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Title: Non-equilibrium adatom thermal state enables rapid additive nanomanufacturing

Abstract

A new state of radical thermal non-equilibrium in surface adsorbed molecules is discovered that enables rapid surface diffusion of energized adatoms with a negligible effect on the substrate surface temperature. Due to enhanced surface diffusion, growth rates can be achieved that improve the feasibility of many nanofabrication techniques. Since the adatom temperature cannot be directly measured without disturbing its thermodynamic state, the first principle hard-cube model is used to predict both the adatom effective temperature and the surface temperature in response to gaseous particle impingement in a vacuum. The validity of the approach is supported by local, spatially-resolved surface temperature measurements of the thermal response to supersonic microjet gas impingement. The ability to determine and control the adatom effective temperature, and therefore the surface diffusion rate, opens new degrees of freedom in controlling a wide range of nanofabrication processes that critically depend on surface diffusion of precursor molecules. Furthermore, this fundamental understanding has the potential to accelerate research into nanoscale fabrication and to yield the new materials with unique properties that are only accessible with nanoscale features.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1594427
Alternate Identifier(s):
OSTI ID: 1511759
Grant/Contract Number:  
SC0010729
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 21; Journal Issue: 20; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; electron beam; non-equilibrium thermodynamics; gas jet

Citation Formats

Henry, Matthew R., Kim, Songkil, and Fedorov, Andrei G. Non-equilibrium adatom thermal state enables rapid additive nanomanufacturing. United States: N. p., 2019. Web. doi:10.1039/C9CP01478K.
Henry, Matthew R., Kim, Songkil, & Fedorov, Andrei G. Non-equilibrium adatom thermal state enables rapid additive nanomanufacturing. United States. https://doi.org/10.1039/C9CP01478K
Henry, Matthew R., Kim, Songkil, and Fedorov, Andrei G. Mon . "Non-equilibrium adatom thermal state enables rapid additive nanomanufacturing". United States. https://doi.org/10.1039/C9CP01478K. https://www.osti.gov/servlets/purl/1594427.
@article{osti_1594427,
title = {Non-equilibrium adatom thermal state enables rapid additive nanomanufacturing},
author = {Henry, Matthew R. and Kim, Songkil and Fedorov, Andrei G.},
abstractNote = {A new state of radical thermal non-equilibrium in surface adsorbed molecules is discovered that enables rapid surface diffusion of energized adatoms with a negligible effect on the substrate surface temperature. Due to enhanced surface diffusion, growth rates can be achieved that improve the feasibility of many nanofabrication techniques. Since the adatom temperature cannot be directly measured without disturbing its thermodynamic state, the first principle hard-cube model is used to predict both the adatom effective temperature and the surface temperature in response to gaseous particle impingement in a vacuum. The validity of the approach is supported by local, spatially-resolved surface temperature measurements of the thermal response to supersonic microjet gas impingement. The ability to determine and control the adatom effective temperature, and therefore the surface diffusion rate, opens new degrees of freedom in controlling a wide range of nanofabrication processes that critically depend on surface diffusion of precursor molecules. Furthermore, this fundamental understanding has the potential to accelerate research into nanoscale fabrication and to yield the new materials with unique properties that are only accessible with nanoscale features.},
doi = {10.1039/C9CP01478K},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 20,
volume = 21,
place = {United States},
year = {Mon Apr 29 00:00:00 EDT 2019},
month = {Mon Apr 29 00:00:00 EDT 2019}
}

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Works referenced in this record:

Surface Diffusion Directed Growth of Anisotropic Graphene Domains on Different Copper Lattices
journal, February 2016

  • Jung, Da Hee; Kang, Cheong; Nam, Ji Eun
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep21136

What Controls Deposition Rate in Electron-Beam Chemical Vapor Deposition?
journal, August 2006


Analysis of electron beam induced deposition (EBID) of residual hydrocarbons in electron microscopy
journal, March 2007

  • Rykaczewski, Konrad; White, William B.; Fedorov, Andrei G.
  • Journal of Applied Physics, Vol. 101, Issue 5
  • DOI: 10.1063/1.2437065

From Isolated Ions to Multilayer Functional Materials Using Ion Soft Landing
journal, November 2018

  • Laskin, Julia; Johnson, Grant E.; Warneke, Jonas
  • Angewandte Chemie International Edition, Vol. 57, Issue 50
  • DOI: 10.1002/anie.201712296

Hard‐cube model analysis of gas‐surface energy accommodation
journal, January 1980

  • Grimmelmann, Erik K.; Tully, John C.; Cardillo, Mark J.
  • The Journal of Chemical Physics, Vol. 72, Issue 2
  • DOI: 10.1063/1.439271

Dynamics of molecular adsorption of ethane with platinum(111): a supersonic molecular beam study
journal, February 1991

  • Arumainayagam, Christopher R.; Schoofs, Gregory R.; McMaster, Mark C.
  • The Journal of Physical Chemistry, Vol. 95, Issue 3
  • DOI: 10.1021/j100156a005

On effective properties of materials at the nano- and microscales considering surface effects
journal, July 2015


High-Fidelity 3D-Nanoprinting via Focused Electron Beams: Computer-Aided Design (3BID)
journal, February 2018

  • Fowlkes, Jason D.; Winkler, R.; Lewis, Brett B.
  • ACS Applied Nano Materials, Vol. 1, Issue 3
  • DOI: 10.1021/acsanm.7b00342

Reference potentials for adsorption of helium, argon, methane, and krypton in high-silica zeolites
journal, August 2001

  • Talu, Orhan; Myers, Alan L.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 187-188, p. 83-93
  • DOI: 10.1016/S0927-7757(01)00628-8

Exploring Ag(111) Substrate for Epitaxially Growing Monolayer Stanene: A First-Principles Study
journal, July 2016

  • Gao, Junfeng; Zhang, Gang; Zhang, Yong-Wei
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep29107

High Purity Tungsten Nanostructures via Focused Electron Beam Induced Deposition with Carrier Gas Assisted Supersonic Jet Delivery of Organometallic Precursors
journal, May 2016

  • Henry, Matthew R.; Kim, Songkil; Fedorov, Andrei G.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 19
  • DOI: 10.1021/acs.jpcc.5b11488

Engineering atomic and molecular nanostructures at surfaces
journal, September 2005

  • Barth, Johannes V.; Costantini, Giovanni; Kern, Klaus
  • Nature, Vol. 437, Issue 7059
  • DOI: 10.1038/nature04166

TiO2 thin films formation on industrial glass through self-assembly processing
journal, August 1997


Inert gas jets for growth control in electron beam induced deposition
journal, June 2011

  • Henry, M. R.; Kim, S.; Rykaczewski, K.
  • Applied Physics Letters, Vol. 98, Issue 26
  • DOI: 10.1063/1.3605588

Velocity slip of gas mixtures in free jet expansions
journal, January 1978

  • Raghuraman, P.; Davidovits, P.
  • Physics of Fluids, Vol. 21, Issue 9
  • DOI: 10.1063/1.862412

Coordination of Iron Atoms by Tetraphenylporphyrin Monolayers and Multilayers on Ag(111) and Formation of Iron-Tetraphenylporphyrin
journal, September 2008

  • Buchner, Florian; Flechtner, Ken; Bai, Yun
  • The Journal of Physical Chemistry C, Vol. 112, Issue 39
  • DOI: 10.1021/jp8052955

Nanoscience and technology: the next revolution in the Earth sciences
journal, October 2002


Anisotropic capillary instability of silicon nanostructures under hydrogen anneal
journal, February 2012

  • Barwicz, T.; Cohen, G. M.; Reuter, K. B.
  • Applied Physics Letters, Vol. 100, Issue 9
  • DOI: 10.1063/1.3690869

Self-shadowing and surface diffusion effects in obliquely deposited thin films
journal, February 1999


Plateau–Rayleigh crystal growth of periodic shells on one-dimensional substrates
journal, March 2015

  • Day, Robert W.; Mankin, Max N.; Gao, Ruixuan
  • Nature Nanotechnology, Vol. 10, Issue 4
  • DOI: 10.1038/nnano.2015.23

Directing Matter: Toward Atomic-Scale 3D Nanofabrication
journal, May 2016


High-Fidelity 3D-Nanoprinting via Focused Electron Beams: Growth Fundamentals
journal, February 2018

  • Winkler, R.; Lewis, B. B.; Fowlkes, J. D.
  • ACS Applied Nano Materials, Vol. 1, Issue 3
  • DOI: 10.1021/acsanm.8b00158

Self-organizing layers from complex molecular anions
journal, May 2018


All-Atom Force Field for Molecular Dynamics Simulations on Organotransition Metal Solids and Liquids. Application to M(CO) n (M = Cr, Fe, Ni, Mo, Ru, or W) Compounds
journal, October 2013

  • Bernardes, Carlos E. S.; Canongia Lopes, José. N.; da Piedade, Manuel E. Minas
  • The Journal of Physical Chemistry A, Vol. 117, Issue 43
  • DOI: 10.1021/jp407739h

Surface science
journal, November 1973


High-Fidelity 3D-Nanoprinting via Focused Electron Beams: Computer-Aided Design (3BID)
text, January 2018

  • Fowlkes, J.; Winkler, R.; Lewis, B.
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.23278