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Journal of Chemical Physics / Volume 129 / Issue 6 / ARTICLES / Theoretical Methods and Algorithms

J. Chem. Phys. 129, 064102 (2008); http://dx.doi.org/10.1063/1.2958255 (9 pages)

A gradient-directed Monte Carlo approach to molecular design

Xiangqian Hu, David N. Beratan, and Weitao Yang

Department of Chemistry, Duke University, Durham, North Carolina 27708-0354, USA

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(Received 28 April 2008; accepted 24 June 2008; published online 8 August 2008)

The recently developed linear combination of atomic potentials (LCAP) approach [ M. Wang et al., J. Am. Chem. Soc. 128, 3228 (2006) ] allows continuous optimization in a discrete chemical space, and thus is useful in the design of molecules for targeted properties. To address further challenges arising from the rugged, continuous property surfaces in the LCAP approach, we develop a gradient-directed Monte Carlo (GDMC) strategy as an augmentation to the original LCAP optimization method. The GDMC method retains the power of exploring molecular space by utilizing local gradient information computed from the LCAP approach to jump between discrete molecular structures. It also allows random MC moves to overcome barriers between local optima on property surfaces. The combined GDMC–LCAP approach is demonstrated here for optimizing nonlinear optical properties in a class of donor-acceptor substituted benzene and porphyrin frameworks. Specifically, one molecule with four nitrogen atoms in the porphyrin ring was found to have a larger first hyperpolarizability than structures with the conventional porphyrin motif.

© 2008 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. THE LCAP APPROACH FOR THE FIRST HYPERPOLARIZABILITY
  3. THE GENERAL GDMC APPROACH
  4. COMBINING GDMC AND LCAP
  5. GDMC-LCAP OPTIMIZATION OF THE FIRST HYPERPOLARIZABILITY
    1. Case I
    2. Case II
    3. Case III
  6. CONCLUSIONS

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KEYWORDS and PACS

Keywords

molecular configurations, Monte Carlo methods, nonlinear optical susceptibility, optimisation, organic compounds, polarisability

PACS

  • 33.15.Kr

    Electric and magnetic moments (and derivatives), polarizability, and magnetic susceptibility

  • 33.15.Bh

    General molecular conformation and symmetry; stereochemistry

  • 02.70.Uu

    Applications of Monte Carlo methods

  • 02.60.Pn

    Numerical optimization

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.2958255

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
    O. A. von Lilienfeld, R. D. Lins, and U. Rothlisberger, Phys. Rev. Lett. 95, 153002 (2005).

    D. Xiao, W. Yang, and D. N. Beratan, J. Chem. Phys.129, 044106 (2008)JCPSA6000129000004044106000001.

    P. J. Reynolds, D. M. Ceperley, B. J. Alder, and W. A. Lester, Jr., J. Chem. Phys. 77, 5593 (1982)JCPSA6000077000011005593000001.

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    A. F. Garito, K. D. Singer, and C. C. Teng, Appl. Phys. Lett. 39, 1 (1981)APPLAB000039000001000001000001.

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