Origin‐independent sum over states simulations of magnetic and electronic circular dichroism spectra via the localized orbital/local origin method
作者： Petr Štěpánek , Petr Bouř
DOI: 10.1002/JCC.23845
关键词: Magnetic moment 、 Wave function 、 Magnetic circular dichroism 、 Chemistry 、 Atomic physics 、 Density functional theory 、 Molecular geometry 、 Spectral line 、 Electronic structure 、 X-ray magnetic circular dichroism
摘要: Although electronic and magnetic circular dichroism (ECD, MCD) spectra reveal valuable details about molecular geometry structure, quantum-chemical simulations significantly facilitate their interpretation. However, the simulated results may depend on choice of coordinate origin. Previously (Stěpanek Bouř, J. Comput. Chem. 2013, 34, 1531), sum-over-states (SOS) methodology was found useful for efficient MCD computations. Approximate wave functions were "resolved" using time-dependent density functional theory, origin-dependence avoided by placing origin to center mass investigated molecule. In this study, a more elegant way is proposed, based localized orbital/local (LORG) formalism, similar approach also applied generate ECD intensities. The LORG-like yields fully origin-independent spectra. thus indicate that computationally relatively cheap SOS open new modeling properties, including those involving origin-dependent dipole moment operator.
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