Ordered multi-spin assemblies are required for developing solid-state molecule-based spintronics. A linear donor–chromophore–acceptor (D–C–A) molecule was covalently attached inside the 150 nm diam. nanopores of an anodic aluminum oxide (AAO) membrane. Photoexcitation of D–C–A in a 343 mT magnetic field results in sub-nanosecond, two-step electron transfer to yield the spin-correlated radical ion pair (SCRP) 1(D+˙–C–A−˙), which then undergoes radical pair intersystem crossing (RP-ISC) to yield 3(D+˙–C–A−˙). RP-ISC results in S–T0mixing to selectively populate the coherent superposition states |S′〉 and |T′〉. Microwave-induced transitions between these states and the unpopulated |T+1〉 and |T−1〉 states result in spin-polarized time-resolved EPR (TREPR) spectra. The dependence of the electron spin polarization (ESP) phase of the TREPR spectra on the orientation of the AAO membrane pores relative to the externally applied magnetic field is used to determine the overall orientation of the SCRPs within the pores at room temperature.
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