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

A mixture of molecular high-spin species is frequently observed in a variet y of model systems for molecule-based magnetics. Two-Dimensional Electron S pin Transient Nutation (2D-ESTN) spectroscopy based on pulsed ESR is useful to discriminate between high-spin species in spin mixtures and identify un equivocally the spin quantum number of them. In this work, we have performe d the spectral simulation of the 2D ESTN spectrum including forbidden trans itions for EU2+ ion (S=7/2, I=5/2) in a CaF2 single crystal, which has two isotopes ((EU)-E-151 (47.9%) and Eu-153 (52.1%)), based on the transition m oment analysis including nuclear spin transitions. The simulated spectrum i s reasonably consistent with the experimental one, indicating that the tran sition moment spectroscopy-based simulation is a powerful tool for the uneq uivocal identification of the 2D-ESTN spectra from a mixture of electronic and nuclear high-spin systems.