Jeffrey L. Braun

Effect of crystalline/amorphous interfaces on thermal transport across confined thin films and superlattices

We report on the thermal boundary resistances across crystalline and amorphous confined thin films and the thermal conductivities of amorphous/crystalline superlattices for Si/Ge systems as determined via non-equilibrium molecular dynamics simulations. Thermal resistances across disordered Si or Ge thin films increase with increasing length of the interfacial thin films and in general demonstrate higher thermal boundary resistances in comparison to ordered films. However, for films ≲3 nm, the resistances are highly dependent on the spectral overlap of the density of states between the film and leads. Furthermore, the resistances at a single amorphous/crystalline interface in these structures are much lower than those at interfaces between the corresponding crystalline materials, suggesting that diffusive scattering at an interface could result in higher energy transmissions in these systems. We use these findings, together with the fact that high mass ratios between amorphous and crystalline materials can...

Upper limit to the thermal penetration depth during modulated heating of multilayer thin films with pulsed and continuous wave lasers: A numerical study

In this study, we present a method to calculate the temperature and heat flux profiles as a function of depth and radius for bulk, homogeneous materials and samples with layered thin-film structures, including geometries supporting bidirectional heat fluxes, during pulsed and continuous wave (CW) laser heating. We calculate the temperature profiles for both modulated and unmodulated heating events to reveal that the thermal penetration depth (defined as the depth at which temperature decays to 1/e of the surface temperature) for a pulsed laser is highly dependent on time and repetition rate. In the high repetition rate limit, the temperature profile relaxes to that of a CW source profile, while in the opposite extreme, a single pulse response is observed such that the concept of the thermal penetration depth loses any practical meaning. For modulated heating events such as those used in time- and frequency-domain thermoreflectance, we show that there is a limit to the thermal penetration depth obtainable ...

Ballistic transport of long wavelength phonons and thermal conductivity accumulation in nanograined silicon-germanium alloys

Computationally efficient modeling of the thermal conductivity of materials is crucial to thorough experimental planning and theoretical understanding of thermal properties. We present a modeling approach in this work that utilizes frequency-dependent effective medium to calculate lattice thermal conductivity of nanostructured solids. The method accurately predicts a significant reduction in the thermal conductivity of nanostructured Si80Ge20 systems, along with previous reported thermal conductivities in nanowires and nanoparticles-in-matrix materials. We use our model to gain insight into the role of long wavelength phonons on the thermal conductivity of nanograined silicon-germanium alloys. Through thermal conductivity accumulation calculations with our modified effective medium model, we show that phonons with wavelengths much greater than the average grain size will not be impacted by grain boundary scattering, counter to the traditionally assumed notion that grain boundaries in solids will act as diffusive interfaces that will limit long wavelength phonon transport. This is further supported through a modulation frequency dependent thermal conductivity as measured with time-domain thermoreflectance.

On the Steady-State Temperature Rise During Laser Heating of Multilayer Thin Films in Optical Pump–Probe Techniques

Patrick E. Hopkins Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA 22904; Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA 22904; Department of Physics, University of Virginia, Charlottesville, VA 22904 e-mail: phopkins@virginia.edu On the Steady-State Temperature Rise During Laser Heating of Multilayer Thin Films in Optical Pump–Probe Techniques

Reducing the thermal conductivity of chemically ordered binary alloys below the alloy limit via the alteration of phonon dispersion relations

We investigate the effect of crystalline configuration on the thermal conductivity of binary Lennard-Jones based solid solutions via classical molecular dynamics simulations and harmonic lattice dynamics calculations. We show that the pronounced effect of Umklapp scattering causes the cross-plane thermal conductivity of the chemically ordered alloy (1 × 1 monolayer period superlattice) to approach the thermal conductivity of the disordered counterpart (alloy limit) at elevated temperatures. However, we find that for superlattices with thicker periods and larger acoustic mismatch between the layers, the thermal conductivity can approach a minimum that is well below the alloy limit and can even approach the theoretical minimum limit of the corresponding amorphous phase. Our simulations over a wide range of mass ratios between the species suggest two contrasting effects of increasing mass ratio: (i) flattening of modes that leads to lower group velocities and lower overall thermal conductivity and (ii) reduc...

Crystalline coherence length effects on the thermal conductivity of MgO thin films

Phonon scattering in crystalline systems can be strongly dictated by a wide array of defects, many of which can be difficult to observe via standard microscopy techniques. We experimentally demonstrate that the phonon thermal conductivity of MgO thin films is proportional to the crystal’s coherence length, a property of a solid that quantifies the length scale associated with crystalline imperfections. Sputter-deposited films were prepared on (100)-oriented silicon and then annealed to vary the crystalline coherence, as characterized using x-ray diffraction line broadening. We find that the measured thermal conductivity of the MgO films varies proportionally with crystalline coherence length, which is ultimately limited by the grain size. The microstructural length scales associated with crystalline defects, such as small-angle tilt boundaries, dictate this crystalline coherence length, and our results demonstrate the role that this length scale has on the phonon thermal conductivity of thin films. Our results suggest that this crystalline coherence length scale provides a measure of the limiting phonon mean free path in crystalline solids, a quantity that is often difficult to measure and observe with more traditional imagining techniques.

Reduced dependence of thermal conductivity on temperature and pressure of multi-atom component crystalline solid solutions

We investigate the effect of mass disorder, temperature, and pressure on the spectral thermal conductivity of multicomponent crystalline solid solutions via molecular dynamics simulations. The thermal conductivities of Lennard-Jones based solid solutions with one to five different atomic components in the crystalline lattice are simulated at a range of uniaxial strain levels and temperatures. Our results show that for multicomponent alloys, increasing only the mass impurity scattering by adding atoms with different masses in the solid solution does not lead to significant changes in the spectral contributions to thermal conductivity. However, increasing the impurity concentration or changing the local force-field of the impurity atoms in the solid solution has a relatively significant impact on the spectral contributions to thermal conductivity. The effect of chemical order in these alloys is shown to drastically alter the temperature dependence due to the different scattering mechanisms dictating thermal...

Localized thin film damage sourced and monitored via pump-probe modulated thermoreflectance

Damage in the form of dewetting and delamination of thin films is a major concern in applications requiring micro- or nano-fabrication. In non-contact nanoscale characterization, optical interrogation must be kept to energies below damage thresholds in order to conduct measurements such as pump-probe spectroscopy. In this study, we show that the thermoreflectance of thin films can indicate the degree of film damage induced by a modulated optical heating source. By adjusting the absorbed power of the pump heating event, we identify the characteristics of the change in the thermoreflectance signal when leading up to and exceeding the damage threshold of gold films of varying thicknesses on glass substrates.

Breaking network connectivity leads to ultralow thermal conductivities in fully dense amorphous solids

We demonstrate a method to reduce the thermal conductivity of fully dense (above the rigidity percolation threshold) amorphous thin films below the minimum limit by systematically changing the coordination number through hydrogenation. Studying a-SiO:H, a-SiC:H, and a-Si:H thin films, we measure the thermal properties using time-domain thermoreflectance to show that thermal conductivity can be reduced below the amorphous limit by a factor of up to two. By experimentally investigating the thermophysical parameters that determine thermal conductivity, we show that sound speed, atomic density, and heat capacity cannot explain the measured reduction in thermal conductivity, revealing that the coordination number can significantly alter the scattering length scale of heat carriers. Reformulating the minimum limit to consider the propensity for energy to transfer through the non-hydrogen network of atoms, we observe greatly improved agreement with experimental data.

Substrate thermal conductivity controls the ability to manufacture microstructures via laser-induced direct write

In controlling the thermal properties of the surrounding environment, we provide insight into the underlying mechanisms driving the widely used laser direct write method for additive manufacturing. We find that the onset of silver nitrate reduction for the formation of direct write structures directly corresponds to the calculated steady-state temperature rises associated with both continuous wave and high-repetition rate, ultrafast pulsed laser systems. Furthermore, varying the geometry of the heat affected zone, which is controllable based on in-plane thermal diffusion in the substrate, and laser power, allows for control of the written geometries without any prior substrate preparation. These findings allow for the advance of rapid manufacturing of micro- and nanoscale structures with minimal material constraints through consideration of the laser-controllable thermal transport in ionic liquid/substrate media.In controlling the thermal properties of the surrounding environment, we provide insight into the underlying mechanisms driving the widely used laser direct write method for additive manufacturing. We find that the onset of silver nitrate reduction for the formation of direct write structures directly corresponds to the calculated steady-state temperature rises associated with both continuous wave and high-repetition rate, ultrafast pulsed laser systems. Furthermore, varying the geometry of the heat affected zone, which is controllable based on in-plane thermal diffusion in the substrate, and laser power, allows for control of the written geometries without any prior substrate preparation. These findings allow for the advance of rapid manufacturing of micro- and nanoscale structures with minimal material constraints through consideration of the laser-controllable thermal transport in ionic liquid/substrate media.