Ab initio methodology for the calculation of molecular spectroscopic properties

Spectroscopic techniques provide the most accurate and complete information about the physical properties of molecules. The goal of this project is to propose an ab initio methodology for the calculation and analysis of spectroscopic properties of arbitrary molecules. The first part of the project is devoted to electron-vibrational spectroscopies including (1) optical absorption and emission, (2) photoelectron spectroscopy, PES and XPES, (3) Raman spectroscopy and (4) magnetic circular dichroism spectroscopy, MCD and XMCD. The spectra will be simulated by combining ab initio calculations of electronic states and vibrational eigenmodes and electron-vibrational coupling constants. The second part is devoted to magnetic resonance spectroscopy including (1) electron paramagnetic resonance, (2) nuclear magnetic resonance and nuclear quadrupole resonance, (3) Mössbauer spectroscopy and (4) inelastic neutron scattering. In contrast with numerous calculations of these spectroscopic properties based on DFT approaches, in the present project they will be calculated by explicitly correlated ab initio methods including spin-orbit couplings in a non-perturbative way, which will increase qualitatively the accuracy of their predictions. The project arises as a response to the rising demands for detailed analysis of complex spectroscopic data in modern molecular materials of relevance to the fields of spintronics and molecular spinbased quantum computing applications.