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Coherent control of quantum systems has far-reaching implications in quantumengineering. In this context, coherent population trapping (CPT) involving darkresonances has played a prominent role, leading to a wealth of majorapplications including laser cooling of atoms and molecules, opticalmagnetometry, light storage and highly precise atomic clocks. Extending CPTmethods to individual solid-state quantum systems has been only achieved incryogenic environments for electron spin impurities and superconductingcircuits. Here, we demonstrate efficient CPT of a single nuclear spin in a roomtemperature solid. To this end, we make use of a three-level system with a$\Lambda$-configuration in the microwave domain, which consists of nuclear spinstates addressed through their hyperfine coupling to the electron spin of asingle nitrogen-vacancy defect in diamond. Dark state pumping requires arelaxation mechanism which, in atomic systems, is simply provided byspontaneous emission. In this work, the relaxation process is externallycontrolled through incoherent optical pumping and separated in time fromconsecutive coherent microwave excitations of the nuclear spin$\Lambda$-system. Such a pumping scheme with controlled relaxation allows us(i) to monitor the sequential accumulation of population into the dark stateand (ii) to reach a new regime of CPT dynamics for which periodic arrays ofdark resonances can be observed, owing to multiple constructive interferences.This work offers new prospects for quantum state preparation, informationstorage in hybrid quantum systems and metrology.

Coherent population trapping of a single nuclear spin under ambient conditions