Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE
Optical manipulation of single spins in diamond
Charles Santori, Philippe Tamarat, Philipp Neumann, Jörg Wrachtrup, David A. Fattal, Raymond G. Beausoleil, J. R. Rabeau, P. Olivero, Andrew D. Greentree, Steven Prawer, Fedor Jelezko, Philip Hemmer
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.
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.
Coherent population trapping is demonstrated in single nitrogen-vacancy centers in diamond under optical excitation. For sufficient excitation power, the fluorescence intensity drops almost to the background level when the laser modulation frequency matches the 2.88 GHz splitting of the ground states. The results are well described theoretically by a four-level model, allowing the relative transition strengths to be determined for individual centers. The results show that all-optical control of single spins is possible in diamond.
Abstract The controlled and coherent manipulation of individual quantum systems is fundamental for the development of quantum information processing. The nitrogen-vacancy (NV) color center in diamond is a promising system since its photoluminescence is perfectly stable at room temperature and its electron spin can be optically read out at the individual level. We review here the experiments currently realized in our laboratory concerning the use of a single NV color center as the single photon source and the coherent magnetic manipulation of the electron spin associated with a single NV color center. Furthermore, we demonstrate a nanoscopy experiment based on the saturation absorption effect, which allows to optically pin-point a single NV color center at sub-λ resolution. This offers the possibility to independently address two or multiple magnetically coupled single NV color centers, which is a necessary step towards the realization of a diamond-based quantum computer.
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.
Coherent population trapping at zero magnetic field was observed for nitrogen-vacancy centers in diamond under optical excitation. This was measured as a reduction in photoluminescence when the detuning between two excitation lasers matched the 2.88 GHz crystal-field splitting of the color center ground states. This behavior is highly sensitive to strain, which modifies the excited states, and was unexpected following recent experiments demonstrating optical readout of single nitrogen-vacancy electron spins based on cycling transitions. These results demonstrate for the first time that three-level Lambda configurations suitable for proposed quantum information applications can be realized simultaneously for all four orientations of nitrogen-vacancy centers at zero magnetic field.
Abstract Multiple-microwave-photon transition is a nonlinear process involving the simultaneous absorption of multiple microwave photons to reach a higher energy state. This phenomenon enables microwave frequency conversion, a crucial technique for spin-wave devices, frequency synthesizers and communication devices. However, it has not been observed in nitrogen-vacancy (NV) centers in diamonds, which serve as a key quantum platform linking flying qubits, microwave photons, and solid-state spins. In this work, we first observed multiple-microwave-photon transitions in NV centers in diamonds, using optically detected magnetic resonance (ODMR) methods with a single laser and microwave beam. We demonstrate that microwave frequencies, effective g-factor, and angular momentum exhibit a 1/n scaling law, but the linewidth exhibits a 1/n^2 scaling law for n-photon transitions between the ground states. Additionally, we detect the hyperfine structure of the ground states and achieve coherent spin manipulation under multi-photon excitation. Our findings offer a novel approach for the precise manipulation of NV center spin states, advancing quantum sensing and quantum information.
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.