Abstract

AbstractBy optical excitation of molecular triplet states along with selective population of their spin sublevels nuclear spin polarization can be generated up to a level far above the Boltzmann equilibrium. This effect known as Optical Nuclear Polarization (ONP) has been applied for the investigation of dynamical processes in solid state matrices in the following three ways: (i) The efficiency of the ONP process and its dependency on an external magnetic field is affected by the fluctuation of local fields which is correlated to molecular motions. (ii) By pulsed irradiation of light and radio‐frequencies one can achieve a temporal resolution of the polarization process; in this way the time evolution of the spin order of the molecular states involved in the optical excitation cycle can be mapped out. (iii) The high nuclear polarization makes time resolved NMR measurements on solid state systems feasible which cannot be studied by conventional techniques because of insufficient sensitivity, e.g. guest molecules in low concentrations or isotopes with small natural abundance. The three methods, which cover together a time range between 10−12 and 103 seconds are illustrated by experiments on various organic crystals.

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