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Dynamic Nuclear Polarization (DNP) has revolutionized the field of solid-state NMR spectroscopy by significantly enhancing the sensitivity of nuclear magnetic resonance experiments. Conventionally, cross effect DNP relies on biradicals to transfer polarization from coupled electron spins to nearby nuclear spins and subsequent relay to target nuclei via spin diffusion mechanism. However, the direct transfer of polarization to distant nuclei remains a significant challenge, limiting its applicability in various contexts. In this work, we propose a novel biradical design concept that involves a very strong electron-electron coupling, with a magnitude of hundreds of MHz, which enables efficient direct polarization transfer from electron spins to nuclear spins over much longer distances, exceeding 2.0 nm. We discuss the potential of this tailored biradicals in scenarios where conventional spin diffusion mechanisms are inefficient or when direct nuclear spin sensing through electron spin interactions is desired. Our study presents a promising avenue for expanding the scope of cross effect DNP in solid-state NMR spectroscopy and opens new opportunities for investigating a wide range of biological and material systems. Our research also provides insight into the DNP buildup time of commercially available biradicals. |
