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Physical Review Letters

Optically Driven Rabi Oscillations and Adiabatic Passage of Single Electron Spins in Diamond

D. Andrew Golter, Hailin Wang

Published Mar 18, 2014• 88 citations
Publisher

Abstract

Rabi oscillations and adiabatic passage of single electron spins in a diamond nitrogen vacancy center are demonstrated with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. We show that the optical spin control is nuclear-spin selective and can be robust against rapid decoherence, including radiative decay and spectral diffusion, of the underlying optical transitions. A direct comparison between the Rabi oscillation and the adiabatic passage, along with a detailed theoretical analysis, provides significant physical insights into the connections and differences between these coherent spin processes and also elucidates the role of spectral diffusion in these processes. The optically driven coherent spin processes enable the use of nitrogen vacancy excited states to mediate coherent spin-phonon coupling, opening the door to combining optical control of both spin and mechanical degrees of freedom.

DOI
10.1103/physrevlett.112.116403

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Optically-driven nuclear-spin-selective Rabi oscillations of single electron spins in diamond

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Optically-driven Rabi oscillations of single electron spins in a diamond nitrogen vacancy center are realized with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. The Rabi oscillations are nuclear-spin selective and are robust against rapid decoherence of the underlying optical transitions, opening the door to generating phonon-mediated spin entanglement in an optically-driven spin-phonon system. A direct comparison between the Rabi oscillations and simulated Raman adiabatic passage along with a detailed theoretical analysis provide a wealth of information on the coherent spin dynamics and in particular reveal that decoherence and environmental fluctuations associated with the optical transitions affect the fidelity of the Rabi oscillations through relatively large jumps in the transition frequencies.

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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.

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The coherent control of spin qubits forms the basis of many applications in quantum information processing and nanoscale sensing, imaging, and spectroscopy. Such control is conventionally achieved by direct driving of the qubit transition with a resonant global field, typically at microwave frequencies. Here we introduce an approach that relies on the resonant driving of nearby environment spins, whose localized magnetic field in turn drives the qubit when the environmental spin Rabi frequency matches the qubit resonance. This concept of environmentally mediated resonance (EMR) is explored experimentally using a qubit based on a single nitrogen-vacancy (NV) center in diamond, with nearby electronic spins serving as the environmental mediators. We demonstrate EMR driven coherent control of the NV spin state, including the observation of Rabi oscillations, free induction decay, and spin echo. This technique also provides a way to probe the nanoscale environment of spin qubits, which we illustrate by acquisition of electron spin resonance spectra from single NV centers in various settings.

arXiv:1702.05822•Physical Review Letters•Apr 19, 2017•14 citations
Rabi oscillations and adiabatic passage of single electron spins in a diamond nitrogen vacancy center are demonstrated with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. We show that the optical spin control is nuclear-spin selective and can be robust against rapid decoherence, including radiative decay and spectral diffusion, of the underlying optical transitions. A direct comparison between the Rabi oscillation and the adiabatic passage, along with a detailed theoretical analysis, provides significant physical insights into the connections and differences between these coherent spin processes and also elucidates the role of spectral diffusion in these processes. The optically driven coherent spin processes enable the use of nitrogen vacancy excited states to mediate coherent spin-phonon coupling, opening the door to combining optical control of both spin and mechanical degrees of freedom.
Optically-driven Rabi oscillations of single electron spins in a diamond nitrogen vacancy center are realized with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. The Rabi oscillations are nuclear-spin selective and are robust against rapid decoherence of the underlying optical transitions, opening the door to generating phonon-mediated spin entanglement in an optically-driven spin-phonon system. A direct comparison between the Rabi oscillations and simulated Raman adiabatic passage along with a detailed theoretical analysis provide a wealth of information on the coherent spin dynamics and in particular reveal that decoherence and environmental fluctuations associated with the optical transitions affect the fidelity of the Rabi oscillations through relatively large jumps in the transition frequencies.
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.
We demonstrate coherent control of the optical transition of single nitrogen-vacancy defect centers in diamond. On applying short resonant laser pulses, we observe optical Rabi oscillations with a half period as short as 1 ns, an order of magnitude shorter than the spontaneous emission time. By studying the decay of Rabi oscillations, we find that the decoherence is dominated by laser-induced spectral jumps. By using a low-power probe pulse as a detuning sensor and applying postselection, we demonstrate that spectral diffusion can be overcome in this system to generate coherent photons.
A collapse and revival shape of Rabi oscillations in an electron spin of a single nitrogen-vacancy centre has been observed in diamond at room temperature. Because of hyperfine interaction between the host 14 N nuclear spin and the nitrogen-vacancy centre electron spin, different orientations of the 14 N nuclear spins lead to a triplet splitting of the transition between ground state ( m s = 0) and excited state ( m s = 1). The manipulation of the single electron spin of nitrogen-vacancy centre is achieved by using a combination of selective microwave excitation and optical pumping at 532 nm. Microwaves can excite three transitions equally to induce three independent nutations and the shape of Rabi oscillations is a combination of the three nutations.
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 coherent control of spin qubits forms the basis of many applications in quantum information processing and nanoscale sensing, imaging, and spectroscopy. Such control is conventionally achieved by direct driving of the qubit transition with a resonant global field, typically at microwave frequencies. Here we introduce an approach that relies on the resonant driving of nearby environment spins, whose localized magnetic field in turn drives the qubit when the environmental spin Rabi frequency matches the qubit resonance. This concept of environmentally mediated resonance (EMR) is explored experimentally using a qubit based on a single nitrogen-vacancy (NV) center in diamond, with nearby electronic spins serving as the environmental mediators. We demonstrate EMR driven coherent control of the NV spin state, including the observation of Rabi oscillations, free induction decay, and spin echo. This technique also provides a way to probe the nanoscale environment of spin qubits, which we illustrate by acquisition of electron spin resonance spectra from single NV centers in various settings.