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Markussen, T., Jin, C. Thygesen, K. S. Quantitatively accurate calculations of conductance and thermopower of molecular junctions. , 2394–2402 (2013).

Venkataraman, L., Klare, J. E., Nuckolls, C., Hybertsen, M. S. Steigerwald, M. L. Dependence of single-molecule junction conductance on molecular conformation. , 904–907 (2006).

Park, Y. S. et al. Contact chemistry and single-molecule conductance: a comparison of phosphines, methyl sulfides, and amines. . , 15768–15769 (2007).

Kim, T., Vázquez, H., Hybertsen, M. S. Venkataraman, L. Conductance of molecular junctions formed with silver electrodes. . , 3358–3364 (2013).

Meisner, J. S. et al. Importance of direct metal− coupling in electronic transport through conjugated single-molecule junctions. . , 20440–20445 (2012).

Li, H. et al. Silver makes better electrical contacts to thiol-terminated silanes than gold. . , 14145–14148 (2017).

G.C.S. and M.H.G. received funding from the Danish Council for Independent Research | Natural Sciences and the Carlsberg Foundation. We thank the National Science Foundation (NSF) for the support of experimental studies under grant no. CHE-1404922 (Ha.L.) and Columbia University’s Research Initiatives in Science and Engineering. Y.C., Z.S., T.L. and S.X. are sponsored by the National Natural Science Foundation of China (grant nos 21473113 and 51502173), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning (no. 2013-57), the “Shuguang Program” supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission (14SG40), the Program of Shanghai Academic/Technology Research Leader (no. 16XD1402700), the National Natural Science Foundation of Shanghai (no. 15ZR1431100), the Ministry of Education of China (PCSIRT_16R49) and the International Joint Laboratory of Resource Chemistry (IJLRC). T.A.S. was supported by an NSF Graduate Research Fellowship under grant no. 11-44155. We thank B. Fowler for mass spectrometry characterization. Single-crystal X-ray diffraction was performed at the Shared Materials Characterization Laboratory (SMCL) at Columbia University. Use of the SMCL was made possible by funding from Columbia University.

Present address: Department of Chemistry, Columbia University, New York, NY, USA

Present address: Department of Chemistry, University of California, Berkeley, Berkeley, CA, USA

Present address: School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, China

These authors contributed equally: M. H. Garner, H. Li, Y. Chen.

Authors

M.H.G., Ha.L., T.A.S., C.N., L.V. and G.C.S. conceived the idea for the paper. M.H.G. conducted the theoretical calculations under the supervision of G.C.S. Ha.L. did the conductance, noise and thermopower measurements under the supervision of L.V. Y.C., T.A.S., Z.S, D.W.P. and T.L. synthesized and characterized the molecules under the supervision of F.N., He.L., C.N. and S.X. M.H.G., Ha.L., L.V. and G.C.S. analysed the data and wrote the paper with contributions from all authors.

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