Optical Absorption Spectra Calculated Using Linear-Scaling Density-Functional Theory

  • Laura┬áRatcliff

Part of the Springer Theses book series (Springer Theses)

Table of contents

  1. Front Matter
    Pages i-xi
  2. Laura Ratcliff
    Pages 1-3
  3. Laura Ratcliff
    Pages 5-21
  4. Laura Ratcliff
    Pages 23-44
  5. Laura Ratcliff
    Pages 45-58
  6. Laura Ratcliff
    Pages 59-79
  7. Laura Ratcliff
    Pages 81-96
  8. Laura Ratcliff
    Pages 97-114
  9. Laura Ratcliff
    Pages 115-116

About this book

Introduction

The development of linear-scaling density functional theory (LS-DFT) has made ab initio calculations on systems containing thousands of atoms possible. These systems range from nanostructures to biomolecules. These methods rely on the use of localized basis sets, which are optimised for the representation of occupied Kohn-Sham states but do not guarantee an accurate representation of the unoccupied states.  This is problematic if one wishes to combine the power of LS-DFT with that of theoretical spectroscopy, which provides a direct link between simulation and experiment.  In this work a new method is presented for optimizing localized functions to accurately represent the unoccupied states, thus allowing theoretical spectroscopy of large systems. Results are presented for optical absorption spectra calculated using the ONETEP code, but the method is equally applicable to other spectroscopies and LS formulations. Other topics covered include a study of some simple one dimensional basis sets and the presentation of two methods for band structure calculation using localized basis sets, both of which have important implications for the use of localized basis sets within LS-DFT.

Keywords

Absorption Spectra for Large Electronic Systems Band Structure Calcuation Kohn-Sham States LS-DFT Linear-scaling Density Functional Theory Localized States in DFT ONETEP Code Spectroscopy Theory and Models Theoretical Spectroscopy Toy Model for Unoccupied States

Authors and affiliations

  • Laura┬áRatcliff
    • 1
  1. 1., Laboratoire de simulation atomistiqueUMR-E CEA / UJF-Grenoble 1GrenobleFrance

Bibliographic information

  • DOI https://doi.org/10.1007/978-3-319-00339-9
  • Copyright Information Springer International Publishing Switzerland 2013
  • Publisher Name Springer, Heidelberg
  • eBook Packages Physics and Astronomy
  • Print ISBN 978-3-319-00338-2
  • Online ISBN 978-3-319-00339-9
  • Series Print ISSN 2190-5053
  • Series Online ISSN 2190-5061
  • About this book