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Bulletin of the American Physical Society

Spin decoherence of a single NV center in its orbital excited state

V. V. Dobrovitski, Gregory D. Fuchs, D.M. Toyli, F. Joseph Heremans, C. D. Weiss, Thomas Schenkel, D. D. Awschalom

Published Mar 16, 2010• 0 citations
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Bulletin of the American Physical Society•Mar 16, 2010•0 citations

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Lee C. Bassett

For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.

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Spin Coherence during Optical Excitation of a Single Nitrogen-Vacancy Center in Diamond

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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.

arXiv:1111.3687•Physical Review Letters•Apr 12, 2012•34 citations
For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.
Optically addressable spin defects in solid-state materials have shown great potential for applications ranging from metrology to quantum information processing. Many of these experiments require a detailed understanding of the full Hamiltonian dynamics in order to develop precise quantum control. Here we use picosecond resonant optical pulses to investigate the coherent orbital and spin dynamics of the nitrogen-vacancy (NV) center in diamond, over timescales spanning six orders of magnitude. We implement an ultrafast optical pump-probe technique to study the NV center’s orbital-doublet, spin-triplet excited state at cryogenic temperatures (T < 20 K), where the excited state becomes stable and optically coherent with the ground state. This technique, coupled with optical polarization selection rules, allows us to probe the coherent orbital dynamics of the NV center’s excited state [1]. These experiments reveal dynamics on femtosecond to nanosecond timescales due to the interplay between the ground and excited state orbital levels. This all-optical technique also provides a method to dynamically control the spin state of the NV center by harnessing the excited state structure. Through studying the spin dynamics of the NV center with coherent pulses of light, we are able to rotate the spin state on sub-nanosecond timescales. Furthermore, by tuning the excited-state spin Hamiltonian with an external magnetic eld, we demonstrate arbitrary-axis spin rotations through controlled unitary evolution of the spin state. Extending this to the full excited-state manifold, we develop a time-domain quantum tomography technique to precisely map the NV center’s excited state Hamiltonian. These techniques generalize to other systems and can be a powerful tool in characterizing and controlling qubits in other optically addressable spin systems.
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.