We examine the quantum spin state of a single nitrogen-vacancy (NV) center in diamond at room temperature as it makes a transition from the orbital ground state (GS) to the orbital excited state (ES) during nonresonant optical excitation. While the fluorescence readout of NV-center spins relies on conservation of the longitudinal spin projection during optical excitation, the question of quantum phase preservation has not been examined. Using Ramsey measurements and quantum process tomography of the optical excitation process, we measure a trace fidelity of F=0.87±0.03, which includes ES spin dephasing during measurement. Extrapolation to the moment of optical excitation yields F≈0.95. This result provides insight into the interaction between spin coherence and nonresonant optical absorption through a vibronic sideband.
We examine the quantum spin state of a single nitrogen-vacancy (NV) center in diamond at room temperature as it makes a transition from the orbital ground state (GS) to the orbital excited state (ES) during nonresonant optical excitation. While the fluorescence readout of NV-center spins relies on conservation of the longitudinal spin projection during optical excitation, the question of quantum phase preservation has not been examined. Using Ramsey measurements and quantum process tomography of the optical excitation process, we measure a trace fidelity of F=0.87±0.03, which includes ES spin dephasing during measurement. Extrapolation to the moment of optical excitation yields F≈0.95. This result provides insight into the interaction between spin coherence and nonresonant optical absorption through a vibronic sideband.
We study the spin and orbital dynamics of single nitrogen vacancy (NV) centers in diamond between room temperature and 700 K. We find that the ability to optically address and coherently control single spins above room temperature is limited by nonradiative processes that quench the NV center’s fluorescence-based spin readout between 550 K and 700 K. Combined with electronic structure calculations, our measurements indicate that the energy difference between the E and A1 electronic states is ∼0.8 eV. We also find that the inhomogeneous spin lifetime (T ∗ 2 ) is independent of temperature up to at least 625 K, suggesting that single NV centers could be applied as nanoscale thermometers over a broad temperature range.
The nitrogen-vacancy (NV) center in diamond has garnered great interest over the past decade as its electronic spin shows promise as a quantum bit (qubit) and nanoscale sensor. Consisting of a substitutional nitrogen adjacent to a vacant site within the carbon lattice of diamond, this defect exhibits millisecond-long spin coherence times extending beyond room temperature, spin-dependent optical addressability, coupling to intrinsic and nearby nuclear spins, and it can be controlled and manipulated through electrical, magnetic, and optical means. In particular, at cryogenic temperatures (T < 25 K), the NV center's excited state becomes sharp and optically resolvable, providing a solid-state quantum optical testbed. In this thesis, I describe several experiments that explore this quantum optical interface to facilitate the development of a photonic network of single spins linked and controlled by light. We begin by exploring how electric fields tune the orbital levels within the NV center through the DC Stark effect, finding a surprising photo-induced field that aids in the ability to tune multiple NV centers' optical transitions to degeneracy. We then develop techniques to fully control the spin state of the NV center by coupling through a lambda system, an energy configuration consisting of two lower levels coupled to one of higher energy. When a lambda system is optically driven, the spin becomes trapped in a dark state, or the eigenstate of the system that is not coupled to the light fields through destructive interference, forming the basis for the various types of control demonstrated. We demonstrate arbitrary-basis initialization and readout of the spin state through coherent population trapping, as well as the ability to rotate about any arbitrary basis through stimulated Raman transitions. Combining these techniques, we measure the NV center's spin coherence through a completely optical measurement. We then extend these lambda system techniques to adiabatically move the dark state in trajectories around the Bloch sphere. Such trajectories accumulate a quantum mechanical phase that depends only on the geometry of the path enclosed, not on the energetics or time of the interaction. We characterize the interaction, measure this phase, known as Berry phase, and explore the limits of its control and resilience to noise. Finally, we demonstrate another all-optical control technique that uses strong ultrafast pulses of light to transfer the spin between the ground and excited states, deriving spin manipulation from the excited state dynamics. This technique also provides time-resolved spectroscopy of the excited state and its various decay and decoherence mechanisms. These experiments advance the progress toward the development of photonic networks coupling and controlling defects through light-matter interactions.
The nitrogen-vacancy (NV) center in diamond has emerged as a versatile atom-like system, finding diverse applications at both ambient and cryogenic temperatures. At room temperature, the NV center's spin-triplet electronic ground state has a long coherence time and can be read out and initialized using nonresonant optical excitation, which has enabled a wide range of metrology and quantum information applications. At cryogenic temperatures, the NV center exhibits a variety of narrow, atom-like optical transitions, which has made the NV center a promising platform for quantum optics applications. We use coherent optical manipulation of the NV center at cryogenic temperatures to probe its internal dynamics and aspects of its interactions with its environment.\nFirst, we investigate the intersystem crossing (ISC) process, which is a spin-dependent nonradiative decay mechanism that enables the electronic spin state to be optically initialized and read out at room temperature. We measure the ISC rates from different excited states as well as the rate at which interactions with phonons redistribute population between these states. Based on these measurements, we develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure.\nSecond, we investigate a novel method of using coherent optical manipulation of the NV center's electronic spin to control a nearby nuclear spin. Coherent interactions between the NV center and nearby nuclear spins have enabled the development of NV center-based, multi-qubit quantum registers, but these techniques have generally required the application of microwave or radio-frequency radiation. We demonstrate control of the nuclear spin using an all-optical Raman technique and theoretically evaluate the extent to which the intrinsic physics of the NV center limits the coherence of this Raman-based manipulation technique.
The negative Nitrogen-Vacancy (NV) colour centre in diamond is an atomic-level impurity that is remarkably well suited for quantum information processing and quantum metrology applications. Underlying these properties is the fact that optical illumination causes the NV centre to preferentially populate one of its three spin levels. The mechanism that gives rise to this spin polarisation has not been well understood, despite intense research interest in the NV centre and its applications. This thesis arrives at an account of the spin polarisation mechanism, although a detailed theoretical treatment remains outstanding. The energy level structure of the NV centre is investigated using techniques of solid state spectroscopy. These include absorption and photoluminescence measurements made on diamonds at cryogenic and room temperatures in the presence of uniaxial stress, magnetic fields, and microwaves. Pulsed light experiments allow the dynamic processes within the NV centre to be measured. It is shown that at room temperature the orbital doublet excited state behaves like an orbital singlet, and this description is elegantly confirmed by single-site observations. This picture of the excited state is inconsistent with cryogenic measurements, and its behaviour is examined across a range of temperatures in order to resolve this tension. It is shown that electron-vibration interaction accounts for the quenching of orbital properties in the excited state with temperature. A new optical transition within the NV centre is reported at a wavelength of 1042 nm. It is established that this transition occurs between the intermediate singlet levels which are thought to provide the decay pathway that produces spin polarisation. The results are consistent with this understanding, and the order and properties of these singlet levels are established. Electron-vibration interaction is observed to be important within the singlet system. It is shown that electron-vibration interaction is an important detail in the NV optical pumping cycle. Taking it into consideration leads to the first plausible physical description of the spin polarisation mechanism. -- provided by Candidate.
Nitrogen-vacancy centers in diamond typically have spin-conserving optical transitions, a feature which allows for optical detection of the long-lived electronic spin states through fluorescence detection. However, by applying stress to a sample it is possible to obtain spin-nonconserving transitions in which a single excited state couples to multiple ground states. Here we describe two-frequency optical spectroscopy on single nitrogen-vacancy centers in a high-purity diamond sample at low temperature. When stress is applied to the sample it is possible to observe coherent population trapping with a single center. By adjusting the stress it is possible to obtain a situation in which all of the transitions from the three ground sublevels to a common excited state are strongly allowed. These results show that all-optical spin manipulation is possible for this system, and we propose that that by coupling single centers to optical microcavities, a scalable quantum network could be realized for photonic quantum information processing.
One of the biggest challenges to implement quantum protocols and quantum information processing (QIP) is achieving long coherence times, usually requiring systems at ultra-low temperatures. The nitrogen-vacancy (NV) center in diamond is a promising alternative to this problem. Due to its spin properties, easy manipulation, and the possibility of doing optical state initialization and readout, it quickly became one of the best solid-state spin systems for QIP at room temperature. Here, we present the characterization of the spin-coherence of an ensemble of NV centers in an engineered sample of ultrapure diamond as a testbed for quantum protocols for quantum metrology.