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arXiv:2007.14673 · Physical Review Letters

Orbital and Spin Dynamics of Single Neutrally-Charged Nitrogen-Vacancy Centers in Diamond

Simon Baier, C. E. Bradley, Thomas Middelburg, V. V. Dobrovitski, T. H. Taminiau, Ronald Hanson

Published Nov 4, 2020• 26 citations
arXivHTMLPDF

Abstract

The neutral charge state plays an important role in quantum information and sensing applications based on nitrogen-vacancy centers. However, the orbital and spin dynamics remain unexplored. Here, we use resonant excitation of single centers to directly reveal the fine structure, enabling selective addressing of spin-orbit states. Through pump-probe experiments, we find the orbital relaxation time (430 ns at 4.7 K) and measure its temperature dependence up to 11.8 K. Finally, we reveal the spin relaxation time (1.5 s) and realize projective high-fidelity single-shot readout of the spin state (≥98%).

DOI
10.1103/physrevlett.125.193601

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The neutral charge state plays an important role in quantum information and sensing applications based on nitrogen-vacancy centers. However, the orbital and spin dynamics remain unexplored. Here, we use resonant excitation of single centers to directly reveal the fine structure, enabling selective addressing of spin-orbit states. Through pump-probe experiments, we find the orbital relaxation time (430 ns at 4.7 K) and measure its temperature dependence up to 11.8 K. Finally, we reveal the spin relaxation time (1.5 s) and realize projective high-fidelity single-shot readout of the spin state (≥98%).
Abstract High-fidelity projective readout of a qubit’s state in a single experimental repetition is a prerequisite for various quantum protocols of sensing and computing. Achieving single-shot readout is challenging for solid-state qubits. For Nitrogen-Vacancy (NV) centers in diamond, it has been realized using nuclear memories or resonant excitation at cryogenic temperature. All of these existing approaches have stringent experimental demands. In particular, they require a high efficiency of photon collection, such as immersion optics or all-diamond micro-optics. For some of the most relevant applications, such as shallow implanted NV centers in a cryogenic environment, these tools are unavailable. Here we demonstrate an all-optical spin readout scheme that achieves single-shot fidelity even if photon collection is poor (delivering less than 10 3 clicks/second). The scheme is based on spin-dependent resonant excitation at cryogenic temperature combined with spin-to-charge conversion, mapping the fragile electron spin states to the stable charge states. We prove this technique to work on shallow implanted NV centers, as they are required for sensing and scalable NV-based quantum registers.
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.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
A functioning qubit must be able to be initialized and measured. The fidelity of these operations is essential for all quantum applications, including quantum sensing, communication, and computation. The diamond nitrogen-vacancy (NV) center is a point defect in the lattice with an optical interface to a coherent ground-state spin, which makes the NV center one of the few spin qubits operable at room temperature. While the NV center spin state can be initialized and read out optically, the fidelity of these operations are far from perfect due to the charge and orbital dynamics. In typical conditions, the NV center is in the proper charge state 75% of the time, and measuring the spin state results in a non-zero signal only 1% of the time. These inefficient mechanisms make many measurements practically intractable. This thesis focuses on improving the preparation and measurement fidelities of NV centers through precise all-optical control of the charge, orbital, and spin dynamics. I first discuss an improved spin readout mechanism which relies on spin-to-charge conversion (SCC) and discuss the potential for single-shot spin readout. Following, I present how charge readout and SCC can be implemented in ensembles of NV centers within nanodiamonds and demonstrate that it provides improvements for spin-relaxometry studies. Finally, I develop a method for initializing a single NV center's charge state with real-time control and show that this capability improves spin readout performance for sensing. To conclude, I discuss how these improved initialization and readout capabilities can be applied to detecting and controlling coupled nuclear spins in the diamond lattice and consider other applications of real-time control.
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.
Abstract The nitrogen‐vacancy (NV) center in diamond is a widely utilized system due to its useful quantum properties. Almost all research focuses on the negative charge state (NV − ) and comparatively little is understood about the neutral charge state (NV 0 ). This is surprising as the charge state often fluctuates between NV 0 and NV − during measurements. There are potentially under‐utilized technical applications that could take advantage of NV 0 , either by improving the performance of NV 0 or utilizing NV − directly. However, the fine structure of NV 0 has not been observed. Here, we rectify this lack of knowledge by performing magnetic circular dichroism measurements that quantitatively determine the fine structure of NV 0 . The observed behavior is accurately described by spin‐Hamiltonians in the ground and excited states with the ground state yielding a spin‐orbit coupling of λ = 2.24 ± 0.05 GHz and a orbital g ‐factor of 0.0186 ± 0.0005. The reasons why this fine structure has not been previously measured are discussed and strain‐broadening is concluded to be the likely reason.