TY - JOUR
T1 - Heating and cooling of ligand-coated colloidal nanocrystals in solid films and solvent matrices
AU - Diroll, Benjamin T.
AU - Schaller, Richard D.
N1 - Funding Information:
†The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf on the Government. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. http://energy.gov/downloads/doe-public-access-plan ‡Electronic supplementary information (ESI) available. See DOI: 10.1039/ c9nr01473j
Funding Information:
This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357.
Publisher Copyright:
© The Royal Society of Chemistry 2019.
PY - 2019/5/7
Y1 - 2019/5/7
N2 - Ligand-to-nanocrystal heating and subsequent cooling to the environmental medium is investigated with infrared pump, electronic probe (IPEP) spectroscopy. Compared to solid films, solvated nanocrystals show faster ligand-to-nanocrystal heat equilibration (c. 11 ps versus c. 17 ps). Solvated nanocrystals also display more cooling of the hot ligand-nanocrystal complex on the experimentally measured time-scale, emphasizing the thermally insulating nature of semiconductor nanocrystal solids. Although heating transfer rates among solvents are all between 150 ps and 330 ps, cooling of the nanocrystal-ligand complex is slower, on average, in chlorinated solvents (c. 315 ps) compared to deuterated hydrocarbon solvents (c. 215 ps). Differences between chlorinated and hydrocarbon solvents show the importance of matching the vibrational energies of the solvent and the ligands for increasing the rate of heat transfer. Increases in the cooling time for poorer hydrocarbon solvents, in which nanocrystals aggregated, such as toluene, compared to better solvents, like methylcyclohexane, indicate that penetration of solvent into the ligand layer facilitates improved heat transfer to the matrix.
AB - Ligand-to-nanocrystal heating and subsequent cooling to the environmental medium is investigated with infrared pump, electronic probe (IPEP) spectroscopy. Compared to solid films, solvated nanocrystals show faster ligand-to-nanocrystal heat equilibration (c. 11 ps versus c. 17 ps). Solvated nanocrystals also display more cooling of the hot ligand-nanocrystal complex on the experimentally measured time-scale, emphasizing the thermally insulating nature of semiconductor nanocrystal solids. Although heating transfer rates among solvents are all between 150 ps and 330 ps, cooling of the nanocrystal-ligand complex is slower, on average, in chlorinated solvents (c. 315 ps) compared to deuterated hydrocarbon solvents (c. 215 ps). Differences between chlorinated and hydrocarbon solvents show the importance of matching the vibrational energies of the solvent and the ligands for increasing the rate of heat transfer. Increases in the cooling time for poorer hydrocarbon solvents, in which nanocrystals aggregated, such as toluene, compared to better solvents, like methylcyclohexane, indicate that penetration of solvent into the ligand layer facilitates improved heat transfer to the matrix.
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U2 - 10.1039/c9nr01473j
DO - 10.1039/c9nr01473j
M3 - Article
C2 - 30972391
AN - SCOPUS:85064895000
VL - 11
SP - 8204
EP - 8209
JO - Nanoscale
JF - Nanoscale
SN - 2040-3364
IS - 17
ER -