Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation

Richard D. Schaller; Samantha M. Harvey; Daniel W. Houck; Matthew S. Kirschner; Nathan C. Flanders; Alexandra Brumberg; Ariel A. Leonard; Nicolas E. Watkins; Lin X. Chen; William R. Dichtel; Xiaoyi Zhang; Brian A. Korgel; Michael R. Wasielewski

doi:10.1021/acsnano.0c05553

Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation

Richard D. Schaller^*, Samantha M. Harvey, Daniel W. Houck, Matthew S. Kirschner, Nathan C. Flanders, Alexandra Brumberg, Ariel A. Leonard, Nicolas E. Watkins, Lin X. Chen, William R. Dichtel, Xiaoyi Zhang, Brian A. Korgel, Michael R. Wasielewski

^*Corresponding author for this work

Chemistry

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

12 Scopus citations

Abstract

CuInSe2 nanocrystals offer promise for optoelectronics including thinfilm photovoltaics and printed electronics. Additive manufacturing methods such as photonic curing controllably sinter particles into quasi-continuous films and offer improved device performance. To gain understanding of nanocrystal response under such processing conditions, we investigate impacts of photoexcitation on colloidal nanocrystal lattices via time-resolved X-ray diffraction. We probe three sizes of particles and two capping ligands (oleylamine and inorganic S2-) to evaluate resultant crystal lattice temperature, phase stability, and thermal dissipation. Elevated fluences produce heating and loss of crystallinity, the onset of which exhibits particle size dependence. We find size-dependent recrystallization and cooling lifetimes ranging from 90 to 200 ps with additional slower cooling on the nanosecond time scale. Sulfide-capped nanocrystals show faster recrystallization and cooling compared to oleylamine-capped nanocrystals. Using these lifetimes, we find interfacial thermal conductivities from 3 to 28 MW/(m2 K), demonstrating that ligand identity strongly influences thermal dissipation.

Original language	English (US)
Pages (from-to)	13548-13556
Number of pages	9
Journal	ACS nano
Volume	14
Issue number	10
DOIs	https://doi.org/10.1021/acsnano.0c05553
State	Published - Oct 27 2020

Funding

We acknowledge student support from the National Science Foundation Macromolecular, Supramolecular, and Nanochemistry Program, NSF CHE 1808590. This work was supported by the National Science Foundation Graduate Research Fellowship Program under Grant DGE-1842165 (S.M.H., A.B., N.E.W.). We acknowledge support from the Ultrafast Initiative of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory under Contract DE-AC02-06CH11357. B.A.K and D.W.H. acknowledge support from the Robert A. Welch Foundation (F-1464) and the National Science Foundation (IIP-182206 and IIP-1540028). Parts of this work were performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, E.I. DuPont de Nemours & Co., and the Dow Chemical Company. N.C.F. and L.X.C. are partially supported by Basic Energy Science, CBG Division, US Department of Energy through Argonne National Laboratory under Contract DE-AC02-06CH11357. N.C.F., R.R.L., and W.R.D. are partially supported by the Army Research Office for a Multidisciplinary University Research Initiatives (MURI) award under Grant W911NF-15-1-0447. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DE-FG02-99ER14999 (M.R.W.). This work was performed, in part, at the Center for Nanoscale Materials and the Advanced Photon Source, both U.S. Department of Energy, Office of Science User Facilities, and supported by the U.S. Department of Energy, Office of Science, under Contract DE-AC02-06CH11357.

Keywords

CuInSe2
Heat dissipation
Ligand
Melting
Time-resolved X-ray diffraction

ASJC Scopus subject areas

General Materials Science
General Engineering
General Physics and Astronomy

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsnano.0c05553

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Schaller, R. D., Harvey, S. M., Houck, D. W., Kirschner, M. S., Flanders, N. C., Brumberg, A., Leonard, A. A., Watkins, N. E., Chen, L. X., Dichtel, W. R., Zhang, X., Korgel, B. A., & Wasielewski, M. R. (2020). Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation. ACS nano, 14(10), 13548-13556. https://doi.org/10.1021/acsnano.0c05553

@article{f995ecbb7f994854a703ad07d34cccd2,

title = "Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation",

abstract = "CuInSe2 nanocrystals offer promise for optoelectronics including thinfilm photovoltaics and printed electronics. Additive manufacturing methods such as photonic curing controllably sinter particles into quasi-continuous films and offer improved device performance. To gain understanding of nanocrystal response under such processing conditions, we investigate impacts of photoexcitation on colloidal nanocrystal lattices via time-resolved X-ray diffraction. We probe three sizes of particles and two capping ligands (oleylamine and inorganic S2-) to evaluate resultant crystal lattice temperature, phase stability, and thermal dissipation. Elevated fluences produce heating and loss of crystallinity, the onset of which exhibits particle size dependence. We find size-dependent recrystallization and cooling lifetimes ranging from 90 to 200 ps with additional slower cooling on the nanosecond time scale. Sulfide-capped nanocrystals show faster recrystallization and cooling compared to oleylamine-capped nanocrystals. Using these lifetimes, we find interfacial thermal conductivities from 3 to 28 MW/(m2 K), demonstrating that ligand identity strongly influences thermal dissipation.",

keywords = "CuInSe2, Heat dissipation, Ligand, Melting, Time-resolved X-ray diffraction",

author = "Schaller, {Richard D.} and Harvey, {Samantha M.} and Houck, {Daniel W.} and Kirschner, {Matthew S.} and Flanders, {Nathan C.} and Alexandra Brumberg and Leonard, {Ariel A.} and Watkins, {Nicolas E.} and Chen, {Lin X.} and Dichtel, {William R.} and Xiaoyi Zhang and Korgel, {Brian A.} and Wasielewski, {Michael R.}",

note = "Publisher Copyright: {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = oct,

day = "27",

doi = "10.1021/acsnano.0c05553",

language = "English (US)",

volume = "14",

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Schaller, RD, Harvey, SM, Houck, DW, Kirschner, MS, Flanders, NC, Brumberg, A, Leonard, AA, Watkins, NE, Chen, LX , Dichtel, WR, Zhang, X, Korgel, BA & Wasielewski, MR 2020, 'Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation', ACS nano, vol. 14, no. 10, pp. 13548-13556. https://doi.org/10.1021/acsnano.0c05553

TY - JOUR

T1 - Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation

AU - Schaller, Richard D.

AU - Harvey, Samantha M.

AU - Houck, Daniel W.

AU - Kirschner, Matthew S.

AU - Flanders, Nathan C.

AU - Brumberg, Alexandra

AU - Leonard, Ariel A.

AU - Watkins, Nicolas E.

AU - Chen, Lin X.

AU - Dichtel, William R.

AU - Zhang, Xiaoyi

AU - Korgel, Brian A.

AU - Wasielewski, Michael R.

PY - 2020/10/27

Y1 - 2020/10/27

N2 - CuInSe2 nanocrystals offer promise for optoelectronics including thinfilm photovoltaics and printed electronics. Additive manufacturing methods such as photonic curing controllably sinter particles into quasi-continuous films and offer improved device performance. To gain understanding of nanocrystal response under such processing conditions, we investigate impacts of photoexcitation on colloidal nanocrystal lattices via time-resolved X-ray diffraction. We probe three sizes of particles and two capping ligands (oleylamine and inorganic S2-) to evaluate resultant crystal lattice temperature, phase stability, and thermal dissipation. Elevated fluences produce heating and loss of crystallinity, the onset of which exhibits particle size dependence. We find size-dependent recrystallization and cooling lifetimes ranging from 90 to 200 ps with additional slower cooling on the nanosecond time scale. Sulfide-capped nanocrystals show faster recrystallization and cooling compared to oleylamine-capped nanocrystals. Using these lifetimes, we find interfacial thermal conductivities from 3 to 28 MW/(m2 K), demonstrating that ligand identity strongly influences thermal dissipation.

AB - CuInSe2 nanocrystals offer promise for optoelectronics including thinfilm photovoltaics and printed electronics. Additive manufacturing methods such as photonic curing controllably sinter particles into quasi-continuous films and offer improved device performance. To gain understanding of nanocrystal response under such processing conditions, we investigate impacts of photoexcitation on colloidal nanocrystal lattices via time-resolved X-ray diffraction. We probe three sizes of particles and two capping ligands (oleylamine and inorganic S2-) to evaluate resultant crystal lattice temperature, phase stability, and thermal dissipation. Elevated fluences produce heating and loss of crystallinity, the onset of which exhibits particle size dependence. We find size-dependent recrystallization and cooling lifetimes ranging from 90 to 200 ps with additional slower cooling on the nanosecond time scale. Sulfide-capped nanocrystals show faster recrystallization and cooling compared to oleylamine-capped nanocrystals. Using these lifetimes, we find interfacial thermal conductivities from 3 to 28 MW/(m2 K), demonstrating that ligand identity strongly influences thermal dissipation.

KW - CuInSe2

KW - Heat dissipation

KW - Ligand

KW - Melting

KW - Time-resolved X-ray diffraction

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JF - ACS nano

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Transient lattice response upon photoexcitation in CuInSe2 nanocrystals with organic or inorganic surface passivation

Abstract

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Keywords

ASJC Scopus subject areas

UN SDGs

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