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Title: The chemical physics of sequential infiltration synthesis—A thermodynamic and kinetic perspective

Abstract

Sequential infiltration synthesis (SIS) is an emerging materials growth method by which inorganic metal oxides are nucleated and grown within the free volume of polymers in association with chemical functional groups in the polymer. SIS enables the growth of novel polymer-inorganic hybrid materials, porous inorganic materials, and spatially templated nanoscale devices of relevance to a host of technological applications. Although SIS borrows from the precursors and equipment of atomic layer deposition (ALD), the chemistry and physics of SIS differ in important ways. These differences arise from the permeable three-dimensional distribution of functional groups in polymers in SIS, which contrast to the typically impermeable two-dimensional distribution of active sites on solid surfaces in ALD. In SIS, metal-organic vapor-phase precursors dissolve and diffuse into polymers and interact with these functional groups through reversible complex formation and/or irreversible chemical reactions. In this perspective, we describe the thermodynamics and kinetics of SIS and attempt to disentangle the tightly coupled physical and chemical processes that underlie this method. Here, we discuss the various experimental, computational, and theoretical efforts that provide insight into SIS mechanisms and identify approaches that may fill out current gaps in knowledge and expand the utilization of SIS.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States); Energy Frontier Research Center (EFRC), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Energy Frontier Research Center (EFRC), Lemont, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; USDOE Office of Science (SC), Energy Frontier Research Center
OSTI Identifier:
1592570
Alternate Identifier(s):
OSTI ID: 1574546
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 19; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Waldman, Ruben Z., Mandia, David J., Yanguas-Gil, Angel, Martinson, Alex B. F., Elam, Jeffrey W., and Darling, Seth B. The chemical physics of sequential infiltration synthesis—A thermodynamic and kinetic perspective. United States: N. p., 2019. Web. doi:10.1063/1.5128108.
Waldman, Ruben Z., Mandia, David J., Yanguas-Gil, Angel, Martinson, Alex B. F., Elam, Jeffrey W., & Darling, Seth B. The chemical physics of sequential infiltration synthesis—A thermodynamic and kinetic perspective. United States. doi:10.1063/1.5128108.
Waldman, Ruben Z., Mandia, David J., Yanguas-Gil, Angel, Martinson, Alex B. F., Elam, Jeffrey W., and Darling, Seth B. Tue . "The chemical physics of sequential infiltration synthesis—A thermodynamic and kinetic perspective". United States. doi:10.1063/1.5128108.
@article{osti_1592570,
title = {The chemical physics of sequential infiltration synthesis—A thermodynamic and kinetic perspective},
author = {Waldman, Ruben Z. and Mandia, David J. and Yanguas-Gil, Angel and Martinson, Alex B. F. and Elam, Jeffrey W. and Darling, Seth B.},
abstractNote = {Sequential infiltration synthesis (SIS) is an emerging materials growth method by which inorganic metal oxides are nucleated and grown within the free volume of polymers in association with chemical functional groups in the polymer. SIS enables the growth of novel polymer-inorganic hybrid materials, porous inorganic materials, and spatially templated nanoscale devices of relevance to a host of technological applications. Although SIS borrows from the precursors and equipment of atomic layer deposition (ALD), the chemistry and physics of SIS differ in important ways. These differences arise from the permeable three-dimensional distribution of functional groups in polymers in SIS, which contrast to the typically impermeable two-dimensional distribution of active sites on solid surfaces in ALD. In SIS, metal-organic vapor-phase precursors dissolve and diffuse into polymers and interact with these functional groups through reversible complex formation and/or irreversible chemical reactions. In this perspective, we describe the thermodynamics and kinetics of SIS and attempt to disentangle the tightly coupled physical and chemical processes that underlie this method. Here, we discuss the various experimental, computational, and theoretical efforts that provide insight into SIS mechanisms and identify approaches that may fill out current gaps in knowledge and expand the utilization of SIS.},
doi = {10.1063/1.5128108},
journal = {Journal of Chemical Physics},
number = 19,
volume = 151,
place = {United States},
year = {2019},
month = {11}
}

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Phase Stabilization of Al:HfO 2 Grown on In x Ga 1– x As Substrates ( x = 0, 0.15, 0.53) via Trimethylaluminum-Based Atomic Layer Deposition
journal, February 2014

  • Cianci, Elena; Molle, Alessandro; Lamperti, Alessio
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 5
  • DOI: 10.1021/am405617q

Real-time sensing and metrology for atomic layer deposition processes and manufacturing
journal, January 2007

  • Henn-Lecordier, Laurent; Lei, Wei; Anderle, Mariano
  • Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 25, Issue 1
  • DOI: 10.1116/1.2429672

Enhanced Block Copolymer Lithography Using Sequential Infiltration Synthesis
journal, July 2011

  • Tseng, Yu-Chih; Peng, Qing; Ocola, Leonidas E.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 36, p. 17725-17729
  • DOI: 10.1021/jp205532e

Post-directed-self-assembly membrane fabrication for in situ analysis of block copolymer structures
journal, September 2016


Characterization of polymer thin films with small‐angle X‐ray scattering under grazing incidence (GISAXS)
journal, September 2002

  • Smilgies, Detlef‐M.; Busch, Peter; Papadakis, Christine M.
  • Synchrotron Radiation News, Vol. 15, Issue 5
  • DOI: 10.1080/08940880208602975

Structural analysis of complex materials using the atomic pair distribution function — a practical guide
journal, January 2003

  • Proffen, Th.; Billinge, S. J. L.; Egami, T.
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 218, Issue 2
  • DOI: 10.1524/zkri.218.2.132.20664

Atomic pair distribution functions analysis of disordered low-Z materials
journal, January 2013

  • Petkov, V.; Ren, Y.; Kabekkodu, S.
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 22
  • DOI: 10.1039/c2cp43378h

Structural Evolution of Molybdenum Disulfide Prepared by Atomic Layer Deposition for Realization of Large Scale Films in Microelectronic Applications
journal, July 2018

  • Letourneau, Steven; Young, Matthias J.; Bedford, Nicholas M.
  • ACS Applied Nano Materials, Vol. 1, Issue 8
  • DOI: 10.1021/acsanm.8b00798

Materials discovery and design using machine learning
journal, September 2017


Surface chemistry of atomic layer deposition: A case study for the trimethylaluminum/water process
journal, June 2005

  • Puurunen, Riikka L.
  • Journal of Applied Physics, Vol. 97, Issue 12, Article No. 121301
  • DOI: 10.1063/1.1940727