Anisotropic and Coherent Control of Radical Pairs by Optimized RF Fields.

Radical pair kinetics is determined by the coherent and incoherent spin dynamics of spin pair and spin-selective chemical reactions. In a previous paper, reaction control and nuclear spin state selection by designed radiofrequency (RF) magnetic resonance was proposed. Here, we present two novel types of reaction control calculated by the local optimization method. One is anisotropic reaction control and the other is coherent path control. In both cases, the weighting parameters for the target states play an important role in the optimizing of the RF field. In the anisotropic control of radical pairs, the weighting parameters play an important role in the selection of the sub-ensemble. In coherent control, one can set the parameters for the intermediate states, and it is possible to specify the path to reach a final state by adjusting the weighting parameters. The global optimization of the weighting parameters for coherent control has been studied. These manifest calculations show the possibility of controlling the chemical reactions of radical pair intermediates in different ways.

Quantum control of radical pair reactions by local optimization theory.

Recently, AWG (arbitrary waveform generator) based pulse electron paramagnetic resonance and nuclear magnetic resonance have been developed in a high field regime for the improvement of sensitivity and selectivity and quantum information processing. Here, we propose the application of AWG based reaction control of radical pairs in a rather low magnetic field regime. We calculated the locally optimized radio frequency (RF) field with the control theory by Sugawara [J. Chem. Phys. 118(15), 6784-6800 (2003)]. The calculation results manifest the applicability of AWG-RF fields to reaction control (reaction yield detected magnetic resonance), stimulated nuclear polarization, magnetic isotope selection, and coherent control of the spin dynamics.