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arXiv:1211.2749

Dressed-State Polarization Transfer between Bright & Dark Spins in Diamond

Chinmay Belthangady, Nir Bar‐Gill, Linh Pham, Keigo Arai, David Le Sage, Paola Cappellaro, R. L. Walsworth

Published Nov 12, 2012• 0 citations
arXivHTMLPDF

Abstract

Under ambient conditions, spin impurities in solid-state systems are found in thermally-mixed states and are optically "dark", i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright", i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a dressed-state, double-resonance scheme to transfer polarization from bright NV electronic spins to dark substitutional-Nitrogen (P1) electronic spins in diamond. This polarization-transfer mechanism could be used to cool a mesoscopic bath of dark spins to near-zero temperature, thus providing a resource for quantum information and sensing, and aiding studies of quantum effects in many-body spin systems.

DOI
10.48550/arxiv.1211.2749

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Under ambient conditions, spin impurities in solid-state systems are found in thermally-mixed states and are optically "dark", i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright", i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a dressed-state, double-resonance scheme to transfer polarization from bright NV electronic spins to dark substitutional-Nitrogen (P1) electronic spins in diamond. This polarization-transfer mechanism could be used to cool a mesoscopic bath of dark spins to near-zero temperature, thus providing a resource for quantum information and sensing, and aiding studies of quantum effects in many-body spin systems.
Under ambient conditions, spin impurities in solid-state systems are found in thermally mixed states and are optically "dark"; i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright"; i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a scheme to resonantly couple bright NV electronic spins to dark substitutional-nitrogen (P1) electronic spins by dressing their spin states with oscillating magnetic fields. This resonant coupling mechanism can be used to transfer spin polarization from NV spins to nearby dark spins and could be used to cool a mesoscopic bath of dark spins to near-zero temperature, thus providing a resource for quantum information and sensing, and aiding studies of quantum effects in many-body spin systems.
The ready optical detection and manipulation of bright nitrogen vacancy center spins in diamond plays a key role in contemporary quantum information science and quantum metrology. Other optically dark defects such as substitutional nitrogen atoms (`P1 centers') could also become potentially useful in this context if they could be as easily optically detected and manipulated. We develop a relatively straightforward continuous wave protocol that takes advantage of the dipolar coupling between nitrogen vacancy and P1 centers in type 1b diamond to detect and polarize the dark P1 spins. By combining mutual spin flip transitions with radio frequency driving, we demonstrate the simultaneous optical polarization and detection of the electron spin resonance of the P1 center. This technique should be applicable to detecting and manipulating a broad range of dark spin populations that couple to the nitrogen vacancy center via dipolar fields, allowing for quantum metrology using these spin populations.
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.
We report polarization of a dense nuclear-spin ensemble in diamond at room temperature. The method is based on the transfer of electron spin polarization of negatively charged nitrogen vacancy (NV) color centers to the nuclear spins via the excited-state level anti-crossing (ESLAC) of the center. We demonstrate polarization of 80% of the 14 N nuclear spins related to the NV centers, as well as that of 50% of the proximal 13 C nuclear spins. This work may enable polarization of the 13 C in bulk diamond, which is of interest to applications of nuclear magnetic resonance, quantum memories in hybrid quantum devices, and in sensing.
By choosing the right system and using the right techniques, it is possible to achieve reliable control of an individual quantum system in a solid. Certain atom-like solid-state systems are especially suited for this goal. The electron spin of the diamond nitrogen-vacancy (NV) impurity center is a leader among such systems and has featured in a great deal of recent experimental work in the context of various quantum technologies. By extending optical control for the NV center we increase the utility of this system, opening it up to fresh applications in quantum optics. \n \nDoing quantum control with a solid-state spin comes with its own challenges. In particular it can be difficult to simultaneously isolate single systems, both for control and from environment-induced decoherence, while also coupling multiple systems together in a controlled way. A goal of the work presented in this dissertation is to develop techniques for answering this problem in the NV center. \n \nOptical control, as opposed to the microwave control usually used for state manipulation in the NV center, would make it easier to address only one spin system at a time. We demonstrate such control using two methods, two-photon optically driven Rabi oscillations and stimulated Raman adiabatic passage. These both have the added advantage that by using Raman-resonant, dipole-detuned optical fields, they protect the spin state from the decoherence normally associated with the optical transitions. Furthermore, we see that this electron spin control is nuclear spin dependent, providing a mechanism for coupling these two spin systems. \n \nWe also investigate a decoherence reduction technique that involves coupling continuous microwave fields to the spin states. The resulting "dressed states" are shielded from spin-bath-induced magnetic field fluctuations. We confirm this using optical coherent population trapping measurements which we have also developed in the NV center. We show that these measurements are sensitive to nuclear spin states as well as to dressed states. \n \nThese results supply the missing piece, optical spin manipulation, to control schemes that are all-optical, and they demonstrate ways to significantly push back the decoherence limit. \n \nThis dissertation includes previously published and unpublished co-authored material.
Harnessing dipolar spin environments as controllable quantum resources is a central challenge in solid-state quantum technologies. Here, we report the observation of a coherent mesoscopic spin state in a disordered ensemble of substitutional nitrogen (P1) centers in diamond. An iterative Hartmann-Hahn protocol transfers polarization from dense nitrogen-vacancy (NV) centers to a P1 ensemble, yielding a 740-fold enhancement over room-temperature thermal equilibrium as revealed by differential readout. The resulting mesoscopic P1 spin ensemble exhibits collective Rabi oscillations and long-lived spin-lock and Hahn-echo coherences. We identify a crossover in the saturation polarization arising from the competition between coherent driving and local disorder, providing a quantitative measure of the system's intrinsic disorder. These results establish a foundation for utilizing dark electron spin ensembles as robust resources for quantum sensing and quantum many-body simulation.