All-optical hyperpolarization of electron and nuclear spins in diamond

Low thermal polarization of nuclear spins is a primary sensitivity limitation for nuclear magnetic resonance. Here we demonstrate optically pumped (microwave-free) nuclear spin polarization of $^{13}\mathrm{C}$ and $^{15}\mathrm{N}$ in $^{15}\mathrm{N}$-doped diamond. $^{15}\mathrm{N}$ polarization enhancements up to $-2000$ above thermal equilibrium are observed in the paramagnetic system $\mathrm{N_s}^{0}$. Nuclear spin polarization is shown to diffuse to bulk $^{13}\mathrm{C}$ with NMR enhancements of $-200$ at room temperature and $-500$ at $\mathrm{240~K}$, enabling a route to microwave-free high-sensitivity NMR study of biological samples in ambient conditions.Comment: 5 pages, 5 figure

Theoretical model of the dynamic spin polarization of nuclei coupled to paramagnetic point defects in diamond and silicon carbide

Dynamic nuclear spin polarization (DNP) mediated by paramagnetic point defects in semiconductors is a key resource for both initializing nuclear quantum memories and producing nuclear hyperpolarization. DNP is therefore an important process in the field of quantum-information processing, sensitivity-enhanced nuclear magnetic resonance, and nuclear-spin-based spintronics. DNP based on optical pumping of point defects has been demonstrated by using the electron spin of nitrogen-vacancy (NV) center in diamond, and more recently, by using divacancy and related defect spins in hexagonal silicon carbide (SiC). Here, we describe a general model for these optical DNP processes that allows the effects of many microscopic processes to be integrated. Applying this theory, we gain a deeper insight into dynamic nuclear spin polarization and the physics of diamond and SiC defects. Our results are in good agreement with experimental observations and provide a detailed and unified understanding. In particular, our findings show that the defects' electron spin coherence times and excited state lifetimes are crucial factors in the entire DNP process

The Principles of Social Order. Selected Essays of Lon L. Fuller, edited With an introduction by Kenneth I. Winston

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab initio simulations, we show that spin-spin interactions in 4H-SiC neutral divacancies give rise to spin states with a strong Stark effect, sub-10(-6) strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15%-36%. These results establish SiC color centers as compelling systems for sensing nanoscale electric and strain fields

High fidelity bi-directional nuclear qubit initialization in SiC

Dynamic nuclear polarization (DNP) is an attractive method for initializing nuclear spins that are strongly coupled to optically active electron spins because it functions at room temperature and does not require strong magnetic fields. In this Letter, we demonstrate that DNP, with near-unity polarization efficiency, can be generally realized in weakly coupled hybrid registers, and furthermore that the nuclear spin polarization can be completely reversed with only sub-Gauss magnetic field variations. This mechanism offers new avenues for DNP-based sensors and radio-frequency free control of nuclear qubits

Optical polarization of nuclear spins in silicon carbide

We demonstrate optically pumped dynamic nuclear polarization of 29-Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H- and 6H-SiC. The 99 +/- 1% degree of polarization at room temperature corresponds to an effective nuclear temperature of 5 microKelvin. By combining ab initio theory with the experimental identification of the color centers' optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging.Comment: 21 pages including supplementary information; four figures in main text and one tabl

Isolated spin qubits in SiC with a high-fidelity infrared spin-to-photon interface

The divacancies in SiC are a family of paramagnetic defects that show promise for quantum communication technologies due to their long-lived electron spin coherence and their optical addressability at near-telecom wavelengths. Nonetheless, a mechanism for high-fidelity spin-to-photon conversion, which is a crucial prerequisite for such technologies, has not yet been demonstrated. Here we demonstrate a high-fidelity spin-to-photon interface in isolated divacancies in epitaxial films of 3C-SiC and 4H-SiC. Our data show that divacancies in 4H-SiC have minimal undesirable spin-mixing, and that the optical linewidths in our current sample are already similar to those of recent remote entanglement demonstrations in other systems. Moreover, we find that 3C-SiC divacancies have millisecond Hahn-echo spin coherence time, which is among the longest measured in a naturally isotopic solid. The presence of defects with these properties in a commercial semiconductor that can be heteroepitaxially grown as a thin film on shows promise for future quantum networks based on SiC defects.Comment: 26 pages, 4 figure

Electrically and mechanically tunable electron spins in silicon carbide color centers

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields.Comment: 10 pages, 4 figures, 1 tabl

Theoretical model of dynamic spin polarization of nuclei coupled to paramagnetic point defects in diamond and silicon carbide

Dynamic nuclear spin polarization (DNP) mediated by paramagnetic point defects in semiconductors is a key resource for both initializing nuclear quantum memories and producing nuclear hyperpolarization. DNP is therefore an important process in the field of quantum-information processing, sensitivity-enhanced nuclear magnetic resonance, and nuclear-spin-based spintronics. DNP based on optical pumping of point defects has been demonstrated by using the electron spin of nitrogen-vacancy (NV) center in diamond, and more recently, by using divacancy and related defect spins in hexagonal silicon carbide (SiC). Here, we describe a general model for these optical DNP processes that allows the effects of many microscopic processes to be integrated. Applying this theory, we gain a deeper insight into dynamic nuclear spin polarization and the physics of diamond and SiC defects. Our results are in good agreement with experimental observations and provide a detailed and unified understanding. In particular, our findings show that the defects electron spin coherence times and excited state lifetimes are crucial factors in the entire DNP process

Optical Polarization of Nuclear Spins in Silicon Carbide

We demonstrate optically pumped dynamic nuclear polarization of 29Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H- and 6H-SiC. The 99 ± 1% degree of polarization at room temperature corresponds to an effective nuclear temperature of 5 K. By combining ab initio theory with the experimental identification of the color centers’ optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging