A new semiempirical approach to study ground and excited states of metal complexes in biological systems

C. J. Margulis, V. Guallar, E. Sim, R. A. Friesner, B. J. Berne

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

In this paper we develop a "diatomic in molecules semiempirical ligand field" (DIMSELF) method to calculate ground and excited many-body potential energy surfaces for an arbitrary transition metal ion in an arbitrary complex system. This method is not restricted to a high-symmetry environment and is meant to be inexpensive and suitable for nonadiabatic excited states dynamics on-the-fly. Within the approximations employed, the method includes full CI (configuration interaction) and SO (spin-orbit) interactions, essential to the description of nonradiative transitions such as those of myoglobin in the presence of carbon monoxide. We test our method against high level ab initio calculations for a simple model system of myoglobin's heme pocket. Finally, we discuss our results and compare with previous calculations in the literature.

Original languageEnglish
Pages (from-to)8038-8046
Number of pages9
JournalJournal of Physical Chemistry B
Volume106
Issue number33
DOIs
Publication statusPublished - 2002 Aug 22

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myoglobin
Myoglobin
Coordination Complexes
Biological systems
Metal complexes
Excited states
Ground state
Potential energy surfaces
ground state
Carbon Monoxide
spin-orbit interactions
complex systems
Heme
Carbon monoxide
metals
carbon monoxide
configuration interaction
excitation
Transition metals
Metal ions

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

Margulis, C. J. ; Guallar, V. ; Sim, E. ; Friesner, R. A. ; Berne, B. J. / A new semiempirical approach to study ground and excited states of metal complexes in biological systems. In: Journal of Physical Chemistry B. 2002 ; Vol. 106, No. 33. pp. 8038-8046.
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A new semiempirical approach to study ground and excited states of metal complexes in biological systems. / Margulis, C. J.; Guallar, V.; Sim, E.; Friesner, R. A.; Berne, B. J.

In: Journal of Physical Chemistry B, Vol. 106, No. 33, 22.08.2002, p. 8038-8046.

Research output: Contribution to journalArticle

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AB - In this paper we develop a "diatomic in molecules semiempirical ligand field" (DIMSELF) method to calculate ground and excited many-body potential energy surfaces for an arbitrary transition metal ion in an arbitrary complex system. This method is not restricted to a high-symmetry environment and is meant to be inexpensive and suitable for nonadiabatic excited states dynamics on-the-fly. Within the approximations employed, the method includes full CI (configuration interaction) and SO (spin-orbit) interactions, essential to the description of nonradiative transitions such as those of myoglobin in the presence of carbon monoxide. We test our method against high level ab initio calculations for a simple model system of myoglobin's heme pocket. Finally, we discuss our results and compare with previous calculations in the literature.

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