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arXiv:1008.1103 · Physical Review A

Multifrequency spin resonance in diamond

Lilian Childress, Jean McIntyre

Published Sep 30, 2010• 62 citations
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Abstract

Magnetic resonance techniques provide a powerful tool for controlling spin systems, with applications ranging from quantum information processing to medical imaging. Nevertheless, the behavior of a spin system under strong excitation remains a rich dynamical problem. In this paper, we examine spin resonance of the nitrogen-vacancy center in diamond under conditions outside the regime where the usual rotating-wave approximation applies, focusing on effects of multifrequency excitation and excitation with orientation parallel to the spin quantization axis. Strong-field phenomena such as multiphoton transitions and coherent destruction of tunneling are observed in the spectra and analyzed via numerical and analytic theory. In addition to illustrating the response of a spin system to strong multifrequency excitation, these observations may inform techniques for manipulating electron-nuclear spin quantum registers.

DOI
10.1103/physreva.82.033839

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Magnetic resonance techniques provide a powerful tool for controlling spin systems, with applications ranging from quantum information processing to medical imaging. Nevertheless, the behavior of a spin system under strong excitation remains a rich dynamical problem. In this paper, we examine spin resonance of the nitrogen-vacancy center in diamond under conditions outside the regime where the usual rotating-wave approximation applies, focusing on effects of multifrequency excitation and excitation with orientation parallel to the spin quantization axis. Strong-field phenomena such as multiphoton transitions and coherent destruction of tunneling are observed in the spectra and analyzed via numerical and analytic theory. In addition to illustrating the response of a spin system to strong multifrequency excitation, these observations may inform techniques for manipulating electron-nuclear spin quantum registers.
The nitrogen-vacancy (NV) center in diamond has been the focus of research efforts because of its suitability for use in applications such as quantum sensing and quantum simulations. Recently, the electron-spin double resonance (ESDR) of NV centers has been exploited for detecting radio-frequency (RF) fields with continuous-wave optically detected magnetic resonance. However, the characteristic phenomenon of ESDR under a strong RF field remains to be fully elucidated. In this study, we theoretically and experimentally analyzed the ESDR spectra under strong RF fields by adopting Floquet theory. Our analytical and numerical calculations could reproduce the ESDR spectra obtained by measuring the spin-dependent photoluminescence under the continuous application of a microwave and a RF field for a DC bias magnetic field perpendicular to the NV axis. We found that anticrossing structures that appear under a strong RF field are induced by the generation of RF-dressed states owing to the two-RF-photon resonances. Moreover, we found that 2n2n2n-RF-photon resonances were allowed by an unintentional DC bias magnetic field parallel to the NV axis. These results should help in the realization of precise MHz-range AC magnetometry with a wide dynamic range beyond the rotating wave approximation regime as well as Floquet engineering in open quantum systems.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.
The nitrogen vacancy (NV) center in diamond is promising as an electron spin qubit due to its long-lived coherence and optical addressability. The ground state is a spin triplet with two levels $({m}_{s}=\ifmmode\pm\else\textpm\fi{}1)$ degenerate at zero magnetic field. Polarization-selective microwave excitation is an attractive method to address the spin transitions independently since this allows operation down to zero magnetic field. Using a resonator designed to produce circularly polarized microwaves, we have investigated the polarization selection rules of the NV center. We first apply this technique to NV ensembles in [100]- and [111]-oriented samples. Next, we demonstrate an imaging technique, based on optical polarization dependence, which allows rapid identification of the orientations of many single NV centers. Finally, we test the microwave polarization selection rules of individual NV centers of known orientation.
Quantum systems driven by strong oscillating fields are the source of many interesting physical phenomena. In this work, we experimentally study the dynamics of a two-level system of a single spin driven in the strong-driving regime where the rotating-wave approximation is not valid. This two-level system is a subsystem of a single nitrogen-vacancy (NV) center in diamond coupled to a first-shell 13C^{13}\mathrm{C}13C nuclear spin at a level anticrossing point. This near degeneracy occurs in the ${m}_{s}=\ifmmode\pm\else\textpm\fi{}1$ manifold of the electron spin when the energy level splitting between the ${m}_{s}=\ensuremath{-}1$ and +1+1+1 states due to the static magnetic field is $\ensuremath{\approx}127$ MHz and thus equal to the splitting due to the 13C^{13}\mathrm{C}13C hyperfine interaction. The transition frequency of this electron spin two-level system in a static magnetic field of 28.9 G is 1.7 MHz and it can be driven only by the component of the radio-frequency (RF) field along the NV symmetry axis. Electron spin Rabi frequencies in this system can reach tens of MHz even for moderate RF powers. The simple sinusoidal Rabi oscillations that occur when the amplitude of the driving field is small compared to the transition frequency evolve into complex patterns when the driving field amplitude is comparable to or greater than the energy level splitting. We observe that the system oscillates faster than the amplitude of the driving field and the response of the system shows multiple frequencies.
Dynamical decoupling multipulse sequences can be applied to solid-state spins for sensing weak oscillating fields from nearby single nuclear spins. By periodically reversing the probing system's evolution, other noises are counteracted and filtered out over the total evolution. However, the technique is subject to intricate interactions resulting in additional resonant responses, which can be misinterpreted with the actual signal intended to be measured. We experimentally characterize three of these effects present in single nitrogen-vacancy centers in diamond, where we also develop a numerical simulation model without rotating-wave approximation, showing robust correlation to the experimental data. Regarding centers with the N 15 nitrogen isotope, we observe that a small misalignment in the bias magnetic field causes the precession of the nitrogen nuclear spin to be sensed by the electronic spin of the center. Another studied case of ambiguous resonances comes from the coupling with lattice C 13 nuclei, where we use the echo modulation frequencies to obtain the interaction Hamiltonian and then utilize the latter to simulate multipulse sequences. Finally, we also measure and simulate the effects from the free evolution of the quantum system during finite pulse durations. Due to the large data volume and the strong dependence of these ambiguous resonances with specific experimental parameters, we provide a simulations data set with a user-friendly graphical interface, where users can compare simulations with their own experimental data for spectral disambiguation. Although focused on nitrogen-vacancy centers and dynamical decoupling sequences, these results and the developed model can potentially be applied to other solid-state spins and quantum sensing techniques.
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.