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Abstract

Nitrogen-vacancy (NV) centers in diamond are excellent model quantum systems, due to a combination of long coherence times, high-fidelity control, and inherent stability. Their atomic scale, solid-state environment, and intrinsic spin-photon interface make them well-suited for a range of quantum communication and quantum sensing applications. The success of these applications depends on developing an array of techniques to initialize, manipulate, and measure the NV center’s quantum state through optical control fields. To that end, this dissertation demonstrates a set of novel techniques for NV center qubit control and sensing which leverage optical interactions. The first class of protocols executes fast, high-fidelity ground state spin operations using an intermediate excited state. By shaping optical control pulses on nanosecond timescales, accelerated adiabatic state transfers and nonadiabatic holonomic single-qubit gates are performed. These techniques are designed to combine error resistance with short duration in pursuit of fault-tolerant qubit operations. In addition, optical control is integrated with established ac magnetometry protocols to enable detection of photocurrents in monolayer molybdenum disulfide. Synchronizing pulsed photoexcitation with spin-echo-based sensing sequences for a near-surface ensemble of NV centers creates a sensitive, local detector of photocurrent density. This capability is used to spatially and temporally map a micron-scale photocurrent vortex. These demonstrations expand the range of optical control methods for single NV centers and provide new methods for probing current distributions in 2D materials and thin films.

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