Issue 77, 2013

Controlling the orientation of spin-correlated radical pairs by covalent linkage to nanoporous anodic aluminum oxide membranes

Abstract

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–T0 mixing 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.

Graphical abstract: Controlling the orientation of spin-correlated radical pairs by covalent linkage to nanoporous anodic aluminum oxide membranes

Supplementary files

Article information

Article type
Communication
Submitted
08 Jul 2013
Accepted
02 Aug 2013
First published
05 Aug 2013

Chem. Commun., 2013,49, 8614-8616

Controlling the orientation of spin-correlated radical pairs by covalent linkage to nanoporous anodic aluminum oxide membranes

H. Chen, D. M. Gardner, R. Carmieli and M. R. Wasielewski, Chem. Commun., 2013, 49, 8614 DOI: 10.1039/C3CC45129A

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