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"Falcone, Roger W"
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new regime of nanoscale thermal transport: Collective diffusion increases dissipation efficiency
2015
Significance A complete description of nanoscale thermal transport is a fundamental problem that has defied understanding for many decades. Here, we uncover a surprising new regime of nanoscale thermal transport where, counterintuitively, nanoscale heat sources cool more quickly when placed close together than when they are widely separated. This increased cooling efficiency is possible when the separation between nanoscale heat sources is comparable to the average mean free paths of the dominant heat-carrying phonons. This finding suggests new approaches for addressing the significant challenge of thermal management in nanosystems, with design implications for integrated circuits, thermoelectric devices, nanoparticle-mediated thermal therapies, and nanoenhanced photovoltaics for improving clean-energy technologies.
Understanding thermal transport from nanoscale heat sources is important for a fundamental description of energy flow in materials, as well as for many technological applications including thermal management in nanoelectronics and optoelectronics, thermoelectric devices, nanoenhanced photovoltaics, and nanoparticle-mediated thermal therapies. Thermal transport at the nanoscale is fundamentally different from that at the macroscale and is determined by the distribution of carrier mean free paths and energy dispersion in a material, the length scales of the heat sources, and the distance over which heat is transported. Past work has shown that Fourier’s law for heat conduction dramatically overpredicts the rate of heat dissipation from heat sources with dimensions smaller than the mean free path of the dominant heat-carrying phonons. In this work, we uncover a new regime of nanoscale thermal transport that dominates when the separation between nanoscale heat sources is small compared with the dominant phonon mean free paths. Surprisingly, the interaction of phonons originating from neighboring heat sources enables more efficient diffusive-like heat dissipation, even from nanoscale heat sources much smaller than the dominant phonon mean free paths. This finding suggests that thermal management in nanoscale systems including integrated circuits might not be as challenging as previously projected. Finally, we demonstrate a unique capability to extract differential conductivity as a function of phonon mean free path in materials, allowing the first (to our knowledge) experimental validation of predictions from the recently developed first-principles calculations.
Journal Article
Ultrafast X-ray Thomson Scattering of Shock-Compressed Matter
by
Morse, Edward C
,
Döppner, Tilo
,
Glenzer, Siegfried H
in
70 PLASMA PHYSICS AND FUSION TECHNOLOGY
,
Astrophysics
,
Coalescence
2008
Spectrally resolved scattering of ultrafast K-α x-rays has provided experimental validation of the modeling of the compression and heating of shocked matter. The elastic scattering component has characterized the evolution and coalescence of two shocks launched by a nanosecond laser pulse into lithium hydride with an unprecedented temporal resolution of 10 picoseconds. At shock coalescence, we observed rapid heating to temperatures of 25,000 kelvin when the scattering spectra show the collective plasmon oscillations that indicate the transition to the dense metallic plasma state. The plasmon frequency determines the material compression, which is found to be a factor of 3, thereby reaching conditions in the laboratory relevant for studying the physics of planetary formation.
Journal Article
A measurement of the equation of state of carbon envelopes of white dwarfs
by
Bachmann, Benjamin
,
Döppner, Tilo
,
Remington, Bruce A.
in
639/766/1960/1134
,
639/766/1960/1135
,
70 PLASMA PHYSICS AND FUSION TECHNOLOGY
2020
White dwarfs represent the final state of evolution for most stars
1
–
3
. Certain classes of white dwarfs pulsate
4
,
5
, leading to observable brightness variations, and analysis of these variations with theoretical stellar models probes their internal structure. Modelling of these pulsating stars provides stringent tests of white dwarf models and a detailed picture of the outcome of the late stages of stellar evolution
6
. However, the high-energy-density states that exist in white dwarfs are extremely difficult to reach and to measure in the laboratory, so theoretical predictions are largely untested at these conditions. Here we report measurements of the relationship between pressure and density along the principal shock Hugoniot (equations describing the state of the sample material before and after the passage of the shock derived from conservation laws) of hydrocarbon to within five per cent. The observed maximum compressibility is consistent with theoretical models that include detailed electronic structure. This is relevant for the equation of state of matter at pressures ranging from 100 million to 450 million atmospheres, where the understanding of white dwarf physics is sensitive to the equation of state and where models differ considerably. The measurements test these equation-of-state relations that are used in the modelling of white dwarfs and inertial confinement fusion experiments
7
,
8
, and we predict an increase in compressibility due to ionization of the inner-core orbitals of carbon. We also find that a detailed treatment of the electronic structure and the electron degeneracy pressure is required to capture the measured shape of the pressure–density evolution for hydrocarbon before peak compression. Our results illuminate the equation of state of the white dwarf envelope (the region surrounding the stellar core that contains partially ionized and partially degenerate non-ideal plasmas), which is a weak link in the constitutive physics informing the structure and evolution of white dwarf stars
9
.
Researchers have measured the equation of state of hydrocarbon in a high-density regime, which is necessary for accurate modelling of the oscillations of white dwarf stars.
Journal Article
Electron Small Polarons and Their Mobility in Iron (Oxyhydr)oxide Nanoparticles
by
Katz, Jordan E.
,
Zarzycki, Piotr
,
Rosso, Kevin M.
in
Absorption spectroscopy
,
Condensed matter: electronic structure, electrical, magnetic, and optical properties
,
Condensed matter: structure, mechanical and thermal properties
2012
Electron mobility within iron (oxyhydr)oxides enables charge transfer between widely separated surface sites. There is increasing evidence that this internal conduction influences the rates of interfacial reactions and the outcomes of redox-driven phase transformations of environmental interest. To determine the links between crystal structure and charge-transport efficiency, we used pump-probe spectroscopy to study the dynamics of electrons introduced into iron(III) (oxyhydr)oxide nanoparticles via ultrafast interfacial electron transfer. Using time-resolved x-ray spectroscopy and ab initio calculations, we observed the formation of reduced and structurally distorted metal sites consistent with small polarons. Comparisons between different phases (hematite, maghemite, and ferrihydrite) revealed that short-range structural topology, not long-range order, dominates the electron-hopping rate.
Journal Article
X-ray linear dichroic ptychography
by
Shapiro, David A.
,
Miao, Jianwei
,
Gentry, Christian
in
4D scanning transmission electron microscopy
,
Animals
,
Anisotropy
2021
Biominerals such as seashells, coral skeletons, bone, and tooth enamel are optically anisotropic crystalline materials with unique nanoscale and microscale organization that translates into exceptional macroscopic mechanical properties, providing inspiration for engineering new and superior biomimetic structures. Using Seriatopora aculeata coral skeleton as a model, here, we experimentally demonstrate X-ray linear dichroic ptychography and map the c-axis orientations of the aragonite (CaCO₃) crystals. Linear dichroic phase imaging at the oxygen K-edge energy shows strong polarization-dependent contrast and reveals the presence of both narrow (< 35°) and wide (>35°) c-axis angular spread in the coral samples. These X-ray ptychography results are corroborated by four-dimensional (4D) scanning transmission electron microscopy (STEM) on the same samples. Evidence of co-oriented, but disconnected, corallite subdomains indicates jagged crystal boundaries consistent with formation by amorphous nanoparticle attachment. We expect that the combination of X-ray linear dichroic ptychography and 4D STEM could be an important multimodal tool to study nano-crystallites, interfaces, nucleation, and mineral growth of optically anisotropic materials at multiple length scales.
Journal Article
Ultrafast X-Ray Pulses from Laser-Produced Plasmas
by
Murnane, Margaret M.
,
Rosen, Mordecai D.
,
Kapteyn, Henry C.
in
70 PLASMA PHYSICS AND FUSION TECHNOLOGY
,
700101 - Fusion Energy- Plasma Research- Confinement, Heating, & Production
,
Braking radiation
1991
A high-temperature plasma is created when an intense laser pulse is focused onto the surface of a solid. An ultrafast pulse of x-ray radiation is emitted from such a plasma when the laser pulse length is less than a picosecond. A high-speed streak camera detector was used to determine the duration of these x-ray pulses, and computer simulations of the plasmas agree with the experimental results. Scaling laws predict that brighter and more efficient x-ray sources will be obtained by the use of more intense laser pulses. These sources can be used for time-resolved x-ray scattering studies and for the development of x-ray lasers.
Journal Article
A new regime of nanoscale thermal transport: Collective diffusion increases dissipation efficiency
by
Jorge N. Hernandez-Charpak
,
Xiaokun Gu
,
Roger W. Falcone
in
high harmonic generation
,
mean free path spectroscopy
,
nanoscale thermal transport
2015
Understanding thermal transport from nanoscale heat sources is important for a fundamental description of energy flow in materials, as well as for many technological applications including thermal management in nanoelectronics and optoelectronics, thermoelectric devices, nanoenhanced photovoltaics, and nanoparticle-mediated thermal therapies. Thermal transport at the nanoscale is fundamentally different from that at the macroscale and is determined by the distribution of carrier mean free paths and energy dispersion in a material, the length scales of the heat sources, and the distance over which heat is transported. Past work has shown that Fourier’s law for heat conduction dramatically overpredicts the rate of heat dissipation from heat sources with dimensions smaller than the mean free path of the dominant heat-carrying phonons. In this work, we uncover a new regime of nanoscale thermal transport that dominates when the separation between nanoscale heat sources is small compared with the dominant phonon mean free paths. Surprisingly, the interaction of phonons originating from neighboring heat sources enables more efficient diffusive-like heat dissipation, even from nanoscale heat sources much smaller than the dominant phonon mean free paths. This finding suggests that thermal management in nanoscale systems including integrated circuits might not be as challenging as previously projected. In conclusion, we demonstrate a unique capability to extract differential conductivity as a function of phonon mean free path in materials, allowing the first (to our knowledge) experimental validation of predictions from the recently developed first-principles calculations.
Journal Article
Simultaneous compression and opacity data from time-series radiography with a Lagrangian marker
by
Bachmann, Benjamin
,
Swift, Damian C
,
Collins, Gilbert W
in
Convergence
,
Data compression
,
Equations of state
2020
Time-resolved radiography can be used to obtain absolute shock Hugoniot states by simultaneously measuring at least two mechanical parameters of the shock, and this technique is particularly suitable for one-dimensional converging shocks where a single experiment probes a range of pressures as the converging shock strengthens. However, at sufficiently high pressures, the shocked material becomes hot enough that the x-ray opacity falls significantly. If the system includes a Lagrangian marker, such that the mass within the marker is known, this additional information can be used to constrain the opacity as well as the Hugoniot state. In the limit that the opacity changes only on shock heating, and not significantly on subsequent isentropic compression, the opacity of shocked material can be determined uniquely. More generally, it is necessary to assume the form of the variation of opacity with isentropic compression, or to introduce multiple marker layers. Alternatively, assuming either the equation of state or the opacity, the presence of a marker layer in such experiments enables the non-assumed property to be deduced more accurately than from the radiographic density reconstruction alone. An example analysis is shown for measurements of a converging shock wave in polystyrene, at the National Ignition Facility.
Shock Hugoniot of diamond from 3 to 80 TPa
by
Bachmann, Benjamin
,
Swift, Damian C
,
Collins, Gilbert W
in
Ablation
,
Atmospheric pressure
,
Compressibility
2022
The principal Hugoniot of carbon, initially diamond, was measured from 3 to 80 TPa (30 to 800 million atmospheres), the highest pressure ever achieved, using radiography of spherically-converging shocks. The shocks were generated by ablation of a plastic coating by soft x-rays in a laser-heated hohlraum at the National Ignition Facility (NIF). Experiments were performed with low and high drive powers, spanning different but overlapping pressure ranges. The radius-time history of the shock, and the profile of mass density behind, were determined by profile-matching from a time-resolved x-ray radiograph across the diameter of the sphere. Above ~50 TPa, the heating induced by the shock was great enough to ionize a significant fraction of K-shell electrons, reducing the opacity to the 10.2 keV probe x-rays. The opacity and mass density were deduced simultaneously using the constraint that the total mass of the sample was constant. The Hugoniot and opacity were consistent with density functional theory calculations of the electronic states and equation of state (EOS), and varied significantly from theoretical Hugoniots based on Thomas-Fermi theory. Theoretical models used to predict the compressibility of diamond ablator experiments at the NIF, producing the highest neutron yields so far from inertial confinement fusion experiments, are qualitatively consistent with our EOS measurements but appear to overpredict the compressibility slightly. These measurements help to evaluate theoretical techniques and constrain wide-range EOS models applicable to white dwarf stars, which are the ultimate evolutionary form of at least 97% of stars in the galaxy.