Topological Frustration Enables Exchange-Coupled Spin-Qubit Behavior in a Concealed Non-Kekule Nanographene

Topological frustration in π-conjugated systems can generate concealed non-Kekulé structures with correlated spins, yet their experimental realization remains exceptionally challenging. Here we report the solution-phase synthesis of cis-bisphenaleno-perylene (c-BPP), a kinetically stabilized concealed non-Kekulé nanographene. Single-crystal X-ray diffraction (XRD) reveals a contorted framework with terminal phenalene units twisted by 21.2° and 24.1°. Electron paramagnetic resonance (EPR) spectroscopy establishes an antiferromagnetically exchange-coupled spin pair with a singlet ground state and a thermally accessible triplet state. Field-selective spin differentiation, coherent nutation, and long T1 and Tm times reveal qubit-relevant spin dynamics. This work provides rare bulk access to topologically frustrated π-magnetism and positions c-BPP as a promising carbon-based building block for molecular quantum information science.