Electron momentum spectroscopy of metal carbonyls: a reinvestigation of the role of nuclear dynamics

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作者：Balázs Hajgató (123) hajgato@vub.ac.be Filippo Morini (1) Michael S. Deleuze (1) michael.deleuze@uhasselt.be
关键词：Electronic structure theory – Electron Momentum Spectroscopy – Orbital imaging experiments – Electron impact (e ; 2e) ionization – Distorted wave effects – Molecular dynamics – Statistical thermodynamics
刊名：Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta)
出版年：2012
出版时间：July 2012
年：2012
卷：131
期：7
页码：DOI: 10.1007/s00214-
全文大小：725.8 KB
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作者单位：1. Research Group of Theoretical Chemistry and Molecular Modeling, Hasselt University, Agoralaan Gebouw D, 3590 Diepenbeek, Belgium2. General Chemistry Division, QCMM Research Group, Alliance Ghent-Brussels, Free University of Brussels, Pleinlaan 2, 1050 Brussels, Belgium3. Algemene Chemie, Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels, Belgium
刊物类别：Chemistry and Materials Science
刊物主题：Chemistry Theoretical and Computational Chemistry Inorganic Chemistry Organic Chemistry Physical Chemistry
出版者：Springer Berlin / Heidelberg
ISSN：1432-2234

文摘

The main purpose of this work is to reinvestigate the influence of nuclear dynamics in the electronic ground state of group 6 metal hexacarbonyl compounds [W(CO)b>6b>, Cr(CO)b>6b>, Mo(CO)b>6b>] on electron momentum density profiles obtained from experimental orbital reconstructions employing Electron Momentum Spectroscopy. We call into question the view (Liu et al. in Chem Phys Lett 497:229, 2010) that thermally induced nuclear displacements associated with the first three triply degenerate 1Tb>2gb>, 1Tb>1ub>, and 1Tb>2ub> vibrational eigenmodes can be large enough at or near room temperature (298–310 K) to explain on their own the unexpectedly large electron densities inferred for the frontier orbitals of these compounds at low momenta. In this purpose, we resort to an analysis of populations over these three vibrational eigenmodes, according to a description of vibrational excitations employing Maxwell–Boltzmann statistical thermodynamics. Comparison is made with Born–Oppenheimer Molecular Dynamical (BOMD) simulations over the potential energy surface associated with the electronic ground state. The role of nuclear dynamics in the final ionized state, in the form of Jahn–Teller distortions, is also tentatively investigated.

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