We present measurements of the thermal conductance of self-assembled monolayer (SAM) junctions formed between metal leads (Au, Ag, Pt, and Pd) with mismatched phonon spectra. The thermal conductance obtained from frequency domain thermoreflectance experiments is 65 ± 7 MW/m(2) K for matched Au-alkanedithiol-Au junctions, while the mismatched Au-alkanedithiol-Pd junctions yield a thermal conductance of 36 ± 3 MW/m(2) K. The experimental observation that junction thermal conductance (per molecule) decreases as the mismatch between the lead vibrational spectra increases, paired with results from molecular dynamics (MD) simulations, suggest that phonons scatter elastically at the metal-SAM interfaces. Furthermore, we resolve a known discrepancy between measurements and MD predictions of SAM thermal conductance by using a contact mechanics model to predict 54 ± 15% areal contact in the Au-alkanedithiol-Au experimental junction. This incomplete contact obscures the actual junction thermal conductance of 115 ± 22 MW/m(2) K, which is comparable to that of metal-dielectric interfaces.

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The thermal conductivity of gas-permeated single-walled carbon nanotube (SWCNT) aerogel (8 kg m − 3 density, 0.0061 volume fraction) is measured experimentally and modeled using mesoscale and atomistic simulations. Despite the high thermal conductivity of isolated SWCNTs, the thermal conductivity of the evacuated aerogel is 0.025 ± 0.010 W m − 1 K − 1 at a temperature of 300 K. This very low value is a result of the high porosity and the low interface thermal conductance at the tube-tube junctions (estimated as 12 pW K − 1 ). Thermal conductivity measurements and analysis of the gas-permeated aerogel (H 2 , He, Ne, N 2 , and Ar) show that gas molecules transport energy over length scales hundreds of times larger than the diameters of the pores in the aerogel. It is hypothesized that ineffi cient energy exchange between gas molecules and SWCNTs gives the permeating molecules a memory of their prior collisions. Low gas-SWCNT accommodation coeffi cients predicted by molecular dynamics simulations support this hypothesis. Amplifi ed energy transport length scales resulting from low gas accommodation are a general feature of CNT-based nanoporous materials.

We demonstrate tunable electrical and thermal conductivities through freezing rate control in solution-based nanocomposites. For a prototypical suspension of 1 vol % multilayer graphene suspended in hexadecane, the solid-liquid electrical conductivity contrast ratio can be tuned from 1 to 4.5 orders of magnitude for freezing rates between 10(2) and 10(-3) °C/min. We hypothesize that this dramatic variation stems from ice-templating, whereby crystal growth drives nanoparticles into concentrated intercrystal regions, increasing the percolation pathways and reducing the internanoparticle electrical resistance. Optical microscopy supports the ice-templating hypothesis, as these dramatic property changes coincide with changing crystal size. Under the same range of freezing rates, the nanocomposite solid-liquid thermal conductivity contrast ratio varies between 2.3 and 3.0, while pure hexadecane's varies between 2.1 and 2.6. The nanocomposite's thermal conductivity contrast ratios and solid phase enhancements are greater than effective medium theory predictions. We suggest this is due to ice-templating, consistent with our electrical measurements, as well as nanoparticle-induced molecular alignment of alkanes.