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Title: First-principles study of the binding energy between nanostructures and its scaling with system size

Abstract

The equilibrium van der Waals binding energy is an important factor in the design of materials and devices. However, it presents great computational challenges for materials built up from nanostructures. Here we investigate the binding-energy scaling behavior from first-principles calculations. We show that the equilibrium binding energy per atom between identical nanostructures can scale up or down with nanostructure size, but can be parametrized for large $$\mathscr{N}$$ with an analytical formula (in meV/atom), $$E_b\mathscr{N} = a + b/\mathscr{N} + c/\mathscr{N}^2 + d/\mathscr{N}^3$$ where $$\mathscr{N}$$ is the number of atoms in a nanostructure and $a, b, c$ and $d$ are fitting parameters, depending on the properties of a nanostructure. The formula is consistent with a finite large-size limit of binding energy per atom. We find that there are two competing factors in the determination of the binding energy: Nonadditivities of van der Waals coefficients and center-to-center distance between nanostructures. To decode the detail, the nonadditivity of the static multipole polarizability is investigated from an accurate spherical-shell model. Finally, we find that the higher-order multipole polarizability displays ultrastrong intrinsic nonadditivity, no matter if the dipole polarizability is additive or not.

Authors:
 [1];  [2];  [1];  [3];  [4];  [2];  [1]
  1. Temple Univ., Philadelphia, PA (United States)
  2. Chalmers Univ. of Technology (Sweden)
  3. China Academy of Engineering Phyiscs, Chengdu (China)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE
OSTI Identifier:
1544288
Grant/Contract Number:  
SC0018194
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 15; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Tao, Jianmin, Jiao, Yang, Mo, Yuxiang, Yang, Zeng-Hui, Zhu, Jian-Xin, Hyldgaard, Per, and Perdew, John P. First-principles study of the binding energy between nanostructures and its scaling with system size. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.155143.
Tao, Jianmin, Jiao, Yang, Mo, Yuxiang, Yang, Zeng-Hui, Zhu, Jian-Xin, Hyldgaard, Per, & Perdew, John P. First-principles study of the binding energy between nanostructures and its scaling with system size. United States. doi:10.1103/PhysRevB.97.155143.
Tao, Jianmin, Jiao, Yang, Mo, Yuxiang, Yang, Zeng-Hui, Zhu, Jian-Xin, Hyldgaard, Per, and Perdew, John P. Thu . "First-principles study of the binding energy between nanostructures and its scaling with system size". United States. doi:10.1103/PhysRevB.97.155143. https://www.osti.gov/servlets/purl/1544288.
@article{osti_1544288,
title = {First-principles study of the binding energy between nanostructures and its scaling with system size},
author = {Tao, Jianmin and Jiao, Yang and Mo, Yuxiang and Yang, Zeng-Hui and Zhu, Jian-Xin and Hyldgaard, Per and Perdew, John P.},
abstractNote = {The equilibrium van der Waals binding energy is an important factor in the design of materials and devices. However, it presents great computational challenges for materials built up from nanostructures. Here we investigate the binding-energy scaling behavior from first-principles calculations. We show that the equilibrium binding energy per atom between identical nanostructures can scale up or down with nanostructure size, but can be parametrized for large $\mathscr{N}$ with an analytical formula (in meV/atom), $E_b\mathscr{N} = a + b/\mathscr{N} + c/\mathscr{N}^2 + d/\mathscr{N}^3$ where $\mathscr{N}$ is the number of atoms in a nanostructure and $a, b, c$ and $d$ are fitting parameters, depending on the properties of a nanostructure. The formula is consistent with a finite large-size limit of binding energy per atom. We find that there are two competing factors in the determination of the binding energy: Nonadditivities of van der Waals coefficients and center-to-center distance between nanostructures. To decode the detail, the nonadditivity of the static multipole polarizability is investigated from an accurate spherical-shell model. Finally, we find that the higher-order multipole polarizability displays ultrastrong intrinsic nonadditivity, no matter if the dipole polarizability is additive or not.},
doi = {10.1103/PhysRevB.97.155143},
journal = {Physical Review B},
issn = {2469-9950},
number = 15,
volume = 97,
place = {United States},
year = {2018},
month = {4}
}

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