Abstract
Manipulating interfacial thermal transport is important for many technologies including nanoelectronics, solid-state lighting, energy generation and nanocomposites1,2,3. Here, we demonstrate the use of a strongly bonding organic nanomolecular monolayer (NML) at model metal/dielectric interfaces to obtain up to a fourfold increase in the interfacial thermal conductance, to values as high as 430 MW m−2 K−1 in the copper–silica system. We also show that the approach of using an NML can be implemented to tune the interfacial thermal conductance in other materials systems. Molecular dynamics simulations indicate that the remarkable enhancement we observe is due to strong NML–dielectric and NML–metal bonds that facilitate efficient heat transfer through the NML. Our results underscore the importance of interfacial bond strength as a means to describe and control interfacial thermal transport in a variety of materials systems.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Pop, E. Energy dissipation and transport in nanoscale devices. Nano Res. 3, 147–169 (2010).
Cahill, D. G. et al. Nanoscale thermal transport. J. Appl. Phys. 93, 793–818 (2003).
Jain, A. & Goodson, K. E. Thermal microdevices for biological and biomedical applications. J. Therm. Biol. 36, 209–218 (2011).
Siemens, M. E. et al. Quasi-ballistic thermal transport from nanoscale interfaces observed using ultrafast coherent soft X-ray beams. Nature Mater. 9, 26–30 (2010).
Minnich, A. J. et al. Thermal conductivity spectroscopy technique to measure phonon mean free paths. Phys. Rev. Lett. 107, 095901 (2011).
Hu, M., Shenogin, S. & Keblinski, P. Molecular dynamics simulation of interfacial thermal conductance between silicon and amorphous polyethylene. Appl. Phys. Lett. 91, 241910 (2007).
Wang, R. Y., Segalman, R. A. & Majumdar, A. Room temperature thermal conductance of alkanedithiol self-assembled monolayers. Appl. Phys. Lett. 89, 173113 (2006).
Lyeo, H-K. & Cahill, D. Thermal conductance of interfaces between highly dissimilar materials. Phys. Rev. B 73, 144301 (2006).
Duda, J. C., Beechem, T. E., Smoyer, J. L., Norris, P. M. & Hopkins, P. E. Role of dispersion on phononic thermal boundary conductance. J. Appl. Phys. 108, 073515 (2010).
Losego, M. D., Moh, L., Arpin, K. A., Cahill, D. G. & Braun, P. V. Interfacial thermal conductance in spun-cast polymer films and polymer brushes. Appl. Phys. Lett. 97, 011908 (2010).
Hu, M., Keblinski, P. & Schelling, P. K. Kapitza conductance of silicon-amorphous polyethylene interfaces by molecular dynamics simulations. Phys. Rev. B 79, 104305 (2009).
Hu, M., Goicochea, J. V., Michel, B. & Poulikakos, D. Water nanoconfinement induced thermal enhancement at hydrophilic quartz interfaces. Nano Lett. 10, 279–285 (2010).
Shenogina, N., Godawat, R., Keblinski, P. & Garde, S. How wetting and adhesion affect thermal conductance of a range of hydrophobic to hydrophilic aqueous interfaces. Phys. Rev. Lett. 102, 156101 (2009).
Gandhi, D. D. et al. Annealing-induced interfacial toughening using a molecular nanolayer. Nature 447, 299–302 (2007).
Jain, A. et al. Atomistic fracture energy partitioning at a metal–ceramic interface using a nanomolecular monolayer. Phys. Rev. B 83, 035412 (2011).
Koh, Y. K., Bae, M-H., Cahill, D. G. & Pop, E. Heat conduction across monolayer and few-layer graphenes. Nano Lett. 10, 4363–4368 (2010).
Huxtable, S. T. et al. Interfacial heat flow in carbon nanotube suspensions. Nature Mater. 2, 731–734 (2003).
Majumdar, A. & Reddy, P. Role of electron–phonon coupling in thermal conductance of metal–nonmetal interfaces. Appl. Phys. Lett. 84, 4768–4770 (2004).
Sun, H., Mumby, S. J., Maple, J. R. & Hagler, A. T. An ab initio CFF93 all-atom force field for polycarbonates. J. Am. Chem. Soc. 116, 2978–2987 (1994).
DelRio, F. W., Jaye, C., Fischer, D. A. & Cook, R. F. Elastic and adhesive properties of alkanethiol self-assembled monolayers on gold. Appl. Phys. Lett. 94, 131909 (2009).
Wang, Z. et al. Ultrafast flash thermal conductance of molecular chains. Science 317, 787–790 (2007).
Duda, J. C., Saltonstall, C. B., Norris, P. M. & Hopkins, P. E. Assessment and prediction of thermal transport at solid–self-assembled monolayer junctions. J. Chem. Phys. 134, 094704 (2011).
Bodapati, A., Schelling, P., Phillpot, S. & Keblinski, P. Vibrations and thermal transport in nanocrystalline silicon. Phys. Rev. B 74, 245207 (2006).
Gandhi, D. D. et al. Molecular-nanolayer-induced suppression of in-plane Cu transport at Cu–silica interfaces. Appl. Phys. Lett. 90, 163507 (2007).
Singh, A. P., Gandhi, D. D., Lipp, E., Eizenberg, M. & Ramanath, G. Suppression of chemical and electrical instabilities in mesoporous silica films by molecular capping. J. Appl. Phys. 100, 114504 (2006).
Thuo, M. M. et al. Odd-even effects in charge transport across self-assembled monolayers. J. Am. Chem. Soc. 133, 2962–2975 (2011).
Amalric, J. et al. Phosphonate monolayers functionalized by silver thiolate species as antibacterial nanocoatings on titanium and stainless steel. J. Mater. Chem. 19, 141–149 (2008).
Schmidt, A. J., Chen, X. & Chen, G. Pulse accumulation, radial heat conduction, and anisotropic thermal conductivity in pump-probe transient thermoreflectance. Rev. Sci. Instrum. 79, 114902 (2009).
Hu, L., Desai, T. & Keblinski, P. Determination of interfacial thermal resistance at the nanoscale. Phys. Rev. B 83, 195423 (2011).
Costescu, R., Wall, M. & Cahill, D. Thermal conductance of epitaxial interfaces. Phys. Rev. B 67, 054302 (2003).
Davison, A. C. & Hinkley, D. V. Bootstrap Methods and Their Application (Cambridge Univ. Press, 1997).
Shenogin, S. & Ozisik, R. Xenoview at http://xenoview.mat.rpi.edu/ (2010).
Acknowledgements
We gratefully acknowledge financial support from National Science Foundation awards CMMI 1100933 and ECCS 1002282, and an NRI grant from the SRC administered through the Index Center at the University at Albany. P.J.O. also acknowledges support from a GK-12 Fellowship from the National Science Foundation, and helpful discussions with T. R. Willemain in formulating the statistical analysis. P.H.M. and D.L. acknowledge support from the Transatlantic Partner University Fund in which both RPI and Université de Montpellier 2 are partners.
Author information
Authors and Affiliations
Contributions
The project was conceived and directed by G.R., and conducted through collaboration with M.Y., P.K. and P.H.M. P.J.O. prepared most samples, carried out the experiments and analysed the data. P.K.C. assembled MDPA and carried out fracture tests for the TiO2 samples. D.L. and P.H.M. synthesized MDPA molecules and provided interface functionalization procedures for the experiments with phosphonate nanolayers. J.L. contributed to experimental design and data analysis under the guidance of M.Y. S.S. conducted the molecular dynamics simulations under the guidance of P.K. P.J.O. wrote the paper together with G.R. using inputs from the other co-authors. All authors discussed the results and implications and commented on the manuscript at all stages.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Supplementary information
Supplementary Information
Supplementary Information (PDF 305 kb)
Rights and permissions
About this article
Cite this article
O’Brien, P., Shenogin, S., Liu, J. et al. Bonding-induced thermal conductance enhancement at inorganic heterointerfaces using nanomolecular monolayers. Nature Mater 12, 118–122 (2013). https://doi.org/10.1038/nmat3465
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nmat3465
This article is cited by
-
Atomically precise photothermal nanomachines
Nature Materials (2024)
-
Self-Modifying Nanointerface Driving Ultrahigh Bidirectional Thermal Conductivity Boron Nitride-Based Composite Flexible Films
Nano-Micro Letters (2023)
-
Quantifying spectral thermal transport properties in framework of molecular dynamics simulations: a comprehensive review
Rare Metals (2023)
-
Viscoelastic bandgap in multilayers of inorganic–organic nanolayer interfaces
Scientific Reports (2022)
-
Physical and chemical descriptors for predicting interfacial thermal resistance
Scientific Data (2020)