We report a versatile method to polarize single nuclear spins in diamond, based on optical pumping of a single nitrogen-vacancy (NV) defect and mediated by a level anticrossing in its excited state. A nuclear-spin polarization higher than 98% is achieved at room temperature for the 15N nuclear spin associated with the NV center, corresponding to microK effective nuclear-spin temperature. We then show simultaneous initialization of two nuclear spins in the vicinity of 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.
Nuclear hyperpolarization from optically pumped color centers in solids offers an alternative to conventional microwave-driven dynamic nuclear polarization (DNP). Diamond can host the nitrogen vacancy (NV) center, whose ground spin state can be readily polarized by light at room temperature, making diamond a candidate platform for nuclear hyperpolarization. We report
13C nuclear hyperpolarization in randomly oriented diamond particles with sizes ranging from 0.2 to 2
μm, both at natural
13C abundance (1.1 %) and at 20 % isotopic enrichment, at magnetic fields of 7.1 T and 9.4 T. The protocol combines optical illumination with magic angle spinning (MAS) and does not require microwave irradiation. By investigating the nuclear polarization as a function of the MAS frequency between 0 and 6 kHz at the magnetic field of 7.1 T, we find maximum light-induced polarization enhancements of
280-fold for the isotopically enriched sample and
411-fold for the natural abundance sample. Under continuous illumination, steady-state absolute
13C polarization levels above 0.1 % are reached. A model involving optical pumping of NV centers and spin dynamics near level anticrossings (LACs) in three-spin clusters formed by NV, a substitutional nitrogen (P1) and
13C is used to describe these findings. The protocol strongly mitigates the effect of the anisotropy of the NV spin Hamiltonian, allowing more than
99.9% of NV orientations to participate in the polarization transfer process. These results represent a first step toward transferring nuclear polarization from diamond particles to external nuclei, with potential applications in sensitive and high-resolution NMR at room temperature.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.
Dephasing and relaxation of the nuclear spins coupled to the nitrogen-vacancy (NV) center during optical initialization and readout is an important issue for various applications of this hybrid quantum register. Here we present both an analytical description and a numerical simulation for this process, which agree reasonably with the experimental measurements. For an NV center under cyclic optical transition, our analytical formulas not only provide a clear physical picture, but also allow control of the nuclear spin dissipation by tuning an external magnetic field. For more general optical pumping, our analytical formulas reveal a significant contribution to the nuclear spin dissipation due to electron random hopping into/out of the m = 0 (or ) subspace. This contribution is not suppressed, even under saturated optical pumping and/or vanishing magnetic field, thus providing a possible solution to the puzzling observation of nuclear spin dephasing in zero perpendicular magnetic field Dutt et al (2007 Science 316 1312). It also implies that enhancing the degree of optical spin polarization of the nitrogen-vacancy center can reduce the effect of optically induced nuclear spin dissipation.
Dephasing and relaxation of the nuclear spins coupled to the nitrogen-vacancy (NV) center during optical initialization and readout is an important issue for various applications of this hybrid quantum register. Here we present both an analytical description and a numerical simulation for this process, which agree reasonably with the experimental measurements. For an NV center under cyclic optical transition, our analytical formulas not only provide a clear physical picture, but also allow control of the nuclear spin dissipation by tuning an external magnetic field. For more general optical pumping, our analytical formulas reveal a significant contribution to the nuclear spin dissipation due to electron random hopping into/out of the m = 0 (or ) subspace. This contribution is not suppressed, even under saturated optical pumping and/or vanishing magnetic field, thus providing a possible solution to the puzzling observation of nuclear spin dephasing in zero perpendicular magnetic field Dutt et al (2007 Science 316 1312 ). It also implies that enhancing the degree of optical spin polarization of the nitrogen-vacancy center can reduce the effect of optically induced nuclear spin dissipation.