Electron Spin Polarization and Rectification Driven by Chiral Perylene Diimide-Based Nanodonuts

Chih Hung Ko; Qirong Zhu; George Bullard; Francesco Tassinari; Mitsuhiko Morisue; Ron Naaman; Michael J. Therien

doi:10.1021/acs.jpclett.3c02722

Electron Spin Polarization and Rectification Driven by Chiral Perylene Diimide-Based Nanodonuts

Chih Hung Ko, Qirong Zhu, George Bullard, Francesco Tassinari, Mitsuhiko Morisue, Ron Naaman^*, Michael J. Therien^*

^*Corresponding author for this work

Department of Chemical and Biological Physics

Research output: Contribution to journal › Article › peer-review

4 Citations (Scopus)

Abstract

The chirality-induced spin selectivity (CISS) effect allows thin-film layers of chiral conjugated molecules to function as spin filters at ambient temperature. Through solvent-modulated dropcasting of chiral l- and d-perylene diimide (PDI) monomeric building blocks, two types of aggregate morphologies, nanofibers and nanodonuts, may be realized. Spin-diode behavior is evidenced in the nanodonut structures. Stacked PDI units, which form the conjugated core of these nanostructures, dominate the nanodonut-Au electrode contact; in contrast, the AFM tip contacts largely the high-resistance solubilizing alkyl chains of the chiral monomers that form these nanodonuts. Current-voltage responses of the nanodonuts, measured by magnetic conductive AFM (mC-AFM), demonstrate substantial spin polarizations as well as spin current rectification ratios (>10) that exceed the magnitudes of those determined to date for other chiral nanoscale systems. These results underscore the potential for chiral nanostructures, featuring asymmetric molecular junctions, to enable CISS-based nanoscale spin current rectifiers.

Original language	English
Pages (from-to)	10271-10277
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	45
DOIs	https://doi.org/10.1021/acs.jpclett.3c02722
Publication status	Published - 16 Nov 2023

Funding

C.-H.K., G.B., and M.J.T. are grateful to the National Science Foundation (CHE-1925690) and the Air Force Office of Scientific Research Multidisciplinary University Research Initiative (MURI) Program (FA9550-23-1-0368) for funding this research. Q.Z., F.T., and R.N. acknowledge the Air Force Office of Scientific Research (FA9550-21-1-0418) and the United States Department of Energy (ER46430) for research support. C.-H.K. is grateful to Duke University for a Graduate Program Nanoscience Fellowship, and G. B. gratefully acknowledges the Fitzpatrick Institute of Photonics at Duke University for a John T. Chambers Scholars Award. M.J.T. is indebted to the John Simon Guggenheim Memorial Foundation for a research fellowship. Publisher Copyright: © 2023 American Chemical Society

All Science Journal Classification (ASJC) codes

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.3c02722

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title = "Electron Spin Polarization and Rectification Driven by Chiral Perylene Diimide-Based Nanodonuts",

abstract = "The chirality-induced spin selectivity (CISS) effect allows thin-film layers of chiral conjugated molecules to function as spin filters at ambient temperature. Through solvent-modulated dropcasting of chiral l- and d-perylene diimide (PDI) monomeric building blocks, two types of aggregate morphologies, nanofibers and nanodonuts, may be realized. Spin-diode behavior is evidenced in the nanodonut structures. Stacked PDI units, which form the conjugated core of these nanostructures, dominate the nanodonut-Au electrode contact; in contrast, the AFM tip contacts largely the high-resistance solubilizing alkyl chains of the chiral monomers that form these nanodonuts. Current-voltage responses of the nanodonuts, measured by magnetic conductive AFM (mC-AFM), demonstrate substantial spin polarizations as well as spin current rectification ratios (>10) that exceed the magnitudes of those determined to date for other chiral nanoscale systems. These results underscore the potential for chiral nanostructures, featuring asymmetric molecular junctions, to enable CISS-based nanoscale spin current rectifiers.",

author = "Ko, {Chih Hung} and Qirong Zhu and George Bullard and Francesco Tassinari and Mitsuhiko Morisue and Ron Naaman and Therien, {Michael J.}",

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T1 - Electron Spin Polarization and Rectification Driven by Chiral Perylene Diimide-Based Nanodonuts

AU - Ko, Chih Hung

AU - Zhu, Qirong

AU - Bullard, George

AU - Tassinari, Francesco

AU - Morisue, Mitsuhiko

AU - Naaman, Ron

AU - Therien, Michael J.

PY - 2023/11/16

Y1 - 2023/11/16

N2 - The chirality-induced spin selectivity (CISS) effect allows thin-film layers of chiral conjugated molecules to function as spin filters at ambient temperature. Through solvent-modulated dropcasting of chiral l- and d-perylene diimide (PDI) monomeric building blocks, two types of aggregate morphologies, nanofibers and nanodonuts, may be realized. Spin-diode behavior is evidenced in the nanodonut structures. Stacked PDI units, which form the conjugated core of these nanostructures, dominate the nanodonut-Au electrode contact; in contrast, the AFM tip contacts largely the high-resistance solubilizing alkyl chains of the chiral monomers that form these nanodonuts. Current-voltage responses of the nanodonuts, measured by magnetic conductive AFM (mC-AFM), demonstrate substantial spin polarizations as well as spin current rectification ratios (>10) that exceed the magnitudes of those determined to date for other chiral nanoscale systems. These results underscore the potential for chiral nanostructures, featuring asymmetric molecular junctions, to enable CISS-based nanoscale spin current rectifiers.

AB - The chirality-induced spin selectivity (CISS) effect allows thin-film layers of chiral conjugated molecules to function as spin filters at ambient temperature. Through solvent-modulated dropcasting of chiral l- and d-perylene diimide (PDI) monomeric building blocks, two types of aggregate morphologies, nanofibers and nanodonuts, may be realized. Spin-diode behavior is evidenced in the nanodonut structures. Stacked PDI units, which form the conjugated core of these nanostructures, dominate the nanodonut-Au electrode contact; in contrast, the AFM tip contacts largely the high-resistance solubilizing alkyl chains of the chiral monomers that form these nanodonuts. Current-voltage responses of the nanodonuts, measured by magnetic conductive AFM (mC-AFM), demonstrate substantial spin polarizations as well as spin current rectification ratios (>10) that exceed the magnitudes of those determined to date for other chiral nanoscale systems. These results underscore the potential for chiral nanostructures, featuring asymmetric molecular junctions, to enable CISS-based nanoscale spin current rectifiers.

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JF - Journal of Physical Chemistry Letters

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ER -

Electron Spin Polarization and Rectification Driven by Chiral Perylene Diimide-Based Nanodonuts

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