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Gradual Change between Coherent and Incoherent Tunneling Regimes Induced by Polarizable Halide Substituents in Molecular Tunnel Junctions.

ABSTRACT: This paper describes a gradual transition of charge transport across molecular junctions from coherent to incoherent tunneling by increasing the number and polarizability of halide substituents of phenyl-terminated aliphatic monolayers of the form S(CH₂)₁₀OPhX_n, X = F, Cl, Br, or I; n = 0, 1, 2, 3, or 5. In contrast to earlier work where incoherent tunneling was induced by introducing redox-active groups or increasing the molecular length, we show that increasing the polarizability, while keeping the organization of the monolayer structure unaltered, results in a gradual change in the mechanism of tunneling of charge carriers where the activation energy increased from 23 meV for n = 0 (associated with coherent tunneling) to 257 meV for n = 5 with X = Br (associated with incoherent tunneling). Interestingly, this increase in incoherent tunneling rate with polarizability resulted in an improved molecular diode performance. Our findings suggest an avenue to improve the electronic function of molecular devices by introducing polarizable atoms.

SUBMITTER: Chen X

PROVIDER: S-EPMC11345807 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Gradual Change between Coherent and Incoherent Tunneling Regimes Induced by Polarizable Halide Substituents in Molecular Tunnel Junctions.

Chen Xiaoping X Volkova Ira I Wang Yulong Y Zhang Ziyu Z Nijhuis Christian A CA

Journal of the American Chemical Society 20240808 33

This paper describes a gradual transition of charge transport across molecular junctions from coherent to incoherent tunneling by increasing the number and polarizability of halide substituents of phenyl-terminated aliphatic monolayers of the form S(CH2)10OPhXn, X = F, Cl, Br, or I; n = 0, 1, 2, 3, or 5. In contrast to earlier work where incoherent tunneling was induced by introducing redox-active groups or increasing the molecular length, we show t ...[more]

PMID: 39115108

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Project description:Significance Spintronic devices have become promising candidates for next-generation memory architecture. However, state-of-the-art devices, such as perpendicular magnetic tunnel junctions (MTJs), are still fundamentally constrained by a subnanosecond speed limitation, which has remained a long-lasting scientific obstacle in the ultrafast spintronics field. The highlight of our work is the demonstration of an optospintronic tunnel junction, an all-optical MTJ device which emerges as a new category of integrated photonic–spintronic memory. We demonstrate 1) laser-induced deterministic and efficient writing by an all-optical approach and electrical readout by tunnel magnetoresistance, 2) writing speed within 10 ps, demonstrated by femtosecond-resolved measurements, and 3) integration with state-of-the-art MTJ performance and a complementary metal–oxide–semiconductor-compatible fabrication progress. Perpendicular magnetic tunnel junctions (p-MTJs), as building blocks of spintronic devices, offer substantial potential for next-generation nonvolatile memory applications. However, their performance is fundamentally hindered by a subnanosecond speed limitation, due to spin-polarized-current-based mechanisms. Here, we report an optospintronic tunnel junction (OTJ) device with a picosecond switching speed, ultralow power, high magnetoresistance ratio, high thermal stability, and nonvolatility. This device incorporates an all-optically switchable Gd/Co bilayer coupled to a CoFeB/MgO-based p-MTJ, by subtle tuning of Ruderman–Kittel–Kasuya–Yosida interaction. An all-optical “writing” of the OTJ within 10 ps is experimentally demonstrated by time-resolved measurements. The device shows a reliable resistance “readout” with a relatively high tunnel magnetoresistance of 34.7%, as well as promising scaling toward the nanoscale with ultralow power consumption (<100 fJ for a 50-nm-sized bit). Our proof-of-concept demonstration of OTJ might ultimately pave the way toward a new category of integrated spintronic–photonic memory devices.

Dataset Information

Gradual Change between Coherent and Incoherent Tunneling Regimes Induced by Polarizable Halide Substituents in Molecular Tunnel Junctions.

Publications

Gradual Change between Coherent and Incoherent Tunneling Regimes Induced by Polarizable Halide Substituents in Molecular Tunnel Junctions.

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