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Thermal conductance of
solid-solid and solid-liquid interfaces
  • David G. Cahill,
  • Zhenbin Ge, Ho-Ki Lyeo, Xuan Zheng, Paul Braun
  • Frederick Seitz Materials Research Lab and Department of Materials Science
  • University of Illinois, Urbana
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Interfaces are critical at the nanoscale
  • Low thermal conductivity in nanostructured materials
    • improved thermoelectric energy conversion
    • improved thermal barriers



  • High thermal conductivity composites and suspensions
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Interfaces are critical at the nanoscale
  • High power density devices
    • solid state lighting
    • high speed electronics
    • nanoscale sensors
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Interface thermal conductance
  • Thermal conductivity L is a property of the continuum
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Interface thermal conductance (2001)
  • Observations (2001) span a very limited range
    • Al/sapphire à Pb/diamond
    • no data for hard/soft
  • lattice dynamics (LD) theory by Stoner and Maris (1993)
  • Diffuse mismatch (DMM) theory by Swartz and Pohl (1987)
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Acoustic and diffuse mismatch theory
  • Acoustic mismatch (AMM)
    • perfect interface: average transmission coefficient <t> given by differences in acoustic impedance, Z=rv
    • lattice dynamics (LD) incorporates microscopics
  • Diffuse mismatch (DMM)
    • disordered interface: <t> given by differences in densities of vibrational states
  • Predicted large range of G not observed (2001)
  • For similar materials, scattering decreases G
  • For dissimilar materials, scattering increases G
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2005: Factor of 60 range at room temperature
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Modulated pump-probe apparatus
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psec acoustics and
time-domain thermoreflectance
  • Optical constants and reflectivity depend on strain and temperature
  • Strain echoes give acoustic properties or film thickness
  • Thermoreflectance gives thermal properties
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Modulated pump-probe
  • four times scales:
    • pulse duration, 0.3 ps
    • pulse spacing, 12.5 ns
    • modulation period, 100 ns
    • time-delay, t


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Analytical model for modulated time-domain thermoreflectance
  • frequency domain solution for heat flow in cylindrical coordinates using gaussian beams.



  • G(k) given by iterative solution (transfer matrix)
  • In-phase and out-of-phase signals by series of sum and difference over sidebands



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Iterative solution for layered geometries
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Two basic types of experiments on solid samples
  • thermal conductivity of bulk samples and thermal conductance of interfaces
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Flexible, convenient, and accurate technique...
  • ...with 3 micron resolution
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Interfaces between highly dissimilar materials
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Thermoreflectance data for Bi and Pb interfaces
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Room temperature thermal conductance
  • Pb and Bi show similar behavior.  Electron-phonon coupling is not an important channel.
  • Weak dependence on Debye velocity of the substrate.
  • Pb/diamond 50% smaller than Stoner and Maris but still far too large for a purely elastic process.
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Temperature dependence of the conductance
  • Excess conductance has a linear temperature dependence (not observed by Stoner and Maris).
  • Suggests inelastic (3-phonon?) channel for heat transport
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Application: can we use interfaces to beat the minimum thermal conductivity?
  • If the small thermal conductance of Bi/diamond could be reproduced in a multi-layered film, then placing interfaces every 10 nm would give an incredibly low thermal conductivity of 0.1 W/m-K (factor of 2 smaller than a polymer).
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W/Al2O3 nanolaminates
  • room temperature data
  • sputtered in pure Ar
  • atomic-layer deposition at 177 and 300 °C, S. George (U. Colorado)
  • G = 220 MW m-2 K-1
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Unexpected advance: Thermal conductivity imaging
  • At t=100 ps,
    •  in-phase signal is mostly determined by the heat capacity of the Al film
    • out-of-phase signal is mostly determined by the effusivity (LC)1/2 of the substrate
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ZrO2:Y  thermal barrier
  • after 500 thermal cycles (1 h)
  • 25 °C —>1135 °C—>25 °C
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ZrO2:Y  thermal barrier
  • after 500 thermal cycles (1 h)
  • 25 °C —>1135 °C—>25 °C
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Solid-liquid interfaces: Two approaches
  • Transient absorption measurements of nanoparticles and nanotubes in liquid suspensions.
    • Measure the thermal relaxation time of a suddenly heat particle.  If the particle is small enough, then we have sensitivity to the interface
    • limited to interfaces that give good stability of the suspension
  • Thin planar Al and Au films.  Same as before but heat flows both directions: into the fluid and into the solid substrate.


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Transient absorption
  • Optical absorption depends on temperature of the nanotube
  • Cooling rate gives interface conductance
  •    G = 12 MW m-2 K-1
  • MD suggests channel is low frequency squeezing and bending modes strongly coupled to the fluid.
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Application: Critical aspect ratio for a fiber composite
  • Isotropic fiber composite with high conductivity fibers (and infinite interface conductance)
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Hydrophilic metal nanoparticles: 4 nm diameter Au:Pd nanoparticles in water
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22 nm diameter Au:Pd nanoparticles in water; CTAB surfactant
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Nanoparticle summary
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Application: Critical particle radius for nanocomposite
  • Interface conductance and thermal conductivity of the fluid determine a critical particle radius
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Thermoreflectance of solid-liquid interfaces
  • hydrophobic
  • 37 MW/m2-K





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Conclusions
  • Much to learn about transport of heat across interfaces but we now have good tools.
  • Pb/diamond, Bi/diamond interfaces show a temperature dependent conductance far above the radiation limit.  What is the correct description of this inelastic channel?
  • Can circumvent the “minimum thermal conductivity” with high densities of interfaces.
  • Conductance of hydrophilic nanoparticle/surfactant/water interfaces is essentially independent of the surfactant layer.
  • Heat transfer is reduced by a factor of 4 at hydrophobic interfaces with water.