Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions

Yuxing Liang; Benjamin T. Diroll; Kae Lin Wong; Samantha M. Harvey; Michael Wasielewski; Wee Liat Ong; Richard D. Schaller; Jonathan A. Malen

doi:10.1021/acs.nanolett.2c04627

Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions

Yuxing Liang, Benjamin T. Diroll, Kae Lin Wong, Samantha M. Harvey, Michael Wasielewski, Wee Liat Ong^*, Richard D. Schaller, Jonathan A. Malen^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

Infrared-pump, electronic-probe (IPEP) spectroscopy is used to measure heat flow into and out of CdSe nanocrystals suspended in an organic solvent, where the surface ligands are initially excited with an infrared pump pulse. Subsequently, the heat is transferred from the excited ligands to the nanocrystals and in parallel to the solvent. Parallel heat transfer in opposite directions uniquely enables us to differentiate the thermal conductances at the nanocrystal/ligand and ligand/solvent interfaces. Using a novel solution to the heat diffusion equation, we fit the IPEP data to find that the nanocrystal/ligand conductances range from 88 to 135 MW m^-2 K^-1 and are approximately 1 order of magnitude higher than the ligand/solvent conductances, which range from 7 to 26 MW m^-2 K^-1. Transient nonequilibrium molecular dynamics (MD) simulations of nanocrystal suspensions agree with IPEP data and show that ligands bound to the nanocrystal by bidentate bonds have more than twice the per-ligand conductance as those bound by monodentate bonds.

Original language	English (US)
Pages (from-to)	3687-3693
Number of pages	7
Journal	Nano letters
Volume	23
Issue number	9
DOIs	https://doi.org/10.1021/acs.nanolett.2c04627
State	Published - May 10 2023

Funding

Y.L. and J.A.M. acknowledge support from National Science Foundation award number ENG CBET-2017159, and S.M.H. and R.D.S. acknowledge support from National Science Foundation award number CHE-MSN1808590. W.-L.O. was a principal supervisor supported by the National Natural Science Foundation of China (grant numbers 52150410417 and 51876186), the Natural Science Foundation of Zhejiang Province (grant number LZ19E060002), the Fundamental Research Funds for the Central Universities, the ZJU-UIUC Institute, and the Zhejiang-Saudi EMC2 Laboratory. Work performed by Kae-Lin Wong was supported by CSC Scholarship. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

Keywords

Interfacial thermal conductance
semiconductor nanocrystal

ASJC Scopus subject areas

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.2c04627

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@article{2815a951e22b451ab24f4deb82f3c7dc,

title = "Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions",

abstract = "Infrared-pump, electronic-probe (IPEP) spectroscopy is used to measure heat flow into and out of CdSe nanocrystals suspended in an organic solvent, where the surface ligands are initially excited with an infrared pump pulse. Subsequently, the heat is transferred from the excited ligands to the nanocrystals and in parallel to the solvent. Parallel heat transfer in opposite directions uniquely enables us to differentiate the thermal conductances at the nanocrystal/ligand and ligand/solvent interfaces. Using a novel solution to the heat diffusion equation, we fit the IPEP data to find that the nanocrystal/ligand conductances range from 88 to 135 MW m-2 K-1 and are approximately 1 order of magnitude higher than the ligand/solvent conductances, which range from 7 to 26 MW m-2 K-1. Transient nonequilibrium molecular dynamics (MD) simulations of nanocrystal suspensions agree with IPEP data and show that ligands bound to the nanocrystal by bidentate bonds have more than twice the per-ligand conductance as those bound by monodentate bonds.",

keywords = "Interfacial thermal conductance, semiconductor nanocrystal",

author = "Yuxing Liang and Diroll, \{Benjamin T.\} and Wong, \{Kae Lin\} and Harvey, \{Samantha M.\} and Michael Wasielewski and Ong, \{Wee Liat\} and Schaller, \{Richard D.\} and Malen, \{Jonathan A.\}",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

year = "2023",

month = may,

day = "10",

doi = "10.1021/acs.nanolett.2c04627",

language = "English (US)",

volume = "23",

pages = "3687--3693",

journal = "Nano letters",

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T1 - Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions

AU - Liang, Yuxing

AU - Diroll, Benjamin T.

AU - Wong, Kae Lin

AU - Harvey, Samantha M.

AU - Wasielewski, Michael

AU - Ong, Wee Liat

AU - Schaller, Richard D.

AU - Malen, Jonathan A.

PY - 2023/5/10

Y1 - 2023/5/10

N2 - Infrared-pump, electronic-probe (IPEP) spectroscopy is used to measure heat flow into and out of CdSe nanocrystals suspended in an organic solvent, where the surface ligands are initially excited with an infrared pump pulse. Subsequently, the heat is transferred from the excited ligands to the nanocrystals and in parallel to the solvent. Parallel heat transfer in opposite directions uniquely enables us to differentiate the thermal conductances at the nanocrystal/ligand and ligand/solvent interfaces. Using a novel solution to the heat diffusion equation, we fit the IPEP data to find that the nanocrystal/ligand conductances range from 88 to 135 MW m-2 K-1 and are approximately 1 order of magnitude higher than the ligand/solvent conductances, which range from 7 to 26 MW m-2 K-1. Transient nonequilibrium molecular dynamics (MD) simulations of nanocrystal suspensions agree with IPEP data and show that ligands bound to the nanocrystal by bidentate bonds have more than twice the per-ligand conductance as those bound by monodentate bonds.

AB - Infrared-pump, electronic-probe (IPEP) spectroscopy is used to measure heat flow into and out of CdSe nanocrystals suspended in an organic solvent, where the surface ligands are initially excited with an infrared pump pulse. Subsequently, the heat is transferred from the excited ligands to the nanocrystals and in parallel to the solvent. Parallel heat transfer in opposite directions uniquely enables us to differentiate the thermal conductances at the nanocrystal/ligand and ligand/solvent interfaces. Using a novel solution to the heat diffusion equation, we fit the IPEP data to find that the nanocrystal/ligand conductances range from 88 to 135 MW m-2 K-1 and are approximately 1 order of magnitude higher than the ligand/solvent conductances, which range from 7 to 26 MW m-2 K-1. Transient nonequilibrium molecular dynamics (MD) simulations of nanocrystal suspensions agree with IPEP data and show that ligands bound to the nanocrystal by bidentate bonds have more than twice the per-ligand conductance as those bound by monodentate bonds.

KW - Interfacial thermal conductance

KW - semiconductor nanocrystal

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Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions

Abstract

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Keywords

ASJC Scopus subject areas

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