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Title: Capillary fluctuations of surface steps: An atomistic simulation study for the model Cu(111) system

Abstract

Molecular dynamics (MD) simulations are employed to investigate the capillary fluctuations of steps on the surface of a model metal system. The fluctuation spectrum, characterized by the wave number ($k$) dependence of the mean squared capillary-wave amplitudes and associated relaxation times, is calculated for $$\langle 110 \rangle$$ and $$\langle 112 \rangle$$ steps on the { 111 } surface of elemental copper near the melting temperature of the classical potential model considered. Step stiffnesses are derived from the MD results, yielding values from the largest system sizes of ( 37 ± 1 ) meV / Å for the different line orientations, implying that the stiffness is isotropic within the statistical precision of the calculations. The fluctuation lifetimes are found to vary by approximately four orders of magnitude over the range of wave numbers investigated, displaying a $k$ dependence consistent with kinetics governed by step-edge mediated diffusion. The values for step stiffness derived from these simulations are compared to step free energies for the same system and temperature obtained in a recent MD-based thermodynamic-integration (TI) study [Freitas, Frolov, and Asta, Phys. Rev. B 95, 155444 (2017)]. Results from the capillary-fluctuation analysis and TI calculations yield statistically significant differences that are discussed within the framework of statistical-mechanical theories for configurational contributions to step free energies.

Authors:
 [1];  [2];  [3]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1524294
Alternate Identifier(s):
OSTI ID: 1400431
Report Number(s):
[LLNL-JRNL-732906]
[Journal ID: ISSN 2470-0045; PLEEE8; 884390]
Grant/Contract Number:  
[AC52-07NA27344]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review E
Additional Journal Information:
[ Journal Volume: 96; Journal Issue: 4]; Journal ID: ISSN 2470-0045
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Freitas, Rodrigo, Frolov, Timofey, and Asta, Mark. Capillary fluctuations of surface steps: An atomistic simulation study for the model Cu(111) system. United States: N. p., 2017. Web. doi:10.1103/PhysRevE.96.043308.
Freitas, Rodrigo, Frolov, Timofey, & Asta, Mark. Capillary fluctuations of surface steps: An atomistic simulation study for the model Cu(111) system. United States. doi:10.1103/PhysRevE.96.043308.
Freitas, Rodrigo, Frolov, Timofey, and Asta, Mark. Fri . "Capillary fluctuations of surface steps: An atomistic simulation study for the model Cu(111) system". United States. doi:10.1103/PhysRevE.96.043308. https://www.osti.gov/servlets/purl/1524294.
@article{osti_1524294,
title = {Capillary fluctuations of surface steps: An atomistic simulation study for the model Cu(111) system},
author = {Freitas, Rodrigo and Frolov, Timofey and Asta, Mark},
abstractNote = {Molecular dynamics (MD) simulations are employed to investigate the capillary fluctuations of steps on the surface of a model metal system. The fluctuation spectrum, characterized by the wave number ($k$) dependence of the mean squared capillary-wave amplitudes and associated relaxation times, is calculated for $\langle 110 \rangle$ and $\langle 112 \rangle$ steps on the { 111 } surface of elemental copper near the melting temperature of the classical potential model considered. Step stiffnesses are derived from the MD results, yielding values from the largest system sizes of ( 37 ± 1 ) meV / Å for the different line orientations, implying that the stiffness is isotropic within the statistical precision of the calculations. The fluctuation lifetimes are found to vary by approximately four orders of magnitude over the range of wave numbers investigated, displaying a $k$ dependence consistent with kinetics governed by step-edge mediated diffusion. The values for step stiffness derived from these simulations are compared to step free energies for the same system and temperature obtained in a recent MD-based thermodynamic-integration (TI) study [Freitas, Frolov, and Asta, Phys. Rev. B 95, 155444 (2017)]. Results from the capillary-fluctuation analysis and TI calculations yield statistically significant differences that are discussed within the framework of statistical-mechanical theories for configurational contributions to step free energies.},
doi = {10.1103/PhysRevE.96.043308},
journal = {Physical Review E},
number = [4],
volume = [96],
place = {United States},
year = {2017},
month = {10}
}

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