Graphene–molecule–graphene single-molecule junctions to detect electronic reactions at the molecular scale

Chen Yang, Caiyao Yang, Yilin Guo, Jianfei Feng, Xuefeng Guo

Published: 2023-04-11 DOI: 10.1038/s41596-023-00822-x

Graphene-molecule junctions

Single-molecule detection

CMOS compatibility

Electron-beam lithography

Inelastic electron tunneling

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Supplementary information

Supplementary Information

Supplementary Note and Figs. 1–12.

Reporting Summary

Preparation of single-cell suspensions of mouse glomeruli for high-throughput analysis

cfSNV: a software tool for the sensitive detection of somatic mutations from cell-free DNA

Anaerobic cryoEM protocols for air-sensitive nitrogenase proteins

Engineering megabase-sized genomic deletions with MACHETE (Molecular Alteration of Chromosomes with Engineered Tandem Elements)

Genome-wide pooled CRISPR screening in neurospheres

Neural cell isolation from adult macaques for high-throughput analyses and neurosphere cultures

Design and fabrication of wearable electronic textiles using twisted fiber-based threads

Nacre-inspired underwater superoleophobic films with high transparency and mechanical robustness

Quantification of organelle contact sites by split-GFP-based contact site sensors (SPLICS) in living cells

Scanorama: integrating large and diverse single-cell transcriptomic datasets

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Supplementary information

Coontz, R. & Hanson, B. Not so simple. Science 305, 957 (2004).
Barkai, E., Jung, Y. J. & Silbey, R. Theory of single-molecule spectroscopy: beyond the ensemble average. Annu. Rev. Phys. Chem. 55, 457–507 (2004).
Zrimsek, A. B. et al. Single-molecule chemistry with surface- and tip-enhanced Raman spectroscopy. Chem. Rev. 117, 7583–7613 (2017).
Lu, H. P., Xun, L. & Xie, X. S. Single-molecule enzymatic dynamics. Science 282, 1877–1882 (1998).
Liu, C. et al. Single polymer growth dynamics. Science 358, 352–355 (2017).
Florin, E. L., Moy, V. T. & Gaub, H. E. Adhesion forces between individual ligand-receptor pairs. Science 264, 415–417 (1994).
Li, Y., Yang, C. & Guo, X. Single-molecule electrical detection: a promising route toward the fundamental limits of chemistry and life science. Acc. Chem. Res. 53, 159–169 (2020).
Xin, N. et al. Concepts in the design and engineering of single-molecule electronic devices. Nat. Rev. Phys. 1, 211–230 (2019).
Venkatesan, B. M. & Bashir, R. Nanopore sensors for nucleic acid analysis. Nat. Nanotechnol. 6, 615–624 (2011).
Aviram, A. & Ratner, M. A. Molecular rectifiers. Chem. Phys. Lett. 29, 277–283 (1974).
Xiang, D., Wang, X., Jia, C., Lee, T. & Guo, X. Molecular-scale electronics: from concept to function. Chem. Rev. 116, 4318–4440 (2016).
Li, T., Hu, W. & Zhu, D. Nanogap electrodes. Adv. Mater. 22, 286–300 (2010).
Jia, C. & Guo, X. Molecule-electrode interfaces in molecular electronic devices. Chem. Soc. Rev. 42, 5642–5660 (2013).
Su, T. A., Neupane, M., Steigerwald, M. L., Venkataraman, L. & Nuckolls, C. Chemical principles of single-molecule electronics. Nat. Rev. Mater. 1, 16002 (2016).
Xu, B. & Tao, N. Measurement of single-molecule resistance by repeated formation of molecular junctions. Science 301, 1221–1223 (2003).
Venkataraman, L., Klare, J. E., Nuckolls, C., Hybertsen, M. S. & Steigerwald, M. L. Dependence of single-molecule junction conductance on molecular conformation. Nature 442, 904–907 (2006).
Reed, M. A., Zhou, C., Muller, C. J., Burgin, T. P. & Tour, J. M. Conductance of a molecular junction. Science 278, 252–254 (1997).
Park, H., Lim, A. K. L., Alivisatos, A. P., Park, J. & McEuen, P. L. Fabrication of metallic electrodes with nanometer separation by electromigration. Appl. Phys. Lett. 75, 301–303 (1999).
Park, J. et al. Coulomb blockade and the Kondo effect in single-atom transistors. Nature 417, 722–725 (2002).
Gehring, P. et al. Field-effect control of graphene–fullerene thermoelectric nanodevices. Nano Lett. 17, 7055–7061 (2017).
Burzurí, E. et al. Sequential electron transport and vibrational excitations in an organic molecule coupled to few-layer graphene electrodes. ACS Nano 10, 2521–2527 (2016).
Burzurí, E. et al. Spin-state dependent conductance switching in single molecule-graphene junctions. Nanoscale 10, 7905–7911 (2018).
Island, J. O. et al. Fabrication of hybrid molecular devices using multi-layer graphene break junctions. J. Phys. Condens. Matter 26, 474205 (2014).
Prins, F. et al. Room-temperature gating of molecular junctions using few-layer graphene nanogap electrodes. Nano Lett. 11, 4607–4611 (2011).
Lau, C. S. et al. Redox-dependent Franck–Condon blockade and avalanche transport in a graphene-fullerene single-molecule transistor. Nano Lett. 16, 170–176 (2015).
Limburg, B. et al. Anchor groups for graphene-porphyrin single-molecule transistors. Adv. Funct. Mater. 28, 1803629 (2018).
Mol, J. A. et al. Graphene-porphyrin single-molecule transistors. Nanoscale 7, 13181–13185 (2015).
Thomas, J. O. et al. Understanding resonant charge transport through weakly coupled single-molecule junctions. Nat. Commun. 10, 4628 (2019).
Pei, T. et al. Exchange-induced spin polarization in a single magnetic molecule junction. Nat. Commun. 13, 4506 (2022).
Zhao, S. et al. Charge transport through single-molecule bilayer-graphene junctions with atomic thickness. Chem. Sci. 13, 5854–5859 (2022).
Cao, Y. et al. Building high-throughput molecular junctions using indented graphene point contacts. Angew. Chem. Int. Ed. Engl. 51, 12228–12232 (2012).
Gu, C. H., Su, D. K., Jia, C. C., Ren, S. Z. & Guo, X. F. Building nanogapped graphene electrode arrays by electroburning. RSC Adv. 8, 6814–6819 (2018).
Guo, X. et al. Covalently bridging gaps in single-walled carbon nanotubes with conducting molecules. Science 311, 356–359 (2006).
Jia, C. et al. Covalently bonded single-molecule junctions with stable and reversible photoswitched conductivity. Science 352, 1443–1445 (2016).
Jia, C., Ma, B., Xin, N. & Guo, X. Carbon electrode-molecule junctions: a reliable platform for molecular electronics. Acc. Chem. Res. 48, 2565–2575 (2015).
Xin, N. et al. Stereoelectronic effect-induced conductance switching in aromatic chain single-molecule junctions. Nano Lett. 17, 856–861 (2017).
Meng, L. et al. Atomically precise engineering of single-molecule stereoelectronic effect. Angew. Chem. Int. Ed. Engl. 60, 12274–12278 (2021).
Yang, C. et al. Complete deciphering of the dynamic stereostructures of a single aggregation-induced emission molecule. Matter 5, 1224–1234 (2022).
Wen, H. et al. Complex formation dynamics in a single-molecule electronic device. Sci. Adv. 2, e1601113 (2016).
Zhou, C. et al. Direct observation of single-molecule hydrogen-bond dynamics with single-bond resolution. Nat. Commun. 9, 807 (2018).
Liu, Z. et al. A single-molecule electrical approach for amino acid detection and chirality recognition. Sci. Adv. 7, eabe4365 (2021).
Chen, S. et al. Real-time observation of the dynamics of an individual rotaxane molecular shuttle using a single-molecule junction. Chem 8, 243–252 (2022).
Guo, Y., Yang, C., Jia, C. & Guo, X. Accurate single-molecule indicator of solvent effects. JACS Au 1, 2271–2279 (2021).
Gu, C. et al. Label-free dynamic detection of single-molecule nucleophilic-substitution reactions. Nano Lett. 18, 4156–4162 (2018).
Yang, C. et al. Single-molecule electrical spectroscopy of organocatalysis. Matter 4, 2874–2885 (2021).
Yang, C. et al. Unveiling the full reaction path of the Suzuki–Miyaura cross-coupling in a single-molecule junction. Nat. Nanotechnol. 16, 1214–1223 (2021).
Yang, C. et al. Electric field-catalyzed single-molecule Diels-Alder reaction dynamics. Sci. Adv. 7, eabf0689 (2021).
Guo, Y. et al. Accurate single-molecule kinetic isotope effects. J. Am. Chem. Soc. 144, 3146–3153 (2022).
Meng, L. et al. Side-group chemical gating via reversible optical and electric control in a single molecule transistor. Nat. Commun. 10, 1450 (2019).
Xin, N. et al. Tuning charge transport in aromatic-ring single-molecule junctions via ionic-liquid gating. Angew. Chem. Int. Ed. Engl. 57, 14026–14031 (2018).
Xin, N. et al. Control of unipolar/ambipolar transport in single‐molecule transistors through interface engineering. Adv. Electron. Mater. 6, 1901237 (2020).
Xin, N. et al. Tunable symmetry-breaking-induced dual functions in stable and photoswitched single-molecule junctions. J. Am. Chem. Soc. 143, 20811–20817 (2021).
Stefani, D. et al. Large conductance variations in a mechanosensitive single-molecule junction. Nano Lett. 18, 5981–5988 (2018).
Vazquez, H. et al. Probing the conductance superposition law in single-molecule circuits with parallel paths. Nat. Nanotechnol. 7, 663–667 (2012).
Greenwald, J. E. et al. Highly nonlinear transport across single-molecule junctions via destructive quantum interference. Nat. Nanotechnol. 16, 313–317 (2020).
Zhang, L. et al. Electrochemical and electrostatic cleavage of alkoxyamines. J. Am. Chem. Soc. 140, 766–774 (2018).
Venkataraman, L. et al. Electronics and chemistry: varying single-molecule junction conductance using chemical substituents. Nano Lett. 7, 502–506 (2007).
Zhang, Y. et al. Distinguishing diketopyrrolopyrrole isomers in single-molecule junctions via reversible stimuli-responsive quantum interference. J. Am. Chem. Soc. 140, 6531–6535 (2018).
Su, T. A., Li, H., Steigerwald, M. L., Venkataraman, L. & Nuckolls, C. Stereoelectronic switching in single-molecule junctions. Nat. Chem. 7, 215–220 (2015).
Huang, S. et al. Identifying single bases in a DNA oligomer with electron tunnelling. Nat. Nanotechnol. 5, 868–873 (2010).
Zhao, Y. et al. Single-molecule spectroscopy of amino acids and peptides by recognition tunnelling. Nat. Nanotechnol. 9, 466–473 (2014).
Zhu, J. et al. Solution-processable carbon nanoelectrodes for single-molecule investigations. J. Am. Chem. Soc. 138, 2905–2908 (2016).
Xu, Q. et al. Single electron transistor with single aromatic ring molecule covalently connected to graphene nanogaps. Nano Lett. 17, 5335–5341 (2017).
Caneva, S. et al. Mechanically controlled quantum interference in graphene break junctions. Nat. Nanotechnol. 13, 1126–1131 (2018).
El Abbassi, M. et al. Robust graphene-based molecular devices. Nat. Nanotechnol. 14, 957–961 (2019).
Gehring, P. et al. Distinguishing lead and molecule states in graphene-based single-electron transistors. ACS Nano 11, 5325–5331 (2017).
Nef, C. et al. High-yield fabrication of nm-size gaps in monolayer CVD graphene. Nanoscale 6, 7249–7254 (2014).
Cully, J. J., Swett, J. L., Willick, K., Baugh, J. & Mol, J. A. Graphene nanogaps for the directed assembly of single-nanoparticle devices. Nanoscale 13, 6513–6520 (2021).
Lau, C. S., Mol, J. A., Warner, J. H. & Briggs, G. A. D. Nanoscale control of graphene electrodes. Phys. Chem. Chem. Phys. 16, 20398–20401 (2014).
Agrawal, S., Raghuveer, M. S., Kroger, R. & Ramanath, G. Electrical current-induced structural changes and chemical functionalization of carbon nanotubes. J. Appl. Phys. 100, 094314 (2006). 21.
Ullmann, K. et al. Single-molecule junctions with epitaxial graphene nanoelectrodes. Nano Lett. 15, 3512–3518 (2015).
Tincu, B. et al. Investigation of plasma-assisted functionalization of pristine single layer graphene. Chem. Phys. Lett. 789, 139330 (2022).
Cao, Y., Dong, S., Liu, S., Liu, Z. & Guo, X. Toward functional molecular devices based on graphene molecule junctions. Angew. Chem. Int. Ed. Engl. 52, 3906–3910 (2013).
Imai-Imada, M. et al. Orbital-resolved visualization of single-molecule photocurrent channels. Nature 603, 829–834 (2022).

Graphene–molecule–graphene single-molecule junctions to detect electronic reactions at the molecular scale

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