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At least 271 records · Page 15

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DOE OSTI2021

Signatures of Coherent Phonon Transport in Ultralow Thermal Conductivity Two-Dimensional Ruddlesden–Popper Phase Perovskites

An emerging class of methylammonium lead iodide (MAPbI 3 )-based Ruddlesden-Popper (RP) phase perovskites, BA 2 MA n-1 Pb n I 3n+1 (n = 1-7), exhibit enhanced stability to environmental conditions relative to MAPbI 3 , yet still degrade at elevated temperatures. Here, we experimentally determine the thermal conductivities of these layered RP phases for n = 1-6, where n defines the number of repeated perovskite octahedra per layer. We measure thermal conductivities of 0.37 ± 0.13/0.12, 0.17 ± 0.08/0.07, 0.21 ± 0.05/0.04, and 0.19 ± 0.04/0.03 W/m∙K in thin films of n = 1-4 and 0.08 ± 0.06/0.04, 0.06 ± 0.04/0.03, 0.06 ± 0.03/0.03, and 0.08 ± 0.07/0.04 W/m∙K in single crystals of n = 3-6. With the exception of n = 1, these thermal conductivities are lower than the range of 0.34-0.50 W/m∙K reported for single-crystal MAPbI 3 . Reduced-order lattice dynamics modeling suggests that the initially decreasing trend of thermal conductivity in similarly oriented perovskites with increasing n may result from the transport properties of coherent phonons, emergent from the superstructure, that do not scatter at the interfaces of organic butylammonium chains and perovskite octahedra. Reduced group velocity of coherent phonons in n = 3-6, a consequence of band flattening in the phonon dispersion, is primarily responsible for their ultralow thermal conductivities. Similar effects on thermal conductivity have been experimentally demonstrated in deposited superlattices, but never in naturally defined materials such as RP phases. GIWAXS measurements reveal that higher n RP phase thin films are less orientationally controlled and therefore possess apparently elevated thermal conductivities relative to single crystals of the same n.

2D perovskites↗

DOE OSTI2020

Characterizing Physical Properties of Streambed Interface Sediments Using In Situ Complex Electrical Conductivity Measurements

Streambed sediment physical properties such as surface area, are difficult to quantify in situ but exert a high-level control on a wide range of biogeochemical processes and sorption of contaminants. We introduce the use of complex electrical conductivity (CC) methods (also known as spectral-induced polarization (SIP)) that measure both real and imaginary conductivity to noninvasively and efficiently characterize shallow streambed sediments. We explore the method through synthetic modeling, laboratory, and field measurements to demonstrate the sensitivity of imaginary conductivity to sediment surface area, controlled in part by fine-grained iron oxides produced by anoxic groundwater discharge. Laboratory measurements verify expected relationships between CC parameters and sediment properties. Synthetic modeling using a 1D analytical model illustrates the influence of water layer depth and conductivity on the field CC measurements made at the streambed-stream water interface. Specifically, the inverted sediment imaginary conductivity is less impacted by uncertainty in the water layer depth and conductivity relative to the real conductivity and phase shift. Field CC measurements along a landfill-impacted river reveal discrete streambed zones with enhanced bulk surface area generally corresponding to anoxic groundwater discharge zones with high concentrations of fine-grained iron oxide precipitates.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Intrinsic nanostructure induced ultralow thermal conductivity yields enhanced thermoelectric performance in Zintl phase Eu2ZnSb2

Abstract The Zintl thermoelectric phase Eu 2 ZnSb 2 has a remarkable combination of high mobility and low thermal conductivity that leads to good thermoelectric performance. The key feature of this compound is a crystal structure that has a Zn-site with a 50% occupancy. Here we use comparison of experimental thermal conductivity measurements and first principles thermal conductivity calculations to characterize the thermal conductivity reduction. We find that partial ordering, characterized by local order, but Zn-site disorder on longer scales, leads to an intrinsic nanostructuring induced reduction in thermal conductivity, while retaining electron mobility. This provides a direction for identifying Zintl compounds with ultralow lattice thermal conductivity and good electrical conductivity.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Reversible two-way tuning of thermal conductivity in an end-linked star-shaped thermoset

Polymeric thermal switches that can reversibly tune and significantly enhance their thermal conductivities are desirable for diverse applications in electronics, aerospace, automotives, and medicine; however, they are rarely achieved. Here, we report a polymer-based thermal switch consisting of an end-linked star-shaped thermoset with two independent thermal conductivity tuning mechanisms—strain and temperature modulation—that rapidly, reversibly, and cyclically modulate thermal conductivity. The end-linked star-shaped thermoset exhibits a strain-modulated thermal conductivity enhancement up to 11.5 at a fixed temperature of 60 °C (increasing from 0.15 to 2.1 W m –1 K –1 ). Additionally, it demonstrates a temperature-modulated thermal conductivity tuning ratio up to 2.3 at a fixed stretch of 2.5 (increasing from 0.17 to 0.39 W m –1 K –1 ). When combined, these two effects collectively enable the end-linked star-shaped thermoset to achieve a thermal conductivity tuning ratio up to 14.2. Moreover, the end-linked star-shaped thermoset demonstrates reversible tuning for over 1000 cycles. The reversible two-way tuning of thermal conductivity is attributed to the synergy of aligned amorphous chains, oriented crystalline domains, and increased crystallinity by elastically deforming the end-linked star-shaped thermoset.

42 ENGINEERING↗

DOE OSTI2021

A negative piezo-conductive effect from doped semiconducting polymer thin films

In the past years, piezo-conductive sensors have drawn great attention in both academic and industrial sectors. The piezo-conductive sensors made by inorganic semiconductors exhibited poor mechanical flexibility, restricting their further practical applications. In this study, we report the piezo-conductive sensors by a semiconducting polymer, poly(3,4-ethylenedioxythiophene) doped with tosylate ions (PEDOT:Tos) thin films. Systemically studies indicate that the piezo-conductive response of the PEDOT:Tos thin films is originated from the deformation of the PEDOT crystal cells and the stretched π–π distances induced by Tos. Moreover, the negative piezo-conductive effect, for the first time, is observed from PEDOT:Tos thin film under the pressure. A working mechanism is further proposed to interpret the transient from a positive to a negative piezo-conductive response within the PEDOT:Tos thin films. Our studies offer a facile route to approach effective piezo-conductive sensors based on conjugated polymers.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Conductivity and size quantization effects in semiconductor $$\delta$$-layer systems

Abstract We present an open-system quantum-mechanical 3D real-space study of the conduction band structure and conductive properties of two semiconductor systems, interesting for their beyond-Moore and quantum computing applications: phosphorus $$\delta$$ δ -layers and P $$\delta$$ δ -layer tunnel junctions in silicon. In order to evaluate size quantization effects on the conductivity, we consider two principal cases: nanoscale finite-width structures, used in transistors, and infinitely-wide structures, electrical properties of which are typically known experimentally. For devices widths $$W<10$$ W < 10 nm, quantization effects are strong and it is shown that the number of propagating modes determines not only the conductivity, but the distinctive spatial distribution of the current-carrying electron states. For $$W>10$$ W > 10 nm, the quantization effects practically vanish and the conductivity tends to the infinitely-wide device values. For tunnel junctions, two distinct conductivity regimes are predicted due to the strong conduction band quantization.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Mechanically robust and superior conductive n-type polymer binders for high-performance micro-silicon anodes in lithium-ion batteries

Compared with nanostructured silicon (Si), the Si microparticle (SiMP) has more commercial prospects due to its low cost. However, SiMPs suffer from unavoidable fracture during electrochemical cycling owing to their significant volume change. Here we develop a series of novel n-type conductive polymer binders (CPBs) for SiMP anodes in lithium-ion batteries owing to their superior properties. Extraordinary electrochemical performance of cells with such unique binders could be achieved, which is because these designed polymers contain electron-withdrawing oxadiazole ring groups and easily ionizable sulfonate polar groups, exhibiting excellent ionic conductivity, outstanding wettability to the electrolyte, and improved electronic conductivity after doping. Moreover, the coexistence of rigid and flexible chains enables them to have exceptional strength and ductility. Besides, a unique electrochromic approach has been utilized to investigate the energy gap of the CPBs in n-doping states. The ionic and electronic conductivities of prepared CPBs in an eigenstate and n-doping state have been systematically studied by the electrochemical method, filling the current research gap in this field. Due to the high conductivity of b-POD, the capacity of SiMPs (4200 mA h g –1 ) can be almost entirely released during the first cycle of discharge, while the SiMP anodes prepared with the PAALi or CMC binder show a much lower initial capacity. Here, the high conductivity of b-POD also endows it with better cycling performance than non-conductive binders especially at high current densities, demonstrating its excellent fast-charging ability. More essentially, this work provides polymer binders without any intricate structural designs to obtain high-performance SiMP batteries, significantly enhancing their practical applications.

25 ENERGY STORAGE↗

DOE OSTI2024

Effects of Al concentration on the structure and conductivity of lithium lanthanum zirconium oxide

Cubic Li 7-3x Al x La 3 Zr 2 O 12 (LLZO) is a promising, next-generation solid electrolyte due to its stability with Li-metal and high bulk conductivity (~1 mS cm -1 ). However, the source of the high conductivity is not completely understood. In this work, we address this key knowledge gap through the integration of elemental analysis, neutron diffraction sensitive to Li and O atoms, and impedance spectroscopy to understand the structure–property correlations for LLZO. We show the metal–oxygen framework structure remains constant with variation in Al substitution, resulting in a constant activation energy of ~0.35 eV and little effect on the bulk conductivity. Instead, Li concentration, Al blocking and trapping of mobile defects, and Li–Li nearest neighbor interactions largely control the Al substituted LLZO bulk conductivity, resulting in decreases from 0.73 to 0.22 mS cm -1 as the Al concentration increases from 0.17 to 0.32 mol. These results differ from those of Ta substituted LLZO, where the framework structure and Li–Li site distances play large roles in controlling the conductivity. The increased understanding of the controlling factors of conductivity allows for greater ability to tailor the design of and substitution into the LLZO structure for improved conductivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Effect of surface functional groups on MXene conductivity

In this work, we report the in-plane electron transport in the MXenes (i.e., within the MXene layers) as a function of composition using the density-functional tight-binding method, in conjunction with the non-equilibrium Green’s functions technique. Our study reveals that all MXene compositions have a linear relationship between current and voltage at lower potentials, indicating their metallic character. However, the magnitude of the current at a given voltage (conductivity) has different trends among different compositions. For example, MXenes without any surface terminations (Ti 3 C 2 ) exhibit higher conductivity compared to MXenes with surface functionalization. Among the MXenes with –O and –OH termination, those with –O surface termination have lower conductivity than the ones with –OH surface terminations. Interestingly, conductivity changes with the ratio of –O and –OH on the MXene surface. Our calculated I–V curves and their conductivities correlate well with transmission functions and the electronic density of states around the Fermi level. The surface composition-dependent conductivity of the MXenes provides a path to tune the in-plane conductivity for enhanced pseudocapacitive performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Phonon Olympics: Phonon property and lattice thermal conductivity benchmarking from open-source packages

Three widely used open-source packages for determining phonon properties and lattice thermal conductivities (ALAMODE, phono3py, and ShengBTE) are benchmarked by teams of expert users and the package developers. The phonons for Ge, RbBr, monolayer MoSe 2 , and AlN are modeled at zero temperature, and they scatter through three-phonon and phonon-isotope processes, with thermal conductivities obtained from the linearized Peierls–Boltzmann transport equation with input from density functional theory calculations. Over a wide range of temperatures, the thermal conductivities calculated by the teams fall within at most ±15% of their mean values for each of the four materials. The phonon frequencies, obtained from the harmonic force constants, do not show large differences between the calculations, indicating that the modal heat capacities and group velocities are not responsible for the thermal conductivity variations. It is the lifetimes associated with three-phonon scattering, obtained from the cubic force constants, that drive the variations. The many decisions required to calculate the cubic force constants (e.g., supercell size, atomic displacement, neighbor cutoff, and application of symmetries) make identification of the precise origin of the thermal conductivity variations challenging. The calculated thermal conductivities do not generally show agreement with experimental measurements, which is attributed to the limitations of the density functional theory calculations. Guidance for the development of best practices is provided, which will help to standardize protocols needed for building thermal conductivity databases. The results provide a baseline for future benchmarking of other packages and more advanced calculations.

McGaughey, Alan J. H. [Carnegie Mellon Univ., Pitt↗

DOE OSTI2026

The effect of relative humidity and temperature on the response of stomatal conductance to vapor pressure deficit in tropical trees

Understanding how leaf gas exchange responds to changes in vapor pressure deficit (VPD) is key to predicting tropical forest resilience to climate change. Stomata regulate leaf water and CO2 diffusion, and respond to changes in temperature and relative humidity (RH), two drivers of VPD. At high temperatures, the cuticular pathway may also become significant and participate in the overall leaf conductance. Here, we measured gas exchange under light and dark conditions to investigate the stomatal and cuticular responses to temperature and RH on detached branches in five tropical tree species. Leaf conductance in the dark, when stomata are essentially closed, was not markedly impacted by temperature and RH, suggesting a minimal response of the cuticular pathway to these conditions. We compared six steady-state conductance models incorporating different effects of photosynthesis and evaporative demand on stomatal control. All models performed well (residual standard deviation, σ, < 0.025 mol m-2 s-1), but the best-fitting model (σ = 0.017 mol m-2 s-1) used a nonlinear relationship between photosynthesis and stomatal conductance and incorporated RH rather than vapor pressure difference. All models overestimated the steady-state conductance at high RH. Furthermore, leaf conductance immediately increased after a decrease in RH (wrong-way response), but not after an increase in leaf temperature. This suggests that the mechanisms underlying stomatal response to VPD need further investigation. The non-linear coupling between photosynthetic rate and stomatal conductance indicates a sharper physiological response than previously acknowledged.

Lamour, Julien↗

DOE OSTI2019

Hall viscosity and nonlocal conductivity of gapped graphene

We calculate the Hall viscosity and the nonlocal (i.e., dependent on wave vector q) Hall conductivity of “gapped graphene” (a nontopological insulator with two valleys) in the presence of a strong perpendicular magnetic field. Using the linear-response theory at zero temperature within the Dirac approximation for the Landau levels, we present analytical expressions for both valley and total Hall viscosities and conductivity up to q 2 at all frequencies. Although the final formulas for total Hall viscosity and conductivity are similar to the ones previously obtained for gapless graphene, the derivation reveals a significant difference between the two systems. First of all, both the Hall viscosity and the Hall conductivity vanish when the Fermi level lies in the gap that separates the lowest Landau level in the conduction band from the highest Landau level in the valence band. It is only when the Fermi level is not in the gap that the familiar formulas of gapless graphene are recovered. Second, in the case of gapped graphene, it is not possible (at least, within our present approach) to define a single-valley Hall viscosity: this quantity diverges with a strength proportional to the magnitude of the gap. It is only when both valleys are included that the diverging terms, having opposite signs in the two valleys, cancel out, and the familiar result is recovered. In contrast to this, the nonlocal Hall conductivity is finite in each valley. These results indicate that the Hoyos-Son formula [Phys. Rev. Lett. 108, 066805 (2012)] connecting the Hall viscosity to the coefficient of q 2 in the small-q expansion of the q-dependent Hall conductivity cannot be applied to each valley, but only to the system as a whole. As a result, the problem of defining a “valley Hall viscosity” remains open.

36 MATERIALS SCIENCE↗

NASA NTRS1963

Radiant Heat Transfer to Absorbing Gases Enclosed Between Parallel Flat Plates with Flow and Conduction

An analysis is presented for obtaining two-dimensional temperature profiles and heat transfer in a radiation-absorbing gray gas of uniform absorptivity under the combined influence of thermal radiation, conduction, and gas flow. The gas is enclosed in a channel of infinite width and finite length formed by two semi-infinite parallel flat plates. These plates are black emitting surfaces, and the ends of the channel are formed by porous black surfaces through which the gas can flow into or out of the channel. These porous black end surfaces are used to simulate the radiation environment external to the channel. First, results are obtained for heat transfer between the plates in the absence of both conduction and flow. These results are found to be in good agreement with those obtained for the same conditions by previous workers. Results are then presented for heat transfer between the plates for the case of a radiating and conducting, but stagnant, gas separating the plates. The effects of the interactions between radiation and conduction are discussed. It was found that the heat transfer for combined radiation and conduction in an absorbing gas is slightly greater than the sum for each process taken separately. Finally, results are given for heat transfer from the plates to a flowing, radiating gas in the absence of conduction. The two plates are at the same temperature, and the gas enters the channel with uniform velocity and temperature. The results obtained for this case indicate that the heat transferred to the flowing gas from the constant temperature surfaces goes through a maximum as the absorptivity of the gas increases. This is in qualitative agreement with earlier results obtained by other investigators. All the results are presented in terms of dimensionless parameters, for the sake of generality, and the derivation of the dimensionless parameters, which are indicative of the effects of conduction and flow is presented.

Gray Gas↗

NASA NTRS1977

Electrically Conductive Paints for Satellites

A program was conducted to develop and test electrically conductive paint coatings for spacecraft. A wide variety of organic and inorganic coatings were formulated using conductive binders, conductive pigments, and similar approaches. Z-93, IITRI's standard specification inorganic thermal control coating, exhibits good electrical properties and is a very space-stable coating system. Several coatings based on a conductive pigment (antimony-doped tin oxide) in silicone and silicate binders offer considerable promise. Paint systems using commercially available conductive polymers also appear to be of interest, but will require substantial development. Evaluations were made based on electrical conductivity, paint physical properties, and the stability of spectral reflectance in space environment testing.

Gilligan, J. E.↗

NASA NTRS1983

Conductive damping of coronal motions

Time-dependent motions in the solar corona are subject to modification through conductive transport of thermal energy away from compression regions and into rarefaction regions. The evolution depends on how the energy is introduced - by an essentially thermal perturbation or by a density perturbation. The net effect of thermal conduction is to convert local kinetic energy in the transient into widely distributed thermal energy, which then may in turn be partially converted into kinetic energy of the bulk flow. Local motion in the transient is thereby damped. These effects are modeled here using a numerical solution of the time-dependent solar wind equations for single-fluid thermally conductive flow. The simulations of transient phenomena are made for ordinary collisional thermal conduction and compared with similar simulations done using polytropic flow. Between one and five solar radii, the gross character in the two cases is very similar. However, there are effects with thermal conduction that cannot be modeled with polytropic flow, illustrated here by temperature and velocity forerunners and a delayed and large-amplitude trailing velocity low. If thermal conduction is artificially inhibited by simple reduction of the thermal conduction coefficient, relative velocity amplitudes remain larger in approximate proportion to the amount the coefficient is reduced.

Suess, S. T.↗

NASA NTRS1986

Thermal conductivity of pristine and brominated P-100 fibers

Thermal conductivity of brominated and pristine Union Carbide P-100 graphite fibers in the 30 to 160 C temperature range was determined by measuring thermal conductivities of graphite fiber epoxy composite samples and then excluding the epoxy contribution. A comparative thermal conductivity instrument was used to measure the thermal conductivity of the samples containing fibers. Results showed that the thermal conductivity values were 225 to 370 w/m-K and 215 to 340 w/m-K for pristine and brominated fibers, respectively. Furthermore, the thermal conductivity ratio of brominated to pristine P-100 fibers was 0.89, 0.91, and 0.92 at 55 to 80 C; 108 and 130 C, respectively. Such decrease in thermal conductivity results almost entirely from the 10 percent increase in fiber cross sectional area due to bromination. This result suggests that bromination effects on P-100 fiber structure is small, and that some structural changes, presumably the sharp-angled domain wall becomes less sharp, occurring in the 80 to 108 C temperature range.

Hung, C. C.↗

NASA NTRS1986

Stratospheric conductivity variations over thunderstorms

This paper reports the first in-situ observation of variations in the electrical conductivity over thunderstorms at 26 km altitude. The vector electric field, positive and negative polar conductivity, and optical lightning power/flash were measured by payloads on superpressure balloons in the Southern Hemisphere in early 1984. It is found that in 72 percent of the thunderstorm periods observed (or in 23 of 32 periods) there were clear cases of conductivity variations while the balloons were over the thunderstorms. Examples from two separate balloons at widely separated dates and locations showing both daytime and nighttime events are presented. The conductivity measurements are made with the relaxation technique, and the vector field measurements are based on the double Langmuir probe high-impedance method. It is found that the positive and negative conductivity measurements vary independently and have a different temporal profile than the dc electric field. The polar conductivity variations can exceed a factor of 2 at this altitude. In seven of the nine most intense thunderstorm events the total conductivity increased, while in only one of these nine events did it decrease (one event had no change). Implications of these observations for global current patterns are discussed.

Holzworth, R. H.↗

NASA NTRS1987

Thermal conductivity of pristine and brominated highly graphitized pitch based carbon fibers

Hung, Ching-Cheh↗