Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Heat dissipation in atomic-scale junctions

Nature volume 498, pages 209–212 (2013)Cite this article

Subjects

Abstract

Atomic and single-molecule junctions represent the ultimate limit to the miniaturization of electrical circuits1. They are also ideal platforms for testing quantum transport theories that are required to describe charge and energy transfer in novel functional nanometre-scale devices. Recent work has successfully probed electric and thermoelectric phenomena2,3,4,5,6,7,8 in atomic-scale junctions. However, heat dissipation and transport in atomic-scale devices remain poorly characterized owing to experimental challenges. Here we use custom-fabricated scanning probes with integrated nanoscale thermocouples to investigate heat dissipation in the electrodes of single-molecule (‘molecular’) junctions. We find that if the junctions have transmission characteristics that are strongly energy dependent, this heat dissipation is asymmetric—that is, unequal between the electrodes—and also dependent on both the bias polarity and the identity of the majority charge carriers (electrons versus holes). In contrast, junctions consisting of only a few gold atoms (‘atomic junctions’) whose transmission characteristics show weak energy dependence do not exhibit appreciable asymmetry. Our results unambiguously relate the electronic transmission characteristics of atomic-scale junctions to their heat dissipation properties, establishing a framework for understanding heat dissipation in a range of mesoscopic systems where transport is elastic—that is, without exchange of energy in the contact region. We anticipate that the techniques established here will enable the study of Peltier effects at the atomic scale, a field that has been barely explored experimentally despite interesting theoretical predictions9,10,11. Furthermore, the experimental advances described here are also expected to enable the study of heat transport in atomic and molecular junctions—an important and challenging scientific and technological goal that has remained elusive12,13.

This is a preview of subscription content, access via your institution

Access options

Rent or buy this article

Prices vary by article type

from$1.95

to$39.95

Learn more

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Nanoscale thermocouple probes and atomic and molecular junctions studied in this work.
Figure 2: Relationship between heat dissipation asymmetries and electronic transmission characteristics in Au–BDNC–Au junctions.
Figure 3: Heat dissipation asymmetry for Au–BDA–Au junctions.
Figure 4: No detectable heating asymmetry in Au–Au atomic junctions.

Similar content being viewed by others

References

  1. Cuevas, J. C. & Scheer, E. Molecular Electronics: An Introduction to Theory and Experiment (World Scientific, 2010)

    Book  Google Scholar 

  2. Scheer, E. et al. The signature of chemical valence in the electrical conduction through a single-atom contact. Nature 394, 154–157 (1998)

    Article  ADS  CAS  Google Scholar 

  3. Song, H. et al. Observation of molecular orbital gating. Nature 462, 1039–1043 (2009)

    Article  ADS  CAS  Google Scholar 

  4. 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)

    Article  ADS  CAS  Google Scholar 

  5. Xu, B. Q. & Tao, N. J. Measurement of single-molecule resistance by repeated formation of molecular junctions. Science 301, 1221–1223 (2003)

    Article  ADS  CAS  Google Scholar 

  6. Ludoph, B. & van Ruitenbeek, J. M. Thermopower of atomic-size metallic contacts. Phys. Rev. B 59, 12290–12293 (1999)

    Article  ADS  CAS  Google Scholar 

  7. Reddy, P., Jang, S. Y., Segalman, R. A. & Majumdar, A. Thermoelectricity in molecular junctions. Science 315, 1568–1571 (2007)

    Article  ADS  CAS  Google Scholar 

  8. Widawsky, J. R., Darancet, P., Neaton, J. B. & Venkataraman, L. Simultaneous determination of conductance and thermopower of single molecule junctions. Nano Lett. 12, 354–358 (2012)

    Article  ADS  CAS  Google Scholar 

  9. Galperin, M., Saito, K., Balatsky, A. V. & Nitzan, A. Cooling mechanisms in molecular conduction junctions. Phys. Rev. B 80, 115427 (2009)

    Article  ADS  Google Scholar 

  10. Dubi, Y. & Di Ventra, M. Colloquium: Heat flow and thermoelectricity in atomic and molecular junctions. Rev. Mod. Phys. 83, 131–155 (2011)

    Article  ADS  CAS  Google Scholar 

  11. Karlström, O., Linke, H., Karlström, G. & Wacker, A. Increasing thermoelectric performance using coherent transport. Phys. Rev. B 84, 113415 (2011)

    Article  ADS  Google Scholar 

  12. Lepri, S., Livi, R. & Politi, A. Thermal conduction in classical low-dimensional lattices. Phys. Rep. 377, 1–80 (2003)

    Article  ADS  MathSciNet  CAS  Google Scholar 

  13. Li, N. B. et al. Colloquium: Phononics: Manipulating heat flow with electronic analogs and beyond. Rev. Mod. Phys. 84, 1045–1066 (2012)

    Article  ADS  Google Scholar 

  14. Agraït, N., Untiedt, C., Rubio-Bollinger, G. & Vieira, S. Onset of energy dissipation in ballistic atomic wires. Phys. Rev. Lett. 88, 216803 (2002)

    Article  ADS  Google Scholar 

  15. Kim, Y., Pietsch, T., Erbe, A., Belzig, W. & Scheer, E. Benzenedithiol: a broad-range single-channel molecular conductor. Nano Lett. 11, 3734–3738 (2011)

    Article  ADS  CAS  Google Scholar 

  16. Huang, Z. F. et al. Local ionic and electron heating in single-molecule junctions. Nature Nanotechnol. 2, 698–703 (2007)

    Article  ADS  CAS  Google Scholar 

  17. Ward, D. R., Corley, D. A., Tour, J. M. & Natelson, D. Vibrational and electronic heating in nanoscale junctions. Nature Nanotechnol. 6, 33–38 (2011)

    Article  ADS  CAS  Google Scholar 

  18. Ioffe, Z. et al. Detection of heating in current-carrying molecular junctions by Raman scattering. Nature Nanotechnol. 3, 727–732 (2008)

    Article  ADS  CAS  Google Scholar 

  19. Datta, S. Electronic Transport in Mesoscopic Systems (Cambridge Univ. Press, 1995)

    Book  Google Scholar 

  20. Lee, W. & Reddy, P. Creation of stable molecular junctions with a custom-designed scanning tunneling microscope. Nanotechnology 22, 485703 (2011)

    Article  Google Scholar 

  21. Kiguchi, M., Miura, S., Hara, K., Sawamura, M. & Murakoshi, K. Conductance of a single molecule anchored by an isocyanide substituent to gold electrodes. Appl. Phys. Lett. 89, 213104 (2006)

    Article  ADS  Google Scholar 

  22. Sivan, U. & Imry, Y. Multichannel Landauer formula for thermoelectric transport with application to thermopower near the mobility edge. Phys. Rev. B 33, 551–558 (1986)

    Article  ADS  CAS  Google Scholar 

  23. Paulsson, M. & Datta, S. Thermoelectric effect in molecular electronics. Phys. Rev. B 67, 241403 (2003)

    Article  ADS  Google Scholar 

  24. Pauly, F. et al. Cluster-based density-functional approach to quantum transport through molecular and atomic contacts. New J. Phys. 10, 125019 (2008)

    Article  ADS  Google Scholar 

  25. Xue, Y. Q. & Ratner, M. A. End group effect on electrical transport through individual molecules: a microscopic study. Phys. Rev. B 69, 085403 (2004)

    Article  ADS  Google Scholar 

  26. Malen, J. A. et al. Identifying the length dependence of orbital alignment and contact coupling in molecular heterojunctions. Nano Lett. 9, 1164–1169 (2009)

    Article  ADS  CAS  Google Scholar 

  27. Venkataraman, L. et al. Single-molecule circuits with well-defined molecular conductance. Nano Lett. 6, 458–462 (2006)

    Article  ADS  CAS  Google Scholar 

  28. Brandbyge, M. et al. Quantized conductance in atom-sized wires between two metals. Phys. Rev. B 52, 8499–8514 (1995)

    Article  ADS  CAS  Google Scholar 

  29. Nielsen, S. K. et al. Current-voltage curves of atomic-sized transition metal contacts: an explanation of why Au is ohmic and Pt is not. Phys. Rev. Lett. 89, 066804 (2002)

    Article  ADS  CAS  Google Scholar 

  30. Tsutsui, M., Kawai, T. & Taniguchi, M. Unsymmetrical hot electron heating in quasi-ballistic nanocontacts. Sci. Rep. 2, 217 (2012)

    Article  ADS  Google Scholar 

Download references

Acknowledgements

P.R. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. DE-SC0004871 (nanofabrication of novel scanning probes), from the National Science Foundation under award no. CBET 0844902 (instrumentation for real-time control) and from the Center for Solar and Thermal Energy conversion, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0000957 (development of a scanning probe microscope). L.A.Z. acknowledges financial support from the Spanish MICINN through grant no. FIS2010-21883. F.P. acknowledges funding through the Carl Zeiss Stiftung, the DFG SFB 767, and the Baden-Württemberg Stiftung. P.R. thanks E. Meyhofer for discussions and comments. P.R. and J.C.C. thank A. Nitzan for discussions. J.C.C. is grateful for the hospitality provided by the Institute for Advanced Studies of the Hebrew University of Jerusalem, where part of this work was carried out.

Author information

Author notes

  1. Woochul Lee and Kyeongtae Kim: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Mechanical Engineering, University of Michigan, Ann Arbor, 48109, Michigan, USA

    Woochul Lee, Kyeongtae Kim, Wonho Jeong & Pramod Reddy

  2. Departamento de Física Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, Madrid, 28049, Spain

    Linda Angela Zotti & Juan Carlos Cuevas

  3. Department of Physics, University of Konstanz, D-78457 Konstanz, Germany,

    Fabian Pauly

  4. Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA,

    Pramod Reddy

Authors
  1. Woochul Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Kyeongtae Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Wonho Jeong
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Linda Angela Zotti
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Fabian Pauly
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Juan Carlos Cuevas
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Pramod Reddy
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

The idea for the experiments was conceived by P.R. and J.C.C. The experiments were performed by W.L. and K.K. The custom-fabricated probes were designed, fabricated and characterized by K.K. and W.J. Ab initio charge transport calculations were performed by L.A.Z. and F.P. The manuscript was written by P.R. and J.C.C. with comments and inputs from all authors.

Corresponding authors

Correspondence to Juan Carlos Cuevas or Pramod Reddy.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

This file contains Supplementary Figures 1-14, Supplementary Discussion and Supplementary References. (PDF 4309 kb)

PowerPoint slides

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Lee, W., Kim, K., Jeong, W. et al. Heat dissipation in atomic-scale junctions. Nature 498, 209–212 (2013). https://doi.org/10.1038/nature12183

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature12183

This article is cited by

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing