Heat dissipation in atomic-scale junctions

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.

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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.

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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.

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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.

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The authors declare no competing financial interests.

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

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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

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