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Optically active spin defects in solids offer promising platforms to investigate nuclear spin clusters with high sensitivity and atomic-site resolution. To leverage near-surface defects for molecular structure analysis in chemical and biological contexts using nuclear magnetic resonance (NMR), further advances in spectroscopic characterization of nuclear environments are essential. Here, we report Fourier spectroscopy techniques to improve localization and mapping of the testbed $^{13}\mathrm{C}$ nuclear spin environment of individual, shallow nitrogen-vacancy centers at room temperature. We use multidimensional spectroscopy, well-known from classical NMR, in combination with weak measurements of single-nuclear-spin precession. We demonstrate two examples of multidimensional NMR: (i) improved nuclear spin localization by separate encoding of the two hyperfine components along spectral dimensions and (ii) spectral editing of nuclear-spin pairs, including measurement of internuclear coupling constants. Our work adds important tools for the spectroscopic analysis of molecular structures by single-spin probes., Comment: 7 pages, 3 figures

Coupling between a single quantum emitter and an optical cavity presents a key capability for future quantum networking applications. Here, we explore interactions between individual germanium-vacancy (GeV) defects in diamond and an open microcavity at cryogenic temperatures. Exploiting the tunability of our microcavity system to characterize and select emitters, we observe a Purcell-effect-induced lifetime reduction of up to $4.5\pm0.3$, and extract coherent coupling rates up to $360\pm20$ MHz. Our results indicate that the GeV defect has favorable optical properties for cavity coupling, with a quantum efficiency of at least $0.34\pm0.05$ and likely much higher., Comment: 14 pages, 6 figures, journal accepted version after initial review

The long-lived electronic spin of the nitrogen-vacancy (NV) center in diamond is a promising quantum sensor for detecting nanoscopic magnetic and electric fields in a variety of experimental conditions. Nevertheless, an outstanding challenge in improving measurement sensitivity is the poor signal-to-noise ratio (SNR) of prevalent optical spin-readout techniques. Here, we address this limitation by coupling individual NV centers to optimized diamond nanopillar structures, thereby improving optical collection efficiency of fluorescence. First, we optimize the structure in simulation, observing an increase in collection efficiency for tall ($\geq$ 5 $\mu$m) pillars with tapered sidewalls. We subsequently verify these predictions by fabricating and characterizing a representative set of structures using a reliable and reproducible nanofabrication process. An optimized device yields increased SNR, owing to improvements in collimation and directionality of emission. Promisingly, these devices are compatible with low-numerical-aperture, long-working-distance collection optics, as well as reduced tip radius, facilitating improved spatial resolution for scanning applications., Comment: 22 pages, five figures

Photoexcitable donor-bridge-acceptor (D-B-A) molecules that support intramolecular charge transfer are ideal platforms to probe the influence of chiral-induced spin selectivity (CISS) in electron transfer and resulting radical pairs. In particular, the extent to which CISS influences spin polarization or spin coherence in the initial state of spin-correlated radical pairs following charge transfer through a chiral bridge remains an open question. Here, we introduce a quantum sensing scheme to measure directly the hypothesized spin polarization in radical pairs using shallow nitrogen-vacancy (NV) centers in diamond at the single- to few-molecule level. Importantly, we highlight the perturbative nature of the electron spin-spin dipolar coupling within the radical pair, and demonstrate how Lee-Goldburg decoupling can preserve spin polarization in D-B-A molecules for enantioselective detection by a single NV center. The proposed measurements will provide fresh insight into spin selectivity in electron transfer reactions., Comment: 7 pages and 4 pages appendix including an extensive description of the initial spin state of photo-generated radical pairs

Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen--vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface defects facilitate detection of the minute magnetic fields generated by nuclear or electron spins outside of the diamond crystal, such as those in chemisorbed and physisorbed molecules. However, the promise of NV centers is hindered by a severe degradation of critical sensor properties, namely charge stability and spin coherence, near surfaces (< ca. 10 nm deep). Moreover, applications in the chemical sciences require methods for covalent bonding of target molecules to diamond with robust control over density, orientation, and binding configuration. This forward-looking Review provides a survey of the rapidly converging fields of diamond surface science and NV-center physics, highlighting their combined potential for quantum sensing of molecules. We outline the diamond surface properties that are advantageous for NV-sensing applications, and discuss strategies to mitigate deleterious effects while simultaneously providing avenues for chemical attachment. Finally, we present an outlook on emerging applications in which the unprecedented sensitivity and spatial resolution of NV-based sensing could provide unique insight into chemically functionalized surfaces at the single-molecule level., Comment: Review paper, 36 pages

Nuclear magnetic resonance (NMR) imaging with shallow nitrogen-vacancy (NV) centers in diamond offers an exciting route toward sensitive and localized chemical characterization at the nanoscale. Remarkable progress has been made to combat the degradation in coherence time and stability suffered by near-surface NV centers using suitable chemical surface termination. However, approaches that also enable robust control over adsorbed molecule density, orientation, and binding configuration are needed. We demonstrate a diamond surface preparation for mixed nitrogen- and oxygen-termination that simultaneously improves NV center coherence times for emitters <10-nm-deep and enables direct and recyclable chemical functionalization via amine-reactive crosslinking. Using this approach, we probe single NV centers embedded in nanopillar waveguides to perform $^{19}\mathrm{F}$ NMR sensing of covalently bound trifluoromethyl tags in the ca. 50-100 molecule regime. This work signifies an important step toward nuclear spin localization and structure interrogation at the single-molecule level., Comment: 21 pages and 16 pages supporting information

High-finesse, open-geometry microcavities have recently emerged as a versatile tool for enhancing interactions between photons and material systems, with a range of applications in quantum optics and quantum information science. However, mechanical vibrations pose a considerable challenge to their operation within a closed-cycle cryostat, particularly when spatial tunability and free-space optical access are required. Here, we present the design and characterization of a system that can achieve $\sim$16 pm-rms passive mechanical stability between two high-finesse mirrors while permitting both three-dimensional positioning of the cavity mode and free-space confocal imaging. The design relies on two cascaded vibration isolation stages connected by leaf springs that decouple axial and lateral motion, and incorporates tuned-mass and magnetic damping. Furthermore, we present a technique for quantifying cavity length displacements similar to or larger than the cavity linewidth, allowing in-situ measurement of vibrations with and without active feedback. Our results facilitate operation of a tunable, high-finesse cavity within a closed-cycle cryostat, representing an enabling technology for cavity coupling to a variety of solid-state systems., Comment: Authors Yannik Fontana and Rigel Zifkin contributed equally

Coherent interfaces between optical photons and long-lived matter qubits form a key resource for a broad range of quantum technologies. Cavity quantum electrodynamics (cQED) offers a route to achieve such an interface by enhancing interactions between cavity-confined photons and individual emitters. Over the last two decades, a promising new class of emitters based on defect centers in diamond have emerged, combining long spin coherence times with atom-like optical transitions. More recently, advances in optical resonator technologies have made it feasible to realize cQED in diamond. This article reviews progress towards coupling color centers in diamond to optical resonators, focusing on approaches compatible with quantum networks. We consider the challenges for cQED with solid-state emitters and introduce the relevant properties of diamond defect centers before examining two qualitatively different resonator designs: micron-scale Fabry-Perot cavities and diamond nanophotonic cavities. For each approach, we examine the underlying theory and fabrication, discuss strengths and outstanding challenges, and highlight state-of-the-art experiments., Comment: \copyright 2020 Optical Society of America. One print or electronic copy may be made for personal use only. Systematic reproduction and distribution, duplication of any material in this paper for a fee or for commercial purposes, or modifications of the content of this paper are prohibited

The nitrogen-vacancy center in diamond has been explored extensively as a light-matter interface for quantum information applications, however it is limited by low coherent photon emission and spectral instability. Here, we present a promising interface based on an alternate defect with superior optical properties (the germanium-vacancy) coupled to a finesse $\approx11{,}000$ fiber cavity, resulting in a $31^{+11}_{-15}$-fold increase in the spectral density of emission. This work sets the stage for cryogenic experiments, where we predict a measurable increase in the spontaneous emission rate., Comment: 7 pages, 6 figures

Open Fabry-Perot microcavities represent a promising route for achieving a quantum electrodynamics (cavity-QED) platform with diamond-based emitters. In particular, they offer the opportunity to introduce high purity, minimally fabricated material into a tunable, high quality factor optical resonator. Here, we demonstrate a fiber-based microcavity incorporating a thick (> 10 {\mu}m) diamond membrane with a finesse of 17,000, corresponding to a quality factor Q ~ $10^6$. Such minimally fabricated, thick samples can contain optically stable emitters similar to those found in bulk diamond. We observe modified microcavity spectra in the presence of the membrane, and develop analytic and numerical models to describe the effect of the membrane on cavity modes, including loss and coupling to higher-order transverse modes. We estimate that a Purcell enhancement of approximately 20 should be possible for emitters within the diamond in this device, and provide evidence that better diamond surface treatments and mirror coatings could increase this value to 200 in a realistic system., Comment: 12 pages, 7 figures

We demonstrate an approach, based on plasmonic apertures and gratings, to enhance the radiative decay rate of single NV centers in diamond, while simultaneously improving their collection efficiency. Our structures are based on metallic resonators formed by surrounding sub-wavelength diamond nanoposts with a silver film, which can enhance the spontaneous emission rate of an embedded NV center. However, the collection efficiency of emitted photons remains low due to losses to surface plasmons and reflections at the diamond-air interface. In this work, we mitigate photon losses into these channels by incorporating grating structures into the plasmonic cavity system.