Nuclear magnetic resonance (NMR) spectroscopy is a powerful probe of molecular structure and dynamics but typically requires large spin ensembles. Here, we demonstrate nanoscale NMR detection of fluorinated DNA using individual near-surface nitrogen-vacancy (NV) centers in diamond nanopillar waveguides under ambient conditions. We covalently tether ^19F-labeled oligonucleotides to mixed nitrogen- and oxygen-terminated surfaces, localizing target spins within the nanoscale sensing volume. Probabilistic spin simulations suggest that the measured signals are consistent with those expected from a few molecules and depend strongly on NV-molecule separation, configuration, and local surface heterogeneity. These results establish a framework for NMR of surface-tethered biomolecules and identify key challenges for single-molecule structural elucidation.

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.

High-finesse microcavities offer a platform for compact, high-precision sensing by employing high-reflectivity, low-loss mirrors to create effective optical path lengths that are orders of magnitude larger than the device geometry. Here, we investigate the radiation hardness of Fabry-Pérot microcavities formed from dielectric mirrors deposited on the tips of optical fibers. The microcavities are irradiated under both conventional (∼ 0.1 Gy/s) and ultrahigh (FLASH, ∼ 20 Gy/s) radiotherapy dose rates. Within our measurement sensitivity of ∼ 40 ppm loss, we observe no degradation in the mirror absorption after irradiation with over 300 Gy accumulated dose. This result highlights the excellent radiation hardness of the dielectric mirrors forming the cavities, enabling new optics-based, real-time, in-vivo, tissue-equivalent radiation dosimeters with ∼ 10 micron spatial resolution (our motivation), as well as other applications in high-radiation environments.

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±0.3, and extract coherent coupling rates up to 360±20 MHz. Our results indicate that the GeV defect has favorable optical properties for cavity coupling, with a quantum efficiency of at least 0.34±0.05 and likely much higher.

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.

The long-lived electronic spin of the nitrogen-vacancy (NV) center in diamonds is a promising quantum sensor for detecting nanoscopic magnetic and electric fields in various environments. However, the poor signal-to-noise ratio (SNR) of prevalent optical spin-readout techniques presents a critical challenge in improving measurement sensitivity. Here, we address this limitation by coupling individual NVs to optimized diamond nanopillars, thereby enhancing the collection efficiency of fluorescence. Guided by near-field optical simulations, we predict improved performance for tall (≥5 μm) pillars with tapered sidewalls. This is subsequently verified by fabricating and characterizing a representative set of structures using a newly developed nanofabrication process. We observe increased SNR for optimized devices, owing to improved emission collimation and directionality. Promisingly, these devices are compatible with low-numerical-aperture collection optics and a reduced tip radius, reducing experimental overhead and facilitating improved spatial resolution for scanning applications.

We present a simple, continuous, cavity-enhanced optical absorption measurement technique based on high-bandwidth Pound-Drever-Hall (PDH) sideband locking. The technique provides a resonant amplitude quadrature readout that can be mapped onto the cavity's internal loss rate and is naturally compatible with weak probe beams. With a proof-of-concept 5-cm-long Fabry-Perot cavity, we measure an absorption sensitivity ∼10-10cm-1/Hz from 30 kHz to 1 MHz, and a minimum value of 6.6×10-11cm-1/Hz at 100 kHz, with 38 µW collected from the cavity's circulating power.

A diamond nanopillar with a single nitrogen-vacancy (NV) center at the apex can serve as a promising quantum sensor. Our work is focused on improving the photon collection efficiency to achieve higher sensitivity.

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.

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 <10 nm-deep emitters and enables direct and recyclable chemical functionalization via amine-reactive cross-linking. Using this approach, we probe single NV centers embedded in nanopillar waveguides to perform 19F NMR sensing of covalently bound fluorinated molecules with detection on the order of 100 molecules. This work signifies an important step toward nuclear spin localization and structure interrogation at the single-molecule level.

We report on the detailed spectroscopic investigation of a deeply implanted Germanium vacancy centers in diamond at cryogenic temperatures and using a resonant cross-polarization excitation scheme.

We present a simple, continuous, cavity-enhanced optical absorption measurement technique based on high-bandwidth Pound-Drever-Hall (PDH) sideband locking. The technique provides a resonant amplitude quadrature readout that can be mapped onto the cavity's internal loss rate, and is naturally compatible with weak probe beams. With a proof-of-concept 5-cm-long Fabry-Perot cavity, we measure an absorption sensitivity of $6.6 \times 10^{-11} ~\text{cm}^{-1}/\sqrt{\text{Hz}}$ at 100 kHz (roughly the cavity bandwidth) and $\sim 10^{-10}~\text{cm}^{-1}/\sqrt{\text{Hz}}$ from 30 kHz to 1 MHz, with $38~\mu$W collected from the cavity's circulating power.

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 ∼16 pm-rms passive mechanical stability between two high-finesse mirrors with 34% duty cycle 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 for the 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.

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 alternative defect with superior optical properties (the germanium-vacancy) coupled to a finesse-11000 fiber cavity, resulting in a 31(-15)(+11)-fold increase in the spectral density of zero-phonon-line emission. This work sets the stage for cryogenic experiments, where we predict a measurable increase in the spontaneous emission rate.

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 has 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: micrometer-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.

Fiber-based optical microcavities exhibit high quality factor and low mode volume resonances that make them attractive for coupling light to individual atoms or other microscopic systems. Moreover, their low mass should lead to excellent mechanical response up to high frequencies, opening the possibility for high bandwidth stabilization of the cavity length. Here, we demonstrate a locking bandwidth of 44 kHz achieved using a simple, compact design that exploits these properties. Owing to the simplicity of fiber feedthroughs and lack of free-space alignment, this design is inherently compatible with vacuum and cryogenic environments. We measure the transfer function of the feedback circuit (closed-loop) and the cavity mount itself (open-loop), which, combined with simulations of the mechanical response of our device, provide insight into underlying limitations of the design as well as further improvements that can be made.

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.