ja9b06142_si_001.pdf (2.69 MB)
Low-Resistance Molecular Wires Propagate Spin-Polarized Currents
journal contribution
posted on 2019-09-04, 12:33 authored by George Bullard, Francesco Tassinari, Chih-Hung Ko, Amit Kumar Mondal, Ruobing Wang, Suryakant Mishra, Ron Naaman, Michael J. TherienSpin based properties,
applications, and devices are typically
related to inorganic ferromagnetic materials. The development of organic
materials for spintronic applications has long been encumbered by
its reliance on ferromagnetic electrodes for polarized spin injection.
The discovery of the chirality-induced spin selectivity (CISS) effect,
in which chiral organic molecules serve as spin filters, defines a
marked departure from this paradigm because it exploits soft materials,
operates at ambient temperature, and eliminates the need for a magnetic
electrode. To date, the CISS effect has been explored exclusively
in molecular insulators. Here we combine chiral molecules, which serve
as spin filters, with molecular wires that despite not being chiral,
function to preserve spin polarization. Self-assembled monolayers
(SAMs) of right-handed helical (l-proline)8 (Pro8) and corresponding peptides, N-terminal conjugated
to (porphinato)zinc or meso-to-meso ethyne-bridged (porphinato)zinc
structures (Pro8PZnn), were interrogated via magnetic conducting atomic force microscopy
(mC-AFM), spin-dependent electrochemistry, and spin Hall devices that
measure the spin polarizability that accompanies the charge polarization.
These data show that chiral molecules are not required to transmit
spin-polarized currents made possible by the CISS mechanism. Measured
Hall voltages for Pro8PZn1–3 substantially exceed that determined for the Pro8 control
and increase dramatically as the conjugation length of the achiral PZnn component increases; mC-AFM
data underscore that measured spin selectivities increase with an
increasing Pro8PZn1–3 N-terminal
conjugation. Because of these effects, spin-dependent electrochemical
data demonstrate that spin-polarized currents, which trace their genesis
to the chiral Pro8 moiety, propagate with
no apparent dephasing over the augmented Pro8PZnn length scales, showing that spin
currents may be transmitted over molecular distances that greatly
exceed the length of the chiral moiety that makes possible the CISS
effect.