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At least 37 records · Page 2

Anisotropic Thermal Transport in Quasi-2D Ruddlesden-Popper Hybrid Perovskite Superlattices

Two-dimensional hybrid metal-halide perovskites (2D-MHPs) have emerged as important solution-processed semiconductors with favorable optical and electronic properties for diverse applications in photovoltaics, optoelectronics, and spintronics. The quasi-2D layered structures, featuring large acoustic impedance mismatches between the organic and inorganic sublattices, are expected to result in distinct and anisotropic thermal transport properties along the cross-plane and in-plane directions. Here, we introduce transducer-free vibrational-pump-visible-probe (VPVP) approaches that enable accurate quantification of anisotropic thermal transport properties in various archetypical single-crystalline 2D-MHPs. Specifically, using VPVP spectroscopy and VPVP microscopy, we measure the anisotropic thermal diffusivities of 2D-MHPs with systematically varied Pb-I octahedral layer thicknesses, as well as organic spacer types and lengths, revealing how these structural parameters alter the cross-plane and in-plane thermal transport properties in distinct ways. While diffuse interface scattering plays an important role in dictating cross-plane thermal transport, in-plane thermal transport is primarily determined by phonon transport within interconnected inorganic layers. Density functional theory incorporating four-phonon scatterings provides further insight into the low thermal conductivity and modest thermal conduction anisotropy in 2D-MHPs. Our work demonstrates a new all-optical and noncontact method, which requires minimal sample preparation and allows direct visualization of cross-plane and in-plane thermal transport, potentially compatible with sample environments. The demonstrated VPVP approaches can advance understanding of thermal transport in 2D-MHPs as well as wide-ranging hybrid and polymeric semiconductors beyond 2D-MHPs.

36 MATERIALS SCIENCE↗

A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide

During reactor operation, nuclear fuels are subject to extreme temperature and irradiation conditions which can significantly degrade the fuel's thermal transport properties. The reduction in thermal conductivity of the fuel as a result of irradiation-induced lattice defects is arguably the most important fuel performance metric in regard to reactor efficiency and safety. Because thorium dioxide (ThO2) is suitable as a model system for more complex materials such as UO2 and its mixed oxides, we present a theoretical investigation of thermal conductivity reduction seen in defect-bearing thorium dioxide and compare directly to experimental measurements. Phonon-mediated thermal transport of the fuel is modeled by a solution to the Boltzmann transport equation (BTE) for phonons. A cluster dynamics (CD) model for lattice defect evolution during irradiation predicts defect densities which are used as input to the BTE for modeling phonon-defect scatterings. Phonon scatterings by lattice defects include those from point defects and vacancy clusters and interstitial clusters of various sizes. The CD model is benchmarked against structural defect characterization of irradiated thorium dioxide using electron microscopy. Thermal conductivity predicted by the BTE model is compared to measured values for irradiated thorium dioxide specimens below room temperature to isolate effects of phonon-defect scattering from intrinsic 3-phonon processes, which dominate at higher temperatures. The computed conductivity values are in partial agreement at temperatures close to room temperature while slight deviations are observed at the lowest measured temperatures, suggesting that implemented phonon-defect scattering cross-section expressions may not be adequate for low temperatures. The presented work provides a necessary investigation of the influence of irradiation induced defects on fuel performance and represents a first step toward a full characterization of phonon mediated thermal transport in irradiated materials with complex defect microstructure.

36 MATERIALS SCIENCE↗

Picosecond magneto-optic thermometry measurements of nanoscale thermal transport in AlN thin films

The thermal conductivity Λ of wide bandgap semiconductor thin films, such as AlN, affects the performance of high-frequency devices, power devices, and optoelectronics. However, accurate measurements of Λ in thin films with sub-micrometer thicknesses and Λ > 100 W m -1 K -1 is challenging. Widely used pump/probe metrologies, such as time–domain thermoreflectance (TDTR) and frequency–domain thermoreflectance, lack the spatiotemporal resolution necessary to accurately quantify thermal properties of sub-micrometer thin films with high Λ. In this work, we use a combination of magneto-optic thermometry and TiN interfacial layers to significantly enhance the spatiotemporal resolution of pump/probe thermal transport measurements. We use our approach to measure Λ of 100, 400, and 1000 nm AlN thin films. We coat AlN thin films with a ferromagnetic thin-film transducer with the geometry of (1 nm-Pt/0.4 nm-Co) x3 /(2 nm-TiN). This PtCo/TiN transducer has a fast thermal response time of <50 ps, which allows us to differentiate between the thermal response of the transducer, AlN thin film, and substrate. For the 100, 400, and 1000 nm thick AlN films, we determine Λ to be 200 ± 80, 165 ± 35, and 300 ± 70 W m -1 K -1 , respectively. We conclude with an uncertainty analysis that quantifies the errors associated with pump/probe measurements of thermal conductivity, as a function of transducer type, thin-film thermal conductivity, and thin-film thickness. Time resolved magneto-optic Kerr effect experiments can measure films that are three to five times thinner than is possible with standard pump/probe metrologies, such as TDTR. This advance in metrology will enable better characterization of nanoscale heat transfer in high thermal conductivity material systems like wide bandgap semiconductor heterostructures and devices.

36 MATERIALS SCIENCE↗

On the role of ion temperature gradient turbulence in driving ion thermal transport in neutral beam injection-heated L-mode plasmas in a superconducting tokamak

In this paper, we report a detailed experimental study of the role of ion-temperature-gradient driven turbulence in driving ion thermal transport in neutral beam injection (NBI)-heated L-mode plasmas in Experimental Advanced Superconducting Tokamak (EAST) (Wan et al 2000 Nucl. Fusion 40 1057) coupled with linear and nonlinear gyrokinetic simulations. Significant ion-scale turbulence k ⟂ < cm −1 (k ⟂ < 1.5, where k ⟂ where is the perpendicular wavenumber and ρ s is the ion gyroradius calculated using local electron temperature T e ), measured with a microwave reflectometer, is observed in the plasma core at for r/a ≈ 0.265 and 0.5 (where r is half the diameter of the closed flux surface at a given radial position, and a is half the diameter of the last closed flux surface). Local linear stability analysis with experimental equilibrium quantities at these two radial locations using the GS2 gyrokinetic code shows that the most unstable ion-scale micro-instability is the ion temperature gradient (ITG) mode. Since the computed maximum ion-scale linear growth rates are larger than the local Waltz-Miller E × B shearing rate (Waltz and Miller 1999 Phys. Plasmas 6 4265), the E × B shear is unable to suppress ion-scale turbulence, consistent with the experimental observation of ion-scale turbulence. Experimental ion and electron thermal transports, calculated with power balance analysis, are both anomalous with ion thermal transport being the dominant channel. Nonlinear gyrokinetic simulations using the electrostatic global particle-in-cell gyrokinetic tokamak simulation (GTS) code (Weixing Wang et al 2010 Phys. Plasmas 17 072511) show good quantitative agreement between predicted ion thermal transport and that from the power balance analysis. These results demonstrate for the first time the important role of ITG turbulence in driving thermal transport in NBI-heated L-mode plasmas in EAST, showing the effectiveness of GTS code in simulating electrostatic turbulence in EAST and the need of suppressing ITG turbulence to improve energy confinement in EAST.

Sun, P. J. [Chinese Academy of Sciences (CAS), Hef↗

MESOSCALE THERMAL TRANSPORT MEASUREMENTS OF MULTI-PHASE AND POROUS NUCLEAR FUELS USING A SQUARE-WAVE PULSE THERMOREFLECTANCE TECHNIQUE

The safe and efficient operation of nuclear reactors require accurate knowledge of peak temperatures in the fuel assemblies. The temperature profiles are governed by the thermal transport properties of the fuel, namely the thermal conductivities (k) and thermal diffusivities (D). These values can be very difficult to measure as they are known to vary considerably from the measured bulk values of the fresh fuel, and quickly degrade with increasing burnup [1 -3] . Laser-based techniques have been effectively used for non-destructive and non-contact thermal transport measurements of a wide variety of materials, including nuclear materials [4-6] that would otherwise prove too hazardous or difficult to measure otherwise. In this study, a new thermoreflectance technique known as square-pulse transient thermoreflectance (SPTR) is described and used to determine the mesoscale thermal diffusivity of both uranium sesquisilicide (U3Si2) and uranium nitride (UN) phases in a composite fuel with micron level spatial resolution [7]. This technique employs a rapid train of square-wave pulses from an excitation laser to create a periodic heat flux on a gold coated sample surface. Surface adsorption results in transient film temperatures and hence rapid fluctuations in thermoreflectance that can be measured via a detection laser coupled with a digital oscilloscope. The lasers are coaxially focused on the sample surface, allowing for a sample measurement area of a single convolved laser spot size (~2 µm). A sensitivity analysis was conducted to identify key measurement parameters of this technique using reference materials with a range of thermal conductivities comparable to those of both ceramic, composite, and metal nuclear fuel types (1.4 – 27.2 W/m-K). The reference materials were measured using the new technique as well as a spatial-domain thermoreflectance technique (SDTR) previously reported for a comparison [8]. Additionally, measurements of several U3Si2 and UN phase regions of a polished UN/U3Si2 (70/30 vol.%) sample were taken, and the resulting calculated D values are reported, with both techniques showing excellent agreement between samples. This technique was used to scan a multiphase region at 5 micron increments to generate a local diffusivity map, demonstrating the utility of the techniques for measuring thermal transport properties in specimens with precipitates and secondary phases. Furthermore, the technique is currently being applied to measure thermal properties of Fast Flux Test Reactor (FFTR) irradiated metal fuel specimens whose porous microstructure make it very difficult to measure using other techniques. Comparison of the local scale measurements are compared with the pre-irradiated fuel samples to show the degradation of thermal transport in fuels due to pores from fission gas bubbles and other irradiation induced defects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analytic investigation of combined effects of anisotropic thermal transport and energetic particles on stability of resistive plasma resistive wall mode

The combined effects of anisotropic thermal transport and trapped energetic particles (EPs) on the stability of the resistive plasma resistive wall mode (RPRWM) are investigated by an energy-principle based analytical model. The results qualitatively confirm that of a recent toroidal modeling study [Bai et al., Phys. Plasmas 27, 072502 (2020)], in which the thermal transport can stabilize the RPPWM depending on the parameters of both the plasma equilibrium and energetic particles. The analytical model predicts a complete stabilization of the RPRWM in highly resistive plasmas, at sufficiently high EPs’ pressure, and finite plasma flow. The stabilizing effect of thermal transport originates from its enhancement of energy dissipations associated with both the resistive layer and the trapped energetic particles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Phonon Thermal Transport in UO 2 via Self-Consistent Perturbation Theory

Computing thermal transport from first-principles in UO 2 is complicated due to the challenges associated with Mott physics. Here, we use irreducible derivative approaches to compute the cubic and quartic phonon interactions in UO 2 from first principles, and we perform enhanced thermal transport computations by evaluating the phonon Green’s function via self-consistent diagrammatic perturbation theory. Our predicted phonon lifetimes at T = 600 K agree well with our inelastic neutron scattering measurements across the entire Brillouin zone, and our thermal conductivity predictions agree well with previous measurements. Finally, both the changes due to thermal expansion and self-consistent contributions are nontrivial at high temperatures, though the effects tend to cancel, and interband transitions yield a substantial contribution.

36 MATERIALS SCIENCE↗

Phonon-Spin Scattering from Unpaired f-electrons in U atoms and It’s Influence on Thermal Transport in Uranium-doped Thorium Dioxide Single Crystals

In this work, impact of low level of uranium (U) atom substitution on thermal conductivity of thorium dioxide (ThO2) is investigated. ThO2 is an electronic insulator with a wide optical band-gap and no unpaired electrons whose thermal transport is governed by phonons. U-substitution introduces unpaired f-electrons resulting in paramagnetic behavior of U-ThO2 at room temperature, which significantly suppresses its thermal conductivity. A single crystal of U-ThO2 with graded composition of U is grown using a hydrothermal synthesis method, and thermal conductivity measurements are performed in regions with uniform composition of U at levels of 0%, 6%, 9% and 16%. Measured thermal conductivity profiles over 77–300 K temperature range are analyzed using an analytical expression for phonon-mediated thermal transport based on Klemens-Callaway model. Temperature dependent thermal conductivity is found to deviate significantly from the Rayleigh scattering trend expected for a simple substitutional point defect with a small perturbation to mass and interatomic forces. With the resonant scattering term, observed large suppression of thermal conductivity at low temperatures can be closely reproduced. Additionally, the extracted phonon-spin coupling constants imply a nonlinear relation of phonon-spin interaction intensity with respect to U doping percentage. Our study reveals how phonon-spin scattering contributed by unpaired f-electrons in U atoms influences thermal transport in the U-ThO2 system.

36 - MATERIALS SCIENCE↗

Ultimate Suppression of Thermal Transport in Amorphous Silicon Nitride by Phononic Nanostructure.

Engineering the thermal conductivity of amorphous materials is highly essential for the thermal management of future electronic devices. Here, we demonstrate the impact of ultrafine nanostructuring on the thermal conductivity reduction of amorphous silicon nitride (a-Si3N4) thin films, in which the thermal transport is inherently impeded by the atomic disorders. Ultrafine nanostructuring with feature sizes below 20 nm allows us to fully suppress contribution of the propagating vibrational modes (propagons), leaving only the diffusive vibrational modes (diffusons) to contribute to thermal transport in a-Si3N4. A combination of the phonon-gas kinetics model and the Allen-Feldmann theory reproduced the measured results without any fitting parameters. The thermal conductivity reduction was explained as extremely strong diffusive boundary scattering of both propagons and diffusIons. These findings give rise to substantial tunability of thermal conductivity of amorphous materials, which enables us to provide better thermal solutions in microelectronic devices.

Tambo, Naoki↗

Lattice thermal transport in two-dimensional alloys and fractal heterostructures

Abstract Engineering thermal transport in two dimensional materials, alloys and heterostructures is critical for the design of next-generation flexible optoelectronic and energy harvesting devices. Direct experimental characterization of lattice thermal conductivity in these ultra-thin systems is challenging and the impact of dopant atoms and hetero-phase interfaces, introduced unintentionally during synthesis or as part of deliberate material design, on thermal transport properties is not understood. Here, we use non-equilibrium molecular dynamics simulations to calculate lattice thermal conductivity of $${\mathrm {(Mo|W)Se_2}}$$ ( Mo | W ) Se 2 monolayer crystals including $${\mathrm {Mo}}_{1-x}{\mathrm {W}}_x{\mathrm {Se_2}}$$ Mo 1 - x W x Se 2 alloys with substitutional point defects, periodic $${\mathrm {MoSe_2}|\mathrm {WSe_2}}$$ MoSe 2 | WSe 2 heterostructures with characteristic length scales and scale-free fractal $${\mathrm {MoSe_2}}|{\mathrm {WSe_2}}$$ MoSe 2 | WSe 2 heterostructures. Each of these features has a distinct effect on phonon propagation in the crystal, which can be used to design fractal and periodic alloy structures with highly tunable thermal conductivities. This control over lattice thermal conductivity will enable applications ranging from thermal barriers to thermoelectrics.

42 ENGINEERING↗

Sample-dependent and sample-independent thermal transport properties of α – RuCl 3

In this study, we investigated the thermal transport properties of two α–RuCl 3 crystals with different degrees of stacking disorder to understand the origin of the previously reported oscillatory feature in the field dependence of thermal conductivity. Crystal I shows only one magnetic order around 13 K, which is near the highest T N for α–RuCl 3 with stacking faults. Crystal II has less stacking disorder, with a dominant heat capacity at 7.6 K along with weak anomalies at 10 and 13 K. In the temperature and field dependence of thermal conductivity, no obvious anomaly was observed to be associated with the magnetic order around 13 K for either crystal or around 10 K for crystal II. Crystal II showed clear oscillations in the field dependence of thermal conductivity, while crystal I did not. For crystal I, an L-shaped region in the temperature-field space was observed where thermal Hall conductivity κ xy /T is within ±20% of the half quantized thermal Hall conductivity κ HQ /T, while for crystal II, κ xy /T reaches κ HQ /T only in the high field and high temperature regime with no indication of a plateau at κ HQ /T. Our thermal conductivity data suggest the oscillatory features are inherent to the zigzag ordered phase with T N near 7 K. Our planar thermal Hall effect measurements suggest the sensitivity of this phenomena to stacking disorder. Overall, our results highlight the importance of understanding and controlling crystallographic disorder for obtaining and interpreting intrinsic thermal transport properties in α–RuCl 3 .

36 MATERIALS SCIENCE↗

Giant quantum oscillations in thermal transport in low-density metals via electron absorption of phonons

Oscillations of conductance observed in strong magnetic fields are a striking manifestation of the quantum dynamics of charge carriers in solids. The large charge carrier density in typical metals sets the scale of oscillations in both electrical and thermal conductivity, which characterize the Fermi surface. In semimetals, thermal transport at low-charge carrier density is expected to be phonon dominated, yet several experiments observe giant quantum oscillations in thermal transport. This raises the question of whether there is an overarching mechanism leading to sizable oscillations that survives in phonon-dominated semimetals. In this work, we show that such a mechanism exists. It relies on the peculiar phase-space allowed for phonon scattering by electrons when only a few Landau levels are filled. Our measurements on the Dirac semimetal ZrTe 5 support this counterintuitive mechanism through observation of pronounced thermal quantum oscillations, since they occur in similar magnitude and phase in directions parallel and transverse to the magnetic field. Our phase-space argument applies to all low-density semimetals, topological or not, including graphene and bismuth. Our work illustrates that phonon absorption can be leveraged to reveal degrees of freedom through their imprint on longitudinal thermal transport.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Development of a data-driven neural network model for electron thermal transport in NSTX

A data-driven electron thermal transport neural network (ETT-NN) model, trained on TRANSP interpretative analysis results of National Spherical Torus Experiment (NSTX), was developed to enable faster and more accurate ETT computation for spherical tokamaks (STs). The model incorporates both convolutional NNs and recurrent NNs, allowing it to simultaneously account for the spatial and temporal non-localities and multi-scale features of turbulent transport, which have been considered only in a limited manner in conventional models. The model was validated through interpretative analysis and predictive simulations using Tokamak Reactor Integrated Automated Suite for Simulation and Computation, demonstrating relatively high accuracy. Additionally, parameter scans were performed on test discharges known to exhibit specific turbulent modes, such as microtearing mode, trapped electron mode, kinetic ballooning mode, and electron temperature gradient mode. The scanning results revealed that the ETT-NN model exhibits the same trends as those observed in conventional gyrokinetic simulations or theories, while also capturing the global nature of turbulent transport, indicating that the data-driven model accurately reflects the underlying physical characteristics. Furthermore, due to the dimensionless nature of the model, we can feasibly expand its applicability by incorporating data from other devices and uncovering the characteristics of ETT in STs in the future.

NSTX↗

Microtearing instabilities and electron thermal transport in low and high collisionality NSTX discharges

Microtearing mode (MTM) real frequency, growth rate, magnetic fluctuation amplitude and resulting electron thermal transport are studied in systematic NSTX scans of relevant plasma parameters. Here, the dependency of the MTM real frequency and growth rate on plasma parameters, suitable for low and high collision NSTX discharges, is obtained by using the reduced MTM transport model. The plasma parameter dependencies are compared and found to be consistent with the results obtained from MTM using the Gyrokinetic GYRO code. The scaling trend of collision frequency and plasma beta is found to be consistent with the global energy confinement trend observed in the NSTX experiment. The strength of the magnetic fluctuation is found to be consistent with the gyrokinetic estimate. In earlier studies, it was found that the version of the Multi-Mode (MM) anomalous transport model, which did not contain the effect of MTMs, provided an appropriate description of the electron temperature profiles in standard tokamak discharges and not in spherical tokamaks. When the MM model, which involves transport associated with MTMs, is incorporated in the TRANSP code and is used in the study of electron thermal transport in NSTX discharges, it is observed that the agreement with the experimental electron temperature profile is substantially improved.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Characterization of thermal transport and evolution of Au plasma in ICF experiments by Thomson scattering

Here, this paper demonstrates the capability of optical Thomson scattering (OTS) to measure thermal transport, and provides support to radiation hydrodynamic and kinetic simulations of electron thermal transport and plasma evolution. OTS theory and plasma simulations are applied to the interpretation of experimental measurements of laser-produced plasma from spherical gold targets on the OMEGA laser facility. The dynamical form factor, S($\vec{k}$, ω), of electron density fluctuations that is used in the fitting of Thomson scattering spectra includes ion–ion collisions and effects of non-Maxwellian distribution functions. OTS measurements and their interpretation are consistent with the nonlocal transport model in radiation hydrodynamic simulations as well as with kinetic simulations in the second half of the probe pulse duration. In particular, the reversal of heat transport during cooling is observed to be consistent with simulations, while some discrepancies are noted during the initial heating of the Au targets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Thermal transport measurements through the charge density wave transition in CsV 3 Sb 5

We study thermal transport and thermalization in single crystals of CsV 3 Sb 5 through the CDW transition by directly measuring thermal diffusivity (D), thermal conductivity (κ), specific heat (c), and resistivity (ρ). Commensurate with previous reports, we observe a sharp, narrow anomaly in specific heat associated with a first-order transition that results in a CDW state below ~94 K. While a corresponding sharp anomaly in thermal diffusivity is also observed, resistivity and thermal conductivity only exhibit small steps at the transition, where the feature is sharp for resistivity and broader for thermal conductivity. Scrutinizing the thermal Einstein relation κ = cD, we find that this relation is generally satisfied, except in the narrow two-phase regime of the putative first-order transition. Here, the Wiedemann-Franz law as well seems to work outside the two-phase regime, where strong resemblance between the specific heat and the resistivity derivative below the transition may point to a concurrent emergence of a secondary electronic order parameter.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thermal transport across nanoscale damage profile in sapphire irradiated by swift heavy ions

In this work, we studied the degradation of thermal conductivity in single crystal sapphire (α-Al 2 O 3 ) irradiated by 167 MeV Xe swift heavy ions (SHIs) over the multiple fluences in the range of 10 12 –10 14 ions/cm 2 . Thermal conductivity was measured primarily in the cross-plane direction using a noncontact ultrafast optical pump-probe technique called picosecond time domain thermoreflectance (TDTR). Multiple samples with variable ion fluences allowed us to probe distinct regions resulting from different regimes of microstructure evolution caused by electronic energy loss. By tuning the penetration depth of the thermal waves using different modulation frequencies, two regions with distinct conductivities were identified and the values of which were found to be consistent with phonon-mediated thermal transport models while the microstructure was confirmed by electron microscopy characterization. These damaged regions were determined to be a several micrometer thick ion track region and several tens of nanometer-thick amorphous layer present only above 5.0 × 10 13 ions/cm 2 . These results demonstrate the applicability of TDTR to resolve thermal transport behavior in SHI irradiated oxides having nonhomogeneous damage profile on a nanometer scale. The presented approach facilitates future studies aiming at resolving the impact of distinct damage resulting from electronic and nuclear stopping regimes under irradiation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Thermal Transport Model for Heat Sink Design

A document discusses the development of a finite element model for describing thermal transport through microcalorimeter arrays in order to assist in heat-sinking design. A fabricated multi-absorber transition edge sensor (PoST) was designed in order to reduce device wiring density by a factor of four. The finite element model consists of breaking the microcalorimeter array into separate elements, including the transition edge sensor (TES) and the silicon substrate on which the sensor is deposited. Each element is then broken up into subelements, whose surface area subtends 10 10 microns. The heat capacity per unit temperature, thermal conductance, and thermal diffusivity of each subelement are the model inputs, as are the temperatures of each subelement. Numerical integration using the Finite in Time Centered in Space algorithm of the thermal diffusion equation is then performed in order to obtain a temporal evolution of the subelement temperature. Thermal transport across interfaces is modeled using a thermal boundary resistance obtained using the acoustic mismatch model. The document concludes with a discussion of the PoST fabrication. PoSTs are novel because they enable incident x-ray position sensitivity with good energy resolution and low wiring density.

Chervenak, James A.↗