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.
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.
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.
The nitrogen-vacancy (NV) center in diamond is an ideal candidate for quantum sensing because of its excellent spin coherence property as well as the possibility for optical initialization and readout. Previous studies, on the other hand, have typically been conducted at low or room temperature. The inability to fully understand the coherence properties of the NV center at high temperatures limits NV's further applications. We systematically investigate the coherence properties of NV center ensemble at temperatures ranging from 300 K to 600 K in this paper. Coherence time T2 decreases rapidly from $184\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\text{s}$ at 300 K to $30\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\text{s}$ at 600 K due to the interaction with paramagnetic impurities. At all experiment temperatures, both single-quantum and double-quantum transitions exhibit a T5 relaxation rate, which is attributed to the two-phonon Raman process. Nonetheless, the inhomogeneous dephasing time T2∗ and thermal-echo decoherence time TTE remain almost unchanged at temperature up to 600 K. A thermal-echo-based thermometer is demonstrated to have a sensitivity of 41mK/Hz at 450 K. These findings will pave the way for NV-based high-temperature sensing and provide a more comprehensive understanding of solid-state qubit decoherence.
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.
Among the possible defects that can occur in diamonds, one that draws attention is the nitrogen-vacancy (NV) center.Studied since the early 90s, in recent years, they became one of the most promising platforms for field applications of quantum technology at room temperature, especially for quantum sensing.They are sensitive to electric and magnetic fields, temperature, and strain, making these nanosensors a versatile platform for many applications.The NV center's spin state is easy to read and manipulate by optical means, and, most interestingly, it works well at room temperature, which facilitates its use.The great challenge to implement quantum protocols and quantum algorithms is the coherence time of the quantum states.The NV center stands out for having relatively high coherence times at room temperature.This dissertation presents measurements to characterize the electron spin coherence of NV centers in an ultrapure sample of diamond designed for quantum sensing applications.These measurements combine optical e magnetic resonance techniques.For that, a method was implemented using a conventional CCD camera and a clever imaging protocol, making it possible to perform various pulsed microwave experiments on the electron spin, such as Rabi oscillations and Hahn spin-echo, which were used for determining the characteristic relaxation times (T 1 and T 2 ).Results show that this system provides at least two readily accessible qubits that can be used in quantum protocols even at room temperature.