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Pulse-width-induced polarization enhancement of optically-pumped N-V electron spin in diamond

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 Added by Nanyang Xu
 Publication date 2019
  fields Physics
and research's language is English




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The nitrogen-vacancy (N-V) center in diamond is a widely-used platform for quantum information processing and metrology. The electron-spin state of N-V center could be initialized and readout optically, and manipulated by resonate microwave fields. In this work, we analyze the dependence of electron-spin initialization on widths of laser pulses. We build a numerical model to simulate this process and verify the simulation results in experiment. Both simulations and experiments reveal a fact that shorter laser pulses are helpful to the electron-spin polarization. We therefore propose to use extremely-short laser pulses for electron-spin initialization. In this new scheme, the spin-state contrast could be improved about 10% in experiment by using laser pulses as short as 4 ns in width. Furthermore, we provide a mechanism to explain this effect which is due to the occupation time in the meta-stable spin-singlet states of N-V center. Our new scheme is applicable in a broad range of NV-based applications in the future.



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The sensitivity of Magnetic Resonance Imaging (MRI) depends strongly on nuclear spin polarisation and, motivated by this observation, dynamical nuclear spin polarisation has recently been applied to enhance MRI protocols (Kurhanewicz, J., et al., Neoplasia 13, 81 (2011)). Nuclear spins associated with the 13 C carbon isotope (nuclear spin I = 1/2) in diamond possess uniquely long spin lattice relaxation times (Reynhardt, E.C. and G.L. High, Prog. in Nuc. Mag. Res. Sp. 38, 37 (2011)) If they are present in diamond nanocrystals, especially when strongly polarised, they form a promising contrast agent for MRI. Current schemes for achieving nuclear polarisation, however, require cryogenic temperatures. Here we demonstrate an efficient scheme that realises optically induced 13 C nuclear spin hyperpolarisation in diamond at room temperature and low ambient magnetic field. Optical pumping of a Nitrogen-Vacancy (NV) centre creates a continuously renewable electron spin polarisation which can be transferred to surrounding 13 C nuclear spins. Importantly for future applications we also realise polarisation protocols that are robust against an unknown misalignment between magnetic field and crystal axis.
The interplay between disorder and transport is a problem central to the understanding of a broad range of physical processes, most notably the ability of a system to reach thermal equilibrium. Disorder and many body interactions are known to compete, with the dominance of one or the other giving rise to fundamentally different dynamical phases. Here we investigate the spin diffusion dynamics of 13C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We focus on low-abundance, strongly hyperfine-coupled nuclei, whose role in the polarization transport we expose through the integrated impact of variable radio-frequency excitation on the observable bulk 13C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings. Our results open intriguing opportunities to study the onset of thermalization in a system by controlling the internal interactions within the bath.
The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the transfer protocol suggest slower molecular diffusion near the diamond surface compared to that in bulk, an observation consistent with present models of the microscopic structure of a fluid close to a solid interface.
We study the effect of optical squeezing on the performance of a sensitive, quantum-noise-limited optically-pumped magnetometer. We use Bell-Bloom optical pumping to excite a $^{87}$Rb vapor and Faraday rotation to detect spin precession. The sub-$mathrm{pT}/sqrt{mathrm{Hz}}$ sensitivity is limited by spin projection noise (photon shot noise) at low (high) frequencies. Probe polarization squeezing both improves high-frequency sensitivity and increases signal bandwidth. The accompanying polarization anti-squeezing perturbs only an unmeasured spin component, so there is no loss of sensitivity at any frequency. The method is compatible with high-density and multi-pass techniques that reach extreme sensitivity.
The nitrogen-vacancy (N-V) 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 ($m_s = pm 1$) 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 N-V center. We first apply this technique to N-V ensembles in [100] and [111]-oriented samples. Next, we demonstrate an imaging technique, based on optical polarization dependence, that allows rapid identification of the orientations of many single N-V centers. Finally, we test the microwave polarization selection rules of individual N-V centers of known orientation.
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