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  1. Collective Energy Transport of Excitons in Two-dimensional Materials

    Electronic thermal transport and thermoelectric measurements are pursued in this project to obtain unique insights into the unusual collective energy transport behaviors in two-dimensional (2D) heterostructures. Electronic thermal transport and thermoelectric measurements are essential techniques for characterizing bulk superconductors by probing the heat-carrying quasi-particles. Thermoelectric and electronic thermal transport measurements are expanded in this work beyond bulk systems to probe interactions among electrons, holes, and phonons in 2D heterostructures. In one experiment, a microbridge platform is advanced to demonstrate field-effect resistive-thermometry measurements of the electronic thermal conductivity of graphene heterostructures. Together with first principles theoretical calculations and analytical models, themore » experimental results suggest that tunable electron coupling with flexural phonons provides a knob to control quantum matters in graphene heterostructures with broken reflection symmetry. In another experiment, the Seebeck coefficient (S) is measured to probe interlayer interactions in electron-hole bilayers that are predicted to give rise to the emergence of a variety of correlated states. As a measure of the entropy, the measured S reveals the signature of electric injection of interlayer excitons in transition metal dichalcogenide (TMD) structures.« less
  2. Differential multi-probe thermal transport measurements of multi-walled carbon nanotubes grown by chemical vapor deposition

    Carbon nanotubes (CNTs) are quasi-one dimensional nanostructures that display both high thermal conductivity for potential thermal management applications and intriguing low-dimensional phonon transport phenomena. In comparison to the advances made in the theoretical calculation of the lattice thermal conductivity of CNTs, thermal transport measurements of CNTs have been limited by either the poor temperature sensitivity of Raman thermometry technique or the presence of contact thermal resistance errors in sensitive two-probe resistance thermometry measurements. Here we report advances in a multi-probe measurement of the intrinsic thermal conductivity of individual multi-walled CNT samples that are transferred from the growth substrate onto themore » measurement device. The sample-thermometer thermal interface resistance is directly measured by this multi-probe method and used to model the temperature distribution along the contacted sample segment. The detailed temperature profile helps to eliminate the contact thermal resistance error in the obtained thermal conductivity of the suspended sample segment. A differential electro-thermal bridge measurement method is established to enhance the signal-to-noise ratio and reduce the measurement uncertainty by over 40%. The obtained thermal resistances of multiple suspended segments of the same MWCNT samples increase nearly linearly with increasing length, revealing diffusive phonon transport as a result of phonon-defect scattering in these MWCNT samples. The measured thermal conductivity increases with temperature and reaches up to 390 ± 20 W m–1 K–1 at room temperature for a 9-walled MWCNT. In conclusion, theoretical analysis of the measurement results suggests submicron phonon mean free paths due to extrinsic phonon scattering by extended defects such as grain boundaries. The obtained thermal conductivity is decreased by a factor of 3 upon electron beam damage and surface contamination of the CNT sample.« less
  3. Tunable electron–flexural phonon interaction in graphene heterostructures

    Peculiar electron-phonon interaction characteristics underpin the ultrahigh mobility, electron hydrodynamics, superconductivity, and superfluidity observed in graphene heterostructures. Here, the Lorenz ratio (L) between the electronic thermal conductivity and the product of the electrical conductivity and temperature provides unique insight into electron-phonon interactions that is inaccessible to past graphene measurements. Here we show an unusual L peak in degenerate graphene near 60 Kelvin and decreased peak magnitude with increased mobility. When combined with ab initio calculations of the many-body electron-phonon self-energy and analytical models, this experimental observation reveals that broken reflection symmetry in graphene heterostructures can relax a restrictive selection rulemore » to allow quasielastic electron coupling with an odd number of flexural phonons, contributing to the increase of L toward the Sommerfeld limit at an intermediate temperature sandwiched between the low-temperature hydrodynamic regime and the inelastic electron-phonon scattering regime above 120 Kelvin. In contrast to past practices of neglecting flexural phonon contributions to transport in two-dimensional materials, this work suggests that tunable electron-flexural phonon coupling can provide a handle to control quantum matter at the atomic scale, such as magic angle twisted bilayer graphene where low-energy excitations may mediate Cooper pairing of flat-band electrons.« less
  4. Reexamination of hydrodynamic phonon transport in thin graphite

    The recent hydrodynamic phonon transport theory for graphitic materials has been supported by the measurements of the second sound at temperatures up to about 100 K. When boundary scattering becomes comparable to momentum-conserving normal phonon scattering processes that are responsible for phonon hydrodynamics, Poiseuille phonon flow phenomena can emerge to give rise to unique size-dependent thermal conductivity in thin graphite. Here, we examine the thickness range for the Poiseuille phonon flow to become observable in thin graphite with the use of both deviational Monte Carlo simulation of the Peierls-Boltzmann transport equation and four-probe thermal transport measurements. As the basal-plane thermalmore » conductivity calculated by prior first-principles theories saturates to the graphite value when the thickness is increased to five graphene layers, the phonon dispersion of graphite is used in the current calculations of thin graphite of micrometer thickness and a 23-layer thick ultrathin graphite (UTG) sample. The calculations show that diffuse surface scattering by surface defects can lead to Poiseuille phonon flow at 50 K in thin graphite with the thickness close to several micrometers but not in the 65 μm thin graphite and 23-layer UTG, where phonon scattering by the top and bottom surfaces become, respectively, much less and more frequent than the normal processes. In addition, the calculation results with the bulk graphite dispersion and diffuse surface scattering show decreased basal-plane thermal conductivity with decreasing thickness, opposite to recent thermocouple measurements of thin graphite samples. In comparison, the calculation results reveal that partially diffuse surface defect scattering can yield the four-probe measurement results of UTG samples, which are prepared here with an improved process to minimize surface contamination.« less
  5. Pure Spin Current and Magnon Chemical Potential in a Nonequilibrium Magnetic Insulator

    Nonequilibrium phenomena are ubiquitous in nature and in a wide range of systems, including cold atomic gases and solid-state materials. While these phenomena are challenging to describe both theoretically and experimentally, they are essential for the fundamental understanding of many-body systems and practical devices. In the context of spintronics, when a magnetic insulator (MI) is subjected to a thermal gradient, a pure spin current is generated in the form of magnons without the presence and dissipation of a charge current—attractive for reducing energy consumption and central to the emerging field of spin caloritronics. However, the experimental methods for directly quantifyingmore » a spin current in insulators and for probing local phonon-magnon nonequilibrium and the associated magnon chemical potential are largely missing. Here, we apply a heating laser to generate a thermal gradient in the MI yttrium iron garnet (YIG), Y3Fe5O12, and evaluate two components of the spin current, driven by temperature and chemical potential gradients, respectively. The experimental method and theory approach for evaluating quasiparticle chemical potential can be applied for analogous phenomena in other many-body systems.« less
  6. Enhanced Low-Temperature Thermoelectric Performance in (PbSe)1+δ(VSe2)1 Heterostructures due to Highly Correlated Electrons in Charge Density Waves

    We explore the effect of charge density wave (CDW) on the in-plane thermoelectric transport properties of (PbSe)1+δ(VSe2)1 and (PbSe)1+δ(VSe2)2 heterostructures. In (PbSe)1+δ(VSe2)1 we observe an abrupt 86% increase in the Seebeck coefficient, 245% increase in the power factor, and a slight decrease in resistivity over the CDW transition. This behavior is not observed in (PbSe)1+δ(VSe2)2 and is rather unusual compared to the general trend observed in other materials. The abrupt transition causes a deviation from the Mott relationship through correlated electron states. Raman spectra of the (PbSe)1+δ(VSe2)1 material show the emergence of additional peaks below the CDW transition temperature associatedmore » with VSe2 material. Temperature-dependent in-plane X-ray diffraction (XRD) spectra show a change in the in-plane thermal expansion of VSe2 in (PbSe)1+δ(VSe2)1 due to lattice distortion. Here, the increase in the power factor and decrease in the resistivity due to CDW suggest a potential mechanism for enhancing the thermoelectric performance at the low temperature region.« less
  7. Phonon interaction with ripples and defects in thin layered molybdenum disulfide

    Compared to other extrinsic phonon scattering mechanisms such as surface and interior defects, phonon scattering and lattice thermal resistance due to structural rippling in few-layer two-dimensional (2D) materials are under-examined. Here, the temperature-dependent basal-plane thermal conductivities (κ) of one rippled and four flat molybdenum disulfide (MoS2) samples are measured using a four-probe thermal transport measurement method. A flat 18 nm thick sample and a rippled 20 nm thick sample show similar peak κ values of 122 ± 17 and 129 ± 19 W m–1 K–1, respectively. In comparison, a 32 nm thick flat sample has a peak κ value ofmore » only 58 ± 11 W m–1 K–1 despite having an increased thickness. The peak thermal conductivities of the five samples decrease with increasing integrated Raman intensity caused by defects in the frequency range of the phonon bandgap in MoS2. In conjunction with the experimental findings, theoretical calculations of the temperature-, thickness-, strain-, and defect-dependent κ of thin MoS2 layers reveal the importance of interior defect scattering over scattering from compression-induced ripples and surface defects in these samples. Furthermore, the results further clarify the conditions where ripples are important in determining the basal plane thermal resistance in layered systems.« less
  8. Large Reduction of Hot Spot Temperature in Graphene Electronic Devices with Heat-Spreading Hexagonal Boron Nitride

    Not provided.
  9. Enhanced thermoelectric efficiency in topological insulator Bi2Te3 nanoplates via atomic layer deposition-based surface passivation

    We report in-plane thermoelectric measurements of Bi2Te3 nanoplates, a typical topological insulator with Dirac-like metallic surface states, grown by chemical vapor deposition. The as-grown flakes exposed to ambient conditions exhibit relatively small thermopowers around -34 μV/K due to unintentional surface doping (e.g., gas adsorption and surface oxidation). After removal of the unintentional surface doping and surface passivation by deposition of 30 nm of Al2O3 using atomic layer deposition (ALD), the Seebeck coefficient of these flakes increases by a factor of 5× to -169 μV/K. We believe that the ALD-based surface passivation can prevent the degradation of the thermoelectric properties causedmore » by gas adsorption and surface oxidation processes, thus, reducing the unintentional doping in the Bi2Te3 and increasing the Seebeck coefficient. The high surface-to-volume ratio of these thin (~10 nm thick) nanoplates make them especially sensitive to surface doping, which is a common problem among nanomaterials in general. An increase in the sample resistance is also observed after the ALD process, which is consistent with the decrease in doping.« less
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