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Nanoscale molecular rectifiers

Nature Reviews Chemistry volume 7, pages 106–122 (2023)Cite this article

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Abstract

The use of molecules bridged between two electrodes as a stable rectifier is an important goal in molecular electronics. Until recently, however, and despite extensive experimental and theoretical work, many aspects of our fundamental understanding and practical challenges have remained unresolved and prevented the realization of such devices. Recent advances in custom-designed molecular systems with rectification ratios exceeding 105 have now made these systems potentially competitive with existing silicon-based devices. Here, we provide an overview and critical analysis of recent progress in molecular rectification within single molecules, self-assembled monolayers, molecular multilayers, heterostructures, and metal–organic frameworks and coordination polymers. Examples of conceptually important and best-performing systems are discussed, alongside their rectification mechanisms. We present an outlook for the field, as well as prospects for the commercialization of molecular rectifiers.

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Fig. 1: An example of a single-molecule rectifier.
Fig. 2: Examples of SAM-based molecular rectifiers.
Fig. 3: Schematic illustration of representative bilayer and multilayer molecular junctions.
Fig. 4: Examples of heterostructured molecular junctions for studying nanoscale rectification.
Fig. 5: Examples of MOF-based molecular junctions exhibiting current rectification characteristics.
Fig. 6: An example of a SURMOF-based rectifier.

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Acknowledgements

P.C.M. acknowledges the Department of Science and Technology for a start-up research grant (SRG/2019/000391), an initiation and special grant from IIT Kanpur (IITK/CHM/2019044), and the Council of Scientific & Industrial Research (CSIR, sanctioned NO.:01(3049)/21/EMR-II), New Delhi, India.

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Authors and Affiliations

  1. Department of Chemistry, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh, India

    Ritu Gupta, Anurag Pritam & Prakash Chandra Mondal

  2. School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram, Thiruvananthapuram, Kerala, India

    Jerry A. Fereiro

  3. Laboratoire Photonique Numérique et Nanosciences, UMR 5298, Université de Bordeaux, Talence, France

    Akhtar Bayat

  4. Angewandte Physikalische Chemie, Universität Heidelberg, Heidelberg, Germany

    Michael Zharnikov

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Contributions

R.G., J.A.F., A.B., A.P. and P.C.M. researched data for the article. R.G., J.A.F., M.Z. and P.C.M. contributed substantially to discussion of the content. R.G., J.A.F., M.Z. and P.C.M. wrote the article. M.Z. and P.C.M. reviewed and/or edited the manuscript before submission.

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Glossary

Aviram–Ratner model

A model involving two conjugated moieties — a donor (D) and an acceptor (A) — connected via an insulating (non-conjugated) moiety (σ bridge).

Atomic force microscopy

(AFM). A technique widely used to study the morphology and structure of surfaces with nanoscale precision.

Barrier height

The potential difference between the Fermi level of the electrical contact and the band edge or frontier molecular orbital (either HOMO or LUMO) populated by electrons or holes.

Break junctions

A tool to investigate the electrical properties of single molecules and small molecular assemblies by creating a nanometre-sized gap between two metal electrodes, bridged by a molecule or molecules.

Conductive-probe atomic force microscopy

(CP-AFM). A technique capable of mapping the local variation in electrical conductivity and topography of the sample at the nanoscale level.

Fermi level

The highest energy level occupied by electrons in a metal at 0 K, the density of states of which determines the thermal and electrical conductivity of a particular material.

Inelastic electron tunnelling spectroscopy

A technique to investigate the vibrational modes of molecules in which an oxide layer with molecules adsorbed on it is placed between two metal electrodes and subjected to a variable bias.

Mechanically controlled break junction

A tool with which to examine the mechanical and electrical properties of single molecules.

Rectification ratio

Figure of merit for the effectiveness of rectification, usually defined as the ratio of the currents measured at the bias voltages of the same magnitude but reverse polarities.

Scanning tunnelling microscopy

(STM). A technique widely used to study the morphology and structure of surfaces with atomic and nanoscale precision that relies on quantum tunnelling between the conducting tip and sample surface.

Sequential tunnelling

A sequence of tunnelling steps of charge carriers from an electrode across the molecule to the other electrode, which differs from single-step tunnelling in that the tunnelling happens coherently from one electrode to the other with the molecule serving as a tunnelling barrier.

Work function

The minimum energy (usually in electronvolts) required to remove an electron from the bulk of a given material to a point in the vacuum immediately outside the material surface.

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Gupta, R., Fereiro, J.A., Bayat, A. et al. Nanoscale molecular rectifiers. Nat Rev Chem 7, 106–122 (2023). https://doi.org/10.1038/s41570-022-00457-8

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