In standard molecular junctions, a molecular structure is placed between and connected to metal leads. Understanding how mechanical tuning in such molecular junctions can change heat conductance has interesting applications in nanoscale energy transport. In this work, we use nonequilibrium molecular dynamics simulations to address the effect of stretching on the phononic contribution to the heat conduction of molecular junctions consisting of single long-chain alkanes and various metal leads, such as Ag, Au, Cu, Ni, and Pt. The thermal conductance of such junctions is found to be much smaller than the intrinsic thermal conductance of the polymer and significantly depends on the nature of metal leads as expressed by the metal–molecule coupling and metal vibrational density of states. This behavior is expected and reflects the mismatch of phonon spectra at the metal molecule interfaces. As a function of stretching, we find a behavior similar to what was observed earlier [M. Dinpajooh and A. Nitzan, J. Chem. Phys. 153, 164903 (2020)] for pure polymeric structures. At relatively short electrode distances, where the polyethylene chains are compressed, it is found that the thermal conductances of the molecular junctions remain almost constant as one stretches the polymer chains. At critical electrode distances, the thermal conductances start to increase, reaching the values of the fully extended molecular junctions. Similar behaviors are observed for junctions in which several long-chain alkanes are sandwiched between various metal leads. These findings indicate that this behavior under stretching is an intrinsic property of the polymer chain and not significantly associated with the interfacial structures.
In situ and ex situ processes for synthesizing metal multilayers with electronically conductive interfaces
A number of technological applications and scientific experiments require processes for preparing metal multilayers with electronically and thermally conductive interfaces. We investigate how in situ vs ex situ synthesis processes affect the thermal conductance of metal/metal interfaces. We use time-domain thermoreflectance experiments to study thermal transport in Au/Fe, Al/Cu, and Cu/Pt bilayer samples. We quantify the effect of exposing the bottom metal layer to an ambient environment prior to deposition of the top metal layer. We observe that for Au/Fe, exposure of the Fe layer to air before depositing the top Au layer significantly impedes interfacial electronic currents. Exposing Cu to air prior to depositing an Al layer effectively eliminates interfacial electronic heat currents between the two metal layers. Exposure to air appears to have no effect on interfacial transport in the Cu/Pt system. Finally, we show that a short RF sputter etch of the bottom layer surface is sufficient to ensure a thermally and electronically conductive metal/metal interface in all materials we study. We analyze our results with a two-temperature model and bound the electronic interface conductance for the nine samples we study. Our findings have applications for thin-film synthesis and advance fundamental understanding of electronic thermal conductance at different types of interfaces between metals.
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- Award ID(s):
- 1847632
- NSF-PAR ID:
- 10401923
- Date Published:
- Journal Name:
- Journal of Applied Physics
- Volume:
- 131
- Issue:
- 22
- ISSN:
- 0021-8979
- Page Range / eLocation ID:
- 225302
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0084573
