Transition moment spectroscopy-based simulation of 2D electron spin transient nutation spectra for high spin chemistry

Abstract

A mixture of molecular high-spin species is frequently observed in a variety of model systems for molecule-based magnetics. Two-Dimensional Electron Spin Transient Nutation (2D-ESTN) spectroscopy based on pulsed ESR is useful to discriminate between high-spin species in spin mixtures and identify unequivocally the spin quantum number of them. In this work, we have performed the spectral simulation of the 2D ESTN spectrum including forbidden transitions for Eu 2+ ion (S=7/2, I=5/2) in a CaF 2 single crystal, which has two isotopes ( 151 Eu (47.9%) and 153 Eu (52.1%)), based on the transition moment analysis including nuclear spin transitions. The simulated spectrum is reasonably consistent with the experimental one, indicating that the transition moment spectroscopy-based simulation is a powerful tool for the unequivocal identification of the 2D-ESTN spectra from a mixture of electronic and nuclear high-spin systems.