本文报道了在X波段磁场（280-400 mT）和低温（2-70 K）下，金刚石中负电荷氮空位中心（NVPDMATHABMM）系综的脉冲ESR实验。通过高能电子辐照和随后的退火，制备具有本体浓度为$2\cdot 10^{13}$ cm $^{-3}$至$4\cdot 10^{14}$ cm $^{-3}$的合成IIb型金刚石中的NV $^-$中心（氮杂质浓度$<1$ ~ppm）。我们发现，适当的辐射后退火（1000 $^\circ$ C 60分钟）是至关重要的辐射损伤的修复和恢复长的电子自旋相干时间的NV $^-$ s。退火后，在5~K温度下获得了T $_2 = 0.74$ ~ms的自旋相干时间，仅受天然丰度金刚石中$^{13}$ C核谱扩散的限制。在X波段磁场下，观测到了源自中心$^{14}$ N核的强电子自旋回波包络调制（ESEEM）。ESEEM光谱分析允许精确测定$^{14}$ N核超精细和四极张量。此外，ESEEM效应从两个近端$^{13}$ C网站（第二最近的邻居和第四最近的邻居）解决和各自的$^{13}$ C超精细耦合常数提取。
英文摘要：
Pulsed ESR experiments are reported for ensembles of negatively-charged nitrogen-vacancy centers (NV$^-$) in diamonds at X-band magnetic fields (280-400 mT) and low temperatures (2-70 K). The NV$^-$ centers in synthetic type IIb diamonds (nitrogen impurity concentration $<1$~ppm) are prepared with bulk concentrations of $2\cdot 10^{13}$ cm$^{-3}$ to $4\cdot 10^{14}$ cm$^{-3}$ by high-energy electron irradiation and subsequent annealing. We find that a proper post-radiation anneal (1000$^\circ$C for 60 mins) is critically important to repair the radiation damage and to recover long electron spin coherence times for NV$^-$s. After the annealing, spin coherence times of T$_2 = 0.74$~ms at 5~K are achieved, being only limited by $^{13}$C nuclear spectral diffusion in natural abundance diamonds. At X-band magnetic fields, strong electron spin echo envelope modulation (ESEEM) is observed originating from the central $^{14}$N nucleus. The ESEEM spectral analysis allows for accurate determination of the $^{14}$N nuclear hypefine and quadrupole tensors. In addition, the ESEEM effects from two proximal $^{13}$C sites (second-nearest neighbor and fourth-nearest neighbor) are resolved and the respective $^{13}$C hyperfine coupling constants are extracted.
High frequency electron spin resonance (ESR) spectroscopy is an invaluable tool for identification and characterization of spin systems. Nanoscale ESR using the nitrogen-vacancy (NV) center has been demonstrated down to the level of a single spin. However, NV-detected ESR has exclusively been studied at low magnetic fields, where spectral overlap prevents clear identification of spectral features. Within this work, we demonstrate NV-detected ESR measurements of single-substitutional nitrogen impurities in diamond at a NV Larmor frequency of 115 GHz and the corresponding magnetic field of 4.2 T…
The unavoidable presence of vibrations in solid-state devices can drastically modify the expected electron spin resonance (ESR) absorption spectrum in magnetically active systems. In this work, we model the effect of phonons and temperature on the ESR signal in molecular systems with strong $E \otimes e$ Jahn-Teller (JT) effect and an electronic spin-$1/2$. Our microscopic model considers the linear JT interaction with a continuum of phonon modes, the spin-orbit coupling, the Zeeman effect, and the response of the system under a weak oscillating magnetic field. We derive a Lindblad master equa…
Nitrogen-vacancy (NV) centers in diamond can be used for nanoscale sensing with atomic resolution and sensitivity; however, it has been observed that their properties degrade as they approach the diamond surface. Here we report that in addition to degraded spin coherence, NV centers within nanometers of the surface can also exhibit decreased fluorescence contrast for optically detected electron spin resonance (OD-ESR). We demonstrate that this decreased OD-ESR contrast arises from charge state dynamics of the NV center, and that it is strongly surface-dependent, indicating that surface enginee…
Electron spin resonance (ESR) spectroscopy has broad applications in physics, chemistry and biology. As a complementary tool, zero-field ESR (ZF-ESR) spectroscopy has been proposed for decades and shown its own benefits for investigating the electron fine and hyperfine interaction. However, the ZF-ESR method has been rarely used due to the low sensitivity and the requirement of much larger samples than conventional ESR. In this work, we present a method for deploying ZF-ESR spectroscopy at the nanoscale by using a highly sensitive quantum sensor, the nitrogen-vacancy center in diamond. We also…
The nitrogen-vacancy (NV) center has enabled widespread study of nanoscale nuclear magnetic resonance (NMR) spectroscopy at low magnetic fields. NMR spectroscopy at high magnetic fields significantly improves the technique's spectral resolution, enabling clear identification of closely related chemical species. However, NV-detected NMR is typically performed using AC sensing through electron spin echo envelope modulation (ESEEM), a hyperfine spectroscopic technique that is not feasible at high magnetic fields. Within this paper, we have explored an NV-detected NMR technique for applications of…
Electron and nuclear spins of diamond nitrogen-vacancy (NV) centers are good candidates for quantum information processing as they have long coherence time and can be initialized and read out optically. However, creating a large number of coherently coupled and individually addressable NV centers for quantum computing has been a big challenge. Here we propose methods to use high-density diamond NV centers coupled by spin-spin interaction with an average separation on the order of 10 nm for quantum computing. We propose to use a strain gradient to encode the position information of each NV cent…
We consider the problem of determining the spectrum of an electronic spin via polarization transfer to coupled nuclear spins and their subsequent readout. This suggests applications for employing dynamic nuclear polarization (DNP) for "ESR-via-NMR". In this paper, we describe the theoretical basis for this process by developing a model for the evolution dynamics of the coupled electron-nuclear system through a cascade of Landau-Zener anti-crossings (LZ-LACs). We develop a method to map these traversals to the operation of an equivalent "Galton board". Here, LZ-LAC points serve as analogues to …
