Search

We report on the measured thermal conductivity of silicon irradiated with an array of ions: ${\mathrm{C}}^{2+},$ ${\mathrm{N}}^{2+},$ ${\mathrm{Al}}^{2+},$ ${\mathrm{Si}}^{2+},$ ${\mathrm{P}}^{2+},$ and ${\mathrm{Ge}}^{2+}$. Results are analyzed in consideration of ion mass, radius, and induced displacement damage. Recrystallization of select samples via annealing demonstrates that structural disorder imparted by incident ions, rather than the ions themselves, drive the reduction in thermal conductivity. This, in turn, is dictated by the mass of the ion. A generalized model is provided to relate thermal conductivity to displacement damage. Knowledge of the displacements-per-atom profile can thus be used to predict thermal conductivity reduction for silicon devices in extreme environments.

As electronic devices shrink down to their ultimate limit, the fundamental understanding of interfacial thermal transport becomes essential in thermal management. However, a comprehensive understanding of phonon transport mechanisms that drive interfacial thermal transport is still under development. The thermal transport across interfaces can be strongly affected by factors such as crystalline structure, surface roughness, chemical diffusion, etc. These complications lead to a significant quantitative uncertainty between experimentally measured thermal boundary conductance (TBC) across real material interfaces and theoretically calculated TBCs that are often predicted on structurally and/or chemically ideal interfaces. In this paper, we report on the thermal conductance across interfaces between various epitaxially grown metal films (Co, Ru, and Al) and $c$-plane sapphire substrates via time-domain thermoreflectance over the temperature range of \ensuremath{\sim}80 to \ensuremath{\sim}500 K. The room-temperature interface conductances of Al/sapphire, Co/sapphire, and Ru/sapphire are all $\ensuremath{\sim}350\phantom{\rule{0.16em}{0ex}}\mathrm{MW}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{\ensuremath{-}1}\phantom{\rule{0.16em}{0ex}}{\mathrm{K}}^{\ensuremath{-}1}$ despite the phonon spectra differences among the metals. We compare our results to predictions of TBC using atomistic Green's function calculations and the modal nonequilibrium Landauer method with transmission from the diffuse mismatch model. We found a consistent quantitative agreement between the experimentally measured TBCs and the predictions using the modal nonequilibrium Landauer model for the $\mathrm{Al}/{\mathrm{Al}}_{2}{\mathrm{O}}_{3}$, $\mathrm{Co}/{\mathrm{Al}}_{2}{\mathrm{O}}_{3}$, and $\mathrm{Ru}/{\mathrm{Al}}_{2}{\mathrm{O}}_{3}$ interfaces. This result suggests that interfacial elastic phonon thermal transport dominates TBC for the various epitaxial metal/sapphire combinations of interest in this work, while other mechanisms are negligible.

Responses of materials at high pressures can reveal fundamental insights into properties of condensed matter that are otherwise masked under ambient conditions. Using first-principles calculations to determine the electron-phonon interactions of free-electron metals at high pressures, we show that the electrical and thermal transport properties of aluminum, gold, and silver can be significantly enhanced with the application of high pressures. This is partly attributed to the decrease in electron-phonon coupling with increasing pressures. At elevated temperatures, under these high-pressure conditions, the thermal conductivity of aluminum is amongst the highest of any known material, surpassing the thermal conductivity of diamond at ambient pressure. Moreover, through calculation of the spectrally resolved electron-phonon coupling parameter at high pressures, we show an increased contribution to electron-phonon coupling from high-frequency longitudinal phonon modes scattering with electrons in aluminum. Using the same analysis with gold and silver, we show that low frequency acoustic phonon scattering with electrons is increased at high pressures. This work provides valuable insights into the electron-phonon scattering processes occurring under high pressures, which gives rise to new regimes of electrical and thermal transport properties in metals.

Manipulating thermal transport by designing materials with control of their properties over the entire spectral range of vibrational frequencies would provide a unique path to create solids with designer thermal conductivities. Traditional routes of nanostructuring to reduce the vibrational thermal conductivity of solids typically target narrow bands of the vibrational energy spectrum, which is often based on the characteristic dimensions of the nanostructure. In this work, we demonstrate the ability to simultaneously impact the phonon transport of both high- and low-frequency modes by creating defects that act as both high-frequency phonon scattering sites while coherently manipulating low-frequency waves via resonance with the long wavelength phonons. We use atomistic simulations to identify fullerenes functionalized on the sidewalls of carbon nanotubes (CNT) as efficient phonon blocks realized through localized resonances that appear due to hybridization between the modes of the fullerene and the underlying CNT. We show that with a large surface coverage and high periodicity in the inclusion of the covalently bonded fullerenes, the thermal conductivity of individual CNTs can be lowered by more than an order of magnitude, thus providing a large tunability in the thermal transport across these materials. We prescribe the large reduction in thermal conductivity to a combination of resonant phonon localization effects leading to phonon band anticrossings and vibrational scattering effects due to the inclusion of the strongly bonded fullerene molecules.

We report on the room temperature thermal conductivity of AlAs-GaAs superlattices (SLs), in which we systematically vary the period thickness and total thickness between $2--24\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$ and $20.1--2,160\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$, respectively. The thermal conductivity increases with the SL thickness and plateaus at a thickness around 200 nm, showing a clear transition from a quasiballistic to a diffusive phonon transport regime. These results demonstrate the existence of classical size effects in SLs, even at the highest interface density samples. We use harmonic atomistic Green's function calculations to capture incoherence in phonon transport by averaging the calculated transmission over several purely coherent simulations of independent SL with different random mixing at the AlAs-GaAs interfaces. These simulations demonstrate the significant contribution of incoherent phonon transport through the decrease in the transmission and conductance in the SLs as the number of interfaces increases. In spite of this conductance decrease, our simulations show a quasilinear increase in thermal conductivity with the superlattice thickness. This suggests that the observation of a quasilinear increase in thermal conductivity can have important contributions from incoherent phonon transport. Furthermore, this seemingly linear slope in thermal conductivity versus SL thickness data may actually be nonlinear when extended to a larger number of periods, which is a signature of incoherent effects. Indeed, this trend for superlattices with interatomic mixing at the interfaces could easily be interpreted as linear when the number of periods is small. Our results reveal that the change in thermal conductivity with period thickness is dominated by incoherent (particlelike) phonons, whose properties are not dictated by changes in the AlAs or GaAs phonon dispersion relations. This work demonstrates the importance of studying both period and sample thickness dependencies of thermal conductivity to understand the relative contributions of coherent and incoherent phonon transport in the thermal conductivity in SLs.

Fullerene condensed-matter solids can possess thermal conductivities below their minimum glassy limit while theorized to be stiffer than diamond when crystallized under pressure. These seemingly disparate extremes in thermal and mechanical properties raise questions into the pressure dependence on the thermal conductivity of ${\mathrm{C}}_{60}$ fullerite crystals, and how the spectral contributions to vibrational thermal conductivity changes under applied pressure. To answer these questions, we investigate the effect of strain on the thermal conductivity of ${\mathrm{C}}_{60}$ fullerite crystals via pressure-dependent molecular dynamics simulations under the Green-Kubo formalism. We show that the thermal conductivity increases rapidly with compressive strain, which demonstrates a power-law relationship similar to their stress-strain relationship for the ${\mathrm{C}}_{60}$ crystals. Calculations of the density of states for the crystals under compressive strains reveal that the librational modes characteristic in the unstrained case are diminished due to densification of the molecular crystal. Over a large compression range (0--20 GPa), the Leibfried-Schl\"omann equation is shown to adequately describe the pressure dependence of thermal conductivity, suggesting that low-frequency intermolecular vibrations dictate heat flow in the ${\mathrm{C}}_{60}$ crystals. A spectral decomposition of the thermal conductivity supports this hypothesis.

For this paper, single-pulse ablation mechanisms of ultrafast laser pulses ($25\phantom{\rule{0.222222em}{0ex}}\mathrm{ps}$) were studied for thin gold films ($65\phantom{\rule{0.222222em}{0ex}}\mathrm{nm}$) on an array of substrates with varying physical properties. Using time-domain thermoreflectance, the interfacial properties of the thin-film systems are measured: in particular, the thermal boundary conductance. We find that an often used, and widely accepted relation describing threshold fluences of homogeneous bulk targets breaks down at the nanoscale. Rather than relying solely on the properties of the ablated Au film, the ablation threshold of these Au/substrate systems is found to be dependent on the measured thermal boundary conductance; we additionally find no discernible trend between the damage threshold and properties of the underlying substrate. These results are discussed in terms of diffusive thermal transport and the interfacial bond strength.

We investigate thickness-limited size effects on the thermal conductivity of amorphous silicon thin films ranging from 3 to 1636 nm grown via sputter deposition. While exhibiting a constant value up to $\ensuremath{\sim}100$ nm, the thermal conductivity increases with film thickness thereafter. The thickness dependence we demonstrate is ascribed to boundary scattering of long wavelength vibrations and an interplay between the energy transfer associated with propagating modes (propagons) and nonpropagating modes (diffusons). A crossover from propagon to diffuson modes is deduced to occur at a frequency of $\ensuremath{\sim}1.8$ THz via simple analytical arguments. These results provide empirical evidence of size effects on the thermal conductivity of amorphous silicon and systematic experimental insight into the nature of vibrational thermal transport in amorphous solids.

We study the influence of molecular monolayers on the thermal conductivities and heat capacities of hybrid inorganic/organic superlattice thin films fabricated via atomic/molecular layer deposition. We measure the cross plane thermal conductivities and volumetric heat capacities of ${\mathrm{TiO}}_{2}$- and ZnO-based superlattices with periodic inclusion of hydroquinone layers via time domain thermoreflectance. In comparison to their homogeneous counterparts, the thermal conductivities in these superlattice films are considerably reduced. We attribute this reduction in the thermal conductivity mainly due to incoherent phonon boundary scattering at the inorganic/organic interface. Increasing the inorganic/organic interface density reduces the thermal conductivity and heat capacity of these films. High-temperature annealing treatment of the superlattices results in a change in the orientation of the hydroquinone molecules to a 2D graphitic layer along with a change in the overall density of the hybrid superlattice. The thermal conductivity of the hybrid superlattice increases after annealing, which we attribute to an increase in crystallinity.

We argue that the relative thermal conductance between interfaces with different morphologies is controlled by crystal structure through $M_{min}/M_c > 1$, the ratio between the {\it minimum mode} count on either side $M_{min}$, and the {\it conserving modes} $M_c$ that preserve phonon momentum transverse to the interface. Junctions with an added homogenous layer, "uniform", and "abrupt" junctions are limited to $M_c$ while junctions with interfacial disorder, "mixed", exploit the expansion of mode spectrum to $M_{min}$. In our studies with cubic crystals, the largest enhancement of conductance from "abrupt" to "mixed" interfaces seems to be correlated with the emergence of voids in the conserving modes, where $M_c = 0$. Such voids typically arise when the interlayer coupling is weakly dispersive, making the bands shift rigidly with momentum. Interfacial mixing also increases alloy scattering, which reduces conductance in opposition with the mode spectrum expansion. Thus the conductance across a "mixed' junction does not always increase relative to that at a "uniform" interface., 25 pages, 8 figures

The thermal boundary conductance across solid-solid interfaces can be affected by the physical properties of the solid boundary. Atomic composition, disorder, and bonding between materials can result in large deviations in the phonon scattering mechanisms contributing to thermal boundary conductance. Theoretical and computational studies have suggested that the mixing of atoms around an interface can lead to an increase in thermal boundary conductance by creating a region with an average vibrational spectra of the two materials forming the interface. In this paper, we experimentally demonstrate that ion irradiation and subsequent modification of atoms at solid surfaces can increase the thermal boundary conductance across solid interfaces due to a change in the acoustic impedance of the surface. We measure the thermal boundary conductance between thin aluminum films and silicon substrates with native silicon dioxide layers that have been subjected to proton irradiation and post-irradiation surface cleaning procedures. The thermal boundary conductance across the Al/native oxide/Si interfacial region increases with an increase in proton dose. Supported with statistical simulations, we hypothesize that ion beam mixing of the native oxide and silicon substrate within $\ensuremath{\sim}2.2\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ of the silicon surface results in the observed increase in thermal boundary conductance. This ion mixing leads to the spatial gradation of the silicon native oxide into the silicon substrate, which alters the acoustic impedance and vibrational characteristics at the interface of the aluminum film and native oxide/silicon substrate. We confirm this assertion with picosecond acoustic analyses. Our results demonstrate that under specific conditions, a ``more disordered and defected'' interfacial region can have a lower resistance than a more ``perfect'' interface.

Thermal boundary resistance dominates the overall resistance of nanosystems. This effect can be utilized to improve the figure of merit of thermoelectric materials. It is also a concern for thermal failures in microelectronic devices. The interfacial resistance depends sensitively on many interrelated structural details including material properties of the two layers, the system dimensions, the interfacial morphology, and the defect concentrations near the interface. The lack of an analytical understanding of these dependencies has been a major hurdle for a science-based design of optimum systems on a nanoscale. Here we have combined an analytical model with extensive, highly converged direct-method molecular dynamics simulations to derive analytical relationships between interfacial thermal boundary resistance and structural features. We discover that thermal boundary resistance linearly decreases with total interfacial area that can be modified by interfacial roughening. This finding is further elucidated using wave-packet analysis and local density of state calculations.

We investigate the behavior of Kapitza conductance at interfaces between two Lennard-Jones fcc solids as a function of the range and strength of cross-species interactions via molecular dynamics simulations. It is found that decreasing either of these quantities leads to a reduction in the slope of linear temperature dependence of Kapitza conductance, suggesting a corresponding decrease in the probability of inelastic phonon-phonon interactions. To further explore the mechanisms responsible for such behavior, we calculate the phonon density of states and spectral temperature of each of the monolayers adjacent to the interface. It is found that the reduction of the range and strength of cross-species interactions leads to a softening of the density of states near the interface, while the spectral temperature calculations provide further evidence that such reductions decrease the probability of inelastic phonon scattering. These findings help explain varying accounts of the temperature dependence of Kapitza conductance observed in previous works.

We investigate the role of anisotropy on interfacial transport across solid interfaces by measuring the thermal boundary conductance from 100 to 500 K across Al/Si and Al/sapphire interfaces with different substrate orientations. The measured thermal boundary conductances show a dependency on substrate crystallographic orientation in the sapphire samples (trigonal conventional cell) but not in the silicon samples (diamond cubic conventional cell). The change in interface conductance in the sapphire samples is ascribed to anisotropy in the Brillouin zone along the principal directions defining the conventional cell. This leads to resultant phonon velocities in the direction of thermal transport that vary nearly 40% based on crystallographic direction.

We examine the fundamental phonon mechanisms affecting the interfacial thermal conductance across a single layer of quantum dots (QDs) on a planar substrate. We synthesize a series of Ge${}_{x}$Si${}_{1\ensuremath{-}x}$ QDs by heteroepitaxial self-assembly on Si surfaces and modify the growth conditions to provide QD layers with different root-mean-square (rms) roughness levels in order to quantify the effects of roughness on thermal transport. We measure the thermal boundary conductance (${h}_{\mathrm{K}}$) with time-domain thermoreflectance. The trends in thermal boundary conductance show that the effect of the QDs on ${h}_{\mathrm{K}}$ are more apparent at elevated temperatures, while at low temperatures, the QD patterning does not drastically affect ${h}_{\mathrm{K}}$. The functional dependence of ${h}_{\mathrm{K}}$ with rms surface roughness reveals a trend that suggests that both vibrational mismatch and changes in the localized phonon transport near the interface contribute to the reduction in ${h}_{\mathrm{K}}$. We find that QD structures with rms roughnesses greater than 4 nm decrease ${h}_{\mathrm{K}}$ at Si interfaces by a factor of 1.6. We develop an analytical model for phonon transport at rough interfaces based on a diffusive scattering assumption and phonon attenuation that describes the measured trends in ${h}_{\mathrm{K}}$. This indicates that the observed reduction in thermal conductivity in SiGe quantum dot superlattices is primarily due to the increased physical roughness at the interfaces, which creates additional phonon resistive processes beyond the interfacial vibrational mismatch.

Thermal transport across one-dimensional atomic chains is studied using a harmonic nonequilibrium Green's function formalism in the ballistic phonon transport regime. Introducing a mass impurity in the chain and mass loading in the thermal contacts leads to interference of phonon waves, which can be manipulated by varying the magnitude of the loading. This shows that thermal rectification is tunable in a completely harmonic system.