Mapping Out the Nonconjugated Organic Radical Conductors via Chemical or Physical Pathways

Stable, nitroxide-based organic radicals have gained tremendous attention in a wide range of research fields, ranging from solid-state electronics to energy storage devices. While the success of these organics has been their designer flexibility and the processability that can fully potentiate the open-shell chemistry, a significant knowledge gap exists on the solid-state electronics of small-molecular radicals. Herein, we examine the structure-property relationship that governs the solid-state electronics of a model nitroxide and its derivatives by seeking the connection to their well-established, electrolyte-based chemistry. Further, we propose a general strategy of enhancing their solid-state conductivity by systematic humidity control. This study demonstrates an open-shell platform of the device operation and underlying principles thereof, which can potentially be applied in a number of future radical-based electronic devices.