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Precise knowledge of a quantum system's Hamiltonian is a criticalpre-requisite for its use in many quantum information technologies. Here, wereport a method for the precise characterization of the non-secular part of theexcited-state Hamiltonian of an electronic-nuclear spin system in diamond. Themethod relies on the investigation of the dynamic nuclear polarization mediatedby the electronic spin, which is currently exploited as a primary tool forinitializing nuclear qubits and performing enhanced nuclear magnetic resonance.By measuring the temporal evolution of the population of the ground-statehyperfine levels of a nitrogen-vacancy center, we obtain the first directestimation of the excited-state transverse hyperfine coupling between itselectronic and nitrogen nuclear spin. Our method could also be applied to otherelectron-nuclear spin systems, such as those related to defects in siliconcarbide.

Measurement of the excited-state transverse hyperfine coupling in NV centers via dynamic nuclear polarization