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Register a new userMeasurement of the excited-state transverse hyperfine coupling in NV centers via dynamic nuclear polarization
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Precise knowledge of a quantum systems Hamiltonian is a critical pre-requisite for its use in many quantum information technologies. Here, we report a method for the precise characterization of the non-secular part of the excited-state Hamiltonian of an electronic-nuclear spin system in diamond. The method relies on the investigation of the dynamic nuclear polarization mediated by the electronic spin, which is currently exploited as a primary tool for initializing nuclear qubits and performing enhanced nuclear magnetic resonance. By measuring the temporal evolution of the population of the ground-state hyperfine levels of a nitrogen-vacancy center, we obtain the first direct estimation of the excited-state transverse hyperfine coupling between its electronic and nitrogen nuclear spin. Our method could also be applied to other electron-nuclear spin systems, such as those related to defects in silicon carbide.
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We report a versatile method to efficiently polarize single nuclear spins in diamond, which is based on optical pumping of a single NV color center and mediated by a level-anti crossing in its excited state. A nuclear spin polarization higher than 98% is achieved at room temperature for the 15N nuclear spin associated to the NV center, corresponding to $mu$K effective nuclear spin temperature. We then show simultaneous deterministic initialization of two nuclear spins (13C and 15N) in close vicinity to a NV defect. Such robust control of nuclear spin states is a key ingredient for further scaling up of nuclear-spin based quantum registers in diamond.
Dynamic nuclear polarisation (DNP) refers to a class of techniques used to increase the signal in nuclear magnetic resonance measurements by transferring spin polarisation from ensembles of highly polarised electrons to target nuclear analytes. These techniques, however, require the application of strong magnetic fields to maximise electron spin polarisation, limiting pathways for electron-nuclear (hyperfine) spin coupling and transfer. In this work we show that, for systems of electronic spin $Sgeq1$ possessing an intrinsic zero-field splitting, a separate class of stronger hyperfine interactions based on lab-frame cross relaxation may be utilised to improve DNP efficiency and yield, whilst operating at moderate fields. We analytically review existing methods, and determine that this approach increases the rate of polarisation transfer to the nuclear ensemble by up to an order of magnitude over existing techniques. This result is demonstrated experimentally at room temperature using the optically polarisable $S=1$ electron spin system of the nitrogen vacancy (NV) defect in diamond as the source of electron spin polarisation. Finally we assess the utility of these NV-based approaches for the polarisation of macroscopic quantities of molecular spins external to the diamond for NMR and MRI applications.
Hybrid quantum registers consisting of different types of qubits offer a range of advantages as well as challenges. The main challenge is that some types of qubits react only slowly to external control fields, thus considerably slowing down the information processing operations. One promising approach that has been tested in a number of cases is to use indirect control, where external fields are applied only to qubits that interact strongly with resonant excitation pulses. Here we use this approach to indirectly control the nuclear spins of an NV center, using microwave pulses to drive the electron spin, combined with free precession periods optimized for generating logical gate operations on the nuclear spins. The scheme provides universal control and we present two typical applications: polarizing the nuclear spin and measuring nuclear spin free induction decay signals, both without applying radio-frequency pulses. This scheme is versatile as it can be implemented over a wide range of magnetic field strengths and at any temperature.
We studied the dynamic nuclear spin polarization of nitrogen in negatively charged nitrogen-vacancy (NV) centers in diamond both experimentally and theoretically over a wide range of magnetic fields from 0 to 1100 G covering both the excited-state level anti-crossing and the ground-state level anti-crossing magnetic field regions. Special attention was paid to the less studied ground-state level anti-crossing region. The nuclear spin polarization was inferred from measurements of the optically detected magnetic resonance signal. These measurements show that a very large (up to $96 pm 2%$) nuclear spin polarization of nitrogen can be achieved over a very broad range of magnetic field starting from around 400 G up to magnetic field values substantially exceeding the ground-state level anti-crossing at 1024 G. We measured the influence of angular deviations of the magnetic field from the NV axis on the nuclear spin polarization efficiency and found that, in the vicinity of the ground-state level anti-crossing, the nuclear spin polarization is more sensitive to this angle than in the vicinity of the excited-state level anti-crossing. Indeed, an angle as small as a tenth of a degree of arc can destroy almost completely the spin polarization of a nitrogen nucleus. In addition, we investigated theoretically the influence of strain and optical excitation power on the nuclear spin polarization.
Energy levels of nitrogen-vacancy centers in diamond were investigated using optically detected magnetic-resonance spectroscopy near the electronic ground-state level anticrossing (GSLAC) at an axial magnetic field around 102.4~mT in diamond samples with a nitrogen concentration of 1~ppm and 200~ppm. By applying radiowaves in the frequency ranges from 0 to 40 MHz and from 5.6 to 5.9 GHz, we observed transitions that involve energy levels mixed by the hyperfine interaction. We developed a theoretical model that describes the level mixing, transition energies, and transition strengths between the ground-state sublevels, including the coupling to the nuclear spin of the NV centertextquotesingle s $^{14}$N and $^{13}$C atoms. The calculations were combined with the experimental results by fitting the ODMR spectral lines based on a theoretical model, which yielded information about the polarization of nuclear spins. This study is important for the optimization of experimental conditions in GSLAC-based applications, e.g., microwave-free magnetometry and microwave-free nuclear-magnetic-resonance probes.
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