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Dynamic nuclear polarization (DNP) is an out-of-equilibrium method forgenerating non-thermal spin polarization which provides large signalenhancements in modern diagnostic methods based on nuclear magnetic resonance.A particular instance is cross effect DNP, which involves the interaction oftwo coupled electrons with the nuclear spin ensemble. Here we develop a theoryfor this important DNP mechanism and show that the non-equilibrium nuclearpolarization build-up is effectively driven by three-body incoherent Markoviandissipative processes involving simultaneous state changes of two electrons andone nucleus. Our theoretical approach allows for the first time simulations ofthe polarization dynamics on an individual spin level for ensembles consistingof hundreds of nuclear spins. The insight obtained by these simulations can beused to find optimal experimental conditions for cross effect DNP and to designtailored radical systems that provide optimal DNP efficiency.

Many-body kinetics of dynamic nuclear polarization by the cross effect