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

C. J. Margulis, V. Guallar, Eun Ji 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

Fingerprint

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

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

Cite this

Margulis, C. J. ; Guallar, V. ; Sim, Eun Ji ; 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, Eun Ji; 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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