, surface plasmon resonance, heat transfer
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Issue or Number:4
Record Number:CaltechAUTHORS:20210224-122527044
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Official Citation:Spatiotemporal Temperature and Pressure in Thermoplasmonic Gold Nanosphere–Water Systems. Sarah A. Lindley, Qi An, William A. Goddard, and Jason K. Cooper. ACS Nano 2021 15 (4), 6276-6288; DOI: 10.1021/acsnano.0c09804
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108173
Deposited By: Tony Diaz
Deposited On:24 Feb 2021 20:34
Last Modified:06 Jun 2021 00:29

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