A Multireference Density Functional Approach to the Calculation of the Excited States of Uranium Ions

Abstract

An accurate and efficient hybrid Density Functional Theory (DFT)/Multireference Configuration Interaction (MRCI) model for computing electronic excitation energies in heavy element atoms and molecules was developed. This model incorporated relativistic effects essential for accurate qualitative and quantitative spectroscopic predictions on heavy elements, while simultaneously removing spin-multiplicity limitations inherent in the original model on which it is based. This model was used to successfully compute ground and low-lying electronic states for atoms in the first two rows of the period table, which were used for calibration. Once calibrated, calculations on carbon monoxide, bromine fluoride, the bromine atom, uranium +4 and +5 ions and the uranyl (UO2 2+) ion showed the model achieved reductions in relative error with respect to Time Dependent Density Functional Theory (TDDFT) of 11-42%, with a corresponding reduction in computational effort in terms of MRCI expansion sizes of a factor of 25-64.

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Document Details

Document Type
Technical Report
Publication Date
Mar 01, 2007
Accession Number
ADA466101

Entities

People

  • Eric V. Beck

Organizations

  • Air Force Institute of Technology

Tags

Communities of Interest

  • Energy and Power Technologies

DTIC Thesaurus Topics

  • Air Force
  • Chemical Compounds
  • Chemistry
  • Computational Chemistry
  • Computational Chemistry Methods
  • Computational Science
  • Density Functional Theory
  • Dielectric Gases
  • Electronic Structure Theory
  • First Principles Calculations
  • Molecular Physics
  • Physical Chemistry
  • Quantum Chemistry
  • Quantum Mechanics
  • Quantum Numbers
  • Spectra
  • Spectroscopy

Fields of Study

  • Physics

Readers

  • Combustion science or combustion engineering.
  • Computational Modeling and Simulation
  • Quantum Chemistry

Technology Areas

  • Microelectronics