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Quantum sensors have notably advanced high-sensitivity magnetic field detection. Here, we report quantum sensors constructed from polarized spin-triplet electrons in photoexcited organic chromophores, specifically focusing on pentacene-doped para-terphenyl (${\approx}$0.1%). We demonstrate essential quantum sensing properties at room temperature: electronic optical polarization and state-dependent fluorescence contrast, by leveraging differential pumping and relaxation rates between triplet and ground states. We measure high optically detected magnetic resonance (ODMR) contrast ${\approx}16.8\%$ of the triplet states at room temperature, along with long coherence times under spin echo and CPMG sequences, $T_2{=}2.7\mu$s and $T_2^{DD}{=}18.4\mu$s respectively, limited only by the triplet lifetimes. The material offers several advantages for quantum sensing, including the ability to grow large ($cm$-scale) crystals at low cost, the absence of paramagnetic impurities, and the diamagnetism of electronic states used for sensing when not optically illuminated. Utilizing pentacene as a representative of a broader class of spin triplet-polarizable organic molecules, this study highlights new potential for quantum sensing in chemical systems.

We present a novel method for fabricating highly customizable three-dimensional structures hosting quantum sensors based on Nitrogen Vacancy (NV) centers using two-photon polymerization. This approach overcomes challenges associated with structuring traditional single-crystal quantum sensing platforms and enables the creation of complex, fully three-dimensional, sensor assemblies with sub-microscale resolutions (down to 400 nm) and large fields of view (>1 mm). By embedding NV center-containing nanoparticles in exemplary structures, we demonstrate high sensitivity optical sensing of temperature and magnetic fields at the microscale. Our work showcases the potential for integrating quantum sensors with advanced manufacturing techniques, facilitating the incorporation of sensors into existing microfluidic and electronic platforms, and opening new avenues for widespread utilization of quantum sensors in various applications.

C-H bond activation enables the facile synthesis of new chemicals. While C-H activation in short-chain alkanes has been widely investigated, it remains largely unexplored for long-chain organic molecules. Here, we report light-driven C-H activation in complex organic materials mediated by 2D transition metal dichalcogenides (TMDCs) and the resultant solid-state synthesis of luminescent carbon dots in a spatially-resolved fashion. We unravel the efficient H adsorption and a lowered energy barrier of C-C coupling mediated by 2D TMDCs to promote C-H activation. Our results shed light on 2D materials for C-H activation in organic compounds for applications in organic chemistry, environmental remediation, and photonic materials.

Rapid injection of spin polarization into an ensemble of nuclear spins is a problem of broad interest, spanning dynamic nuclear polarization (DNP) to quantum information science. We report on a strategy to boost the spin injection rate by exploiting electrons that can be rapidly polarized via high-power optical pumping. We demonstrate this in a model system of Nitrogen Vacancy center electrons injecting polarization into a bath of 13C nuclei in diamond. We deliver >20W of continuous, nearly isotropic, optical power to the sample, constituting a substantially higher power than in previous experiments. Through a spin-ratchet polarization transfer mechanism, we show boosts in spin injection rates by over two orders of magnitude. Our experiments elucidate bottlenecks in the DNP process caused by rates of electron polarization, polarization transfer to proximal nuclei, and spin diffusion. This work demonstrates opportunities for rapid spin injection employing non-thermally generated electron polarization, and has relevance to a broad class of experimental systems including in DNP, quantum sensing, and spin-based MASERs., Comment: 8 pages, 8 figures. SI: 3 pages, 4 figures