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A general method for the simulation of absorption (ABS) and fluorescence band shapes, resonance-Raman (rR) spectra, and excitation profiles based on the time-dependent theory of Heller is discussed. The following improvements to Heller's theory have been made: (a) derivation of new recurrence relations for the time-dependent wave packet overlap in the case(More)
The reliable correlation of structural features and magnetic or spectroscopic properties of oligonuclear transition-metal complexes is a critical requirement both for research into innovative magnetic materials and for elucidating the structure and function of many metalloenzymes. We have developed a novel method that for the first time enables the(More)
Iron K-edge X-ray absorption pre-edge features have been calculated using a time-dependent density functional approach. The influence of functional, solvation, and relativistic effects on the calculated energies and intensities has been examined by correlation of the calculated parameters to experimental data on a series of 10 iron model complexes, which(More)
Twelve structural models for the S(2) state of the oxygen-evolving complex (OEC) of photosystem II are evaluated in terms of their magnetic properties. The set includes ten models based on the 'fused twist' core topology derived by polarized EXAFS spectra and two related models proposed in recent mechanistic investigations. Optimized geometries and spin(More)
A systematic study of 12 ferric and ferrous Kbeta X-ray emission spectra (XES) is presented. The factors contributing to the Kbeta main line and the valence to core region of the spectra are experimentally assessed and quantitatively evaluated. While the Kbeta main line spectra are dominated by spin state contributions, the valence to core region is shown(More)
In this paper, we present the implementation of efficient approximations to time-dependent density functional theory (TDDFT) within the Tamm-Dancoff approximation (TDA) for hybrid density functionals. For the calculation of the TDDFT/TDA excitation energies and analytical gradients, we combine the resolution of identity (RI-J) algorithm for the computation(More)
Peculiarities of neurostimulation organization by a multi-electrode system are considered. The system forms the spatially distributed field of current pulses that impact the nerve centers of the neck. An example is given for technical implementation of such a system in device SYMPATHOCOR and the method of its application: the dynamic correction of activity(More)
Multiple spectroscopic and computational methods were used to characterize the ground-state electronic structure of the novel {CoNO}(9) species Tp*Co(NO) (Tp* = hydro-tris(3,5-Me(2)-pyrazolyl)borate). The metric parameters about the metal center and the pre-edge region of the Co K-edge X-ray absorption spectrum were reproduced by density functional theory(More)
Hydrogenase proteins catalyze the reversible conversion of molecular hydrogen to protons and electrons. While many enzymatic states of the [NiFe] hydrogenase have been studied extensively, there are multiple catalytically relevant EPR-silent states that remain poorly characterized. Analysis of model compounds using new spectroscopic techniques can provide a(More)
In this work, an improved method for the efficient automatic simulation of optical band shapes and resonance Raman (rR) intensities within the "independent mode displaced harmonic oscillator" is described. Despite the relative simplicity of this model, it is able to account for the intensity distribution in absorption (ABS), fluorescence, and rR spectra(More)