Xiulin Ruan

Thermal Conductivity and Thermal Rectification in Graphene Nanoribbons: A Molecular Dynamics Study

We have used molecular dynamics to calculate the thermal conductivity of symmetric and asymmetric graphene nanoribbons (GNRs) of several nanometers in size (up to approximately 4 nm wide and approximately 10 nm long). For symmetric nanoribbons, the calculated thermal conductivity (e.g., approximately 2000 W/m-K at 400 K for a 1.5 nm x 5.7 nm zigzag GNR) is on the similar order of magnitude of the experimentally measured value for graphene. We have investigated the effects of edge chirality and found that nanoribbons with zigzag edges have appreciably larger thermal conductivity than nanoribbons with armchair edges. For asymmetric nanoribbons, we have found significant thermal rectification. Among various triangularly shaped GNRs we investigated, the GNR with armchair bottom edge and a vertex angle of 30 degrees gives the maximal thermal rectification. We also studied the effect of defects and found that vacancies and edge roughness in the nanoribbons can significantly decrease the thermal conductivity. However, substantial thermal rectification is observed even in the presence of edge roughness.

Tuning the thermal conductivity of graphene nanoribbons by edge passivation and isotope engineering: A molecular dynamics study

Using classical molecular dynamics simulation, we have studied the effect of edge-passivation by hydrogen (H-passivation) and isotope mixture (with random or superlattice distributions) on the thermal conductivity of rectangular graphene nanoribbons (GNRs) (of several nanometers in size). We find that the thermal conductivity is considerably reduced by the edge H-passivation. We also find that the isotope mixing can reduce the thermal conductivities, with the superlattice distribution giving rise to more reduction than the random distribution. These results can be useful in nanoscale engineering of thermal transport and heat management using GNRs.

Reduction of spectral phonon relaxation times from suspended to supported graphene

We have performed molecular dynamics simulations with phonon spectral analysis to predict the mode-wise phonon relaxation times (RT) of suspended and supported graphene at room temperature, and the findings are consistent with recent optical measurements. For acoustic phonons, RTs reduce from up to 50 ps to less than 5 ps when graphene is put on silicon dioxide substrate. Similarly, optical phonon RTs reduce by half when supported. Stronger interfacial bonding is found to result in more RT reduction. Our results provide a fundamental understanding at the spectral phonon property level for the observed thermal conductivity reduction in supported graphene.We perform molecular dynamics (MD) simulations with phonon spectral analysis aiming at understanding the two dimensional (2D) thermal transport in suspended and supported graphene. Within the framework of equilibrium MD simulations, we perform spectral energy density (SED) analysis to obtain the lifetime of individual phonon modes. The per-mode contribution to thermal conductivity is then calculated to obtain the lattice thermal conductivity in the temperature range 300-650 K. In contrast to prior studies, our results suggest that the contribution from out-of-plane acoustic (or ZA) branch to thermal conductivity is around 25-30% in suspended single-layer graphene (SLG) at room temperature. The thermal conductivity is found to reduce when SLG is put on amorphous SiO2 substrate. Such reduction is attributed to the strengthened scattering in all phonon modes in the presence of the substrate. Among them, ZA modes are mostly affected with their contribution to thermal conductivity reduced to around 15%. As a result, thermal transport is dominated by in-plane acoustic phonon modes in supported SLG.

Thermal Transport in Graphene Nanostructures: Experiments and Simulations

a Birck Nanotechnology Center, Purdue University, West Lafayette, IN 47907 b School of Electrical and Computer Engineering, Purdue University, West Lafayette, IN 47907 c Department of Mechanical Engineering, Iowa State University, Ames, IA 50011 d School of Physics, Georgia Institute of Technology, Atlanta, GA 30332 e Department of Electrical and Computer Engineering, University of Houston, Houston, Texas 77204 f Department of Physics, Purdue University, West Lafayette, IN 47907 g School of Mechanical Engineering, Purdue University, West Lafayette, IN 47907

Phonon Lateral Confinement Enables Thermal Rectification in Asymmetric Single-Material Nanostructures

We show that thermal rectification (TR) in asymmetric graphene nanoribbons (GNRs) is originated from phonon confinement in the lateral dimension, which is a fundamentally new mechanism different from that in macroscopic heterojunctions. Our molecular dynamics simulations reveal that, though TR is significant in nanosized asymmetric GNRs, it diminishes at larger width. By solving the heat diffusion equation, we prove that TR is indeed absent in both the total heat transfer rate and local heat flux for bulk-size asymmetric single materials, regardless of the device geometry or the anisotropy of the thermal conductivity. For a deeper understanding of why lateral confinement is needed, we have performed phonon spectra analysis and shown that phonon lateral confinement can enable three possible mechanisms for TR: phonon spectra overlap, inseparable dependence of thermal conductivity on temperature and space, and phonon edge localization, which are essentially related to each other in a complicated manner. Under such guidance, we demonstrate that other asymmetric nanostructures, such as asymmetric nanowires, thin films, and quantum dots, of a single material are potentially high-performance thermal rectifiers.

Multiple scattering and nonlinear thermal emission of yb3+, Er3+:Y2O3 nanopowders

Radiation transport and multiple scattering calculations are presented and compared with experimental observations to characterize light attenuation in high emissivity nanopowders irradiated with low power laser light at room temperature, and to explain the associated white light emission and the onset of melting. Using radiation tuned to an absorption resonance of Yb3+ dopants in Y2O3 nanopowder, we observed the onset of intense blackbody emission above a well-defined intensity threshold. Local melting of the compact above threshold leads to the formation of single crystal microtubes. Evidence is provided to show that two-flux transport theory and diffusion theory both significantly underestimate the absorption due to dependent, multiple scattering and that the threshold for the thermal runaway process responsible for this behavior is very sensitive to porosity of the random medium.

Synthesis and Thermoelectric Properties of Compositional-Modulated Lead Telluride–Bismuth Telluride Nanowire Heterostructures

We demonstrate the rational solution-phase synthesis of compositional modulated telluride nanowire heterostructures containing lead telluride (PbTe) and bismuth telluride (Bi2Te3). By tuning the ratio between PbTe and Bi2Te3 through adjusting the amount of critical reactants and precursors during the synthesis, the influence of composition on the thermoelectric properties of the nanowire heterostructures has been investigated in hot pressed nanocomposite pellets. Measurements of the thermoelectric properties show strongly reduced thermal conductivity that leads to an enhanced thermoelectric figure of merit (ZT) of 1.2 at 620 K.

Edge effect on thermal transport in graphene nanoribbons: A phonon localization mechanism beyond edge roughness scattering

Equilibrium molecular dynamics simulations show that graphene nanoribbons (GNRs) with zigzag edges have higher thermal conductivity (κ) than armchair-edged ones, and the difference diminishes with increasing temperature or ribbon width. The dominant phonon wavelength for thermal transport can be much longer (by orders of magnitude) than the difference between the “roughness” of smooth zigzag and armchair edges. Therefore, the roughness scattering theory is not sufficient to explain the largely different κ of GNRs with different edge chiralities. Cross-sectional decomposition of the steady-state heat flux shows significant suppression of thermal transport at edges, especially in armchair ones. This behavior is explored by phonon spectra analysis. Considerable phonon localization at edges is concluded to underlie the edge-chirality dependent κ of GNRs.

Tunable thermal rectification in graphene nanoribbons through defect engineering: A molecular dynamics study

Using non-equilibrium molecular dynamics, we show that asymmetrically defected graphene nanoribbons (GNR) are promising thermal rectifiers. The optimum conditions for thermal rectification (TR) include low temperature, high temperature bias, ∼1% concentration of single-vacancy or substitutional silicon defects, and a moderate partition of the pristine and defected regions. TR ratio of ∼80% is found in a 14-nm long and 4-nm wide GNR at a temperature of 200 K and bias of 90 K, where heat conduction is in the ballistic regime since the bulk effective phonon mean-free-path is around 775 nm. As the GNR length increases towards the diffusive regime, the TR ratio decreases and eventually stabilizes at a length-independent value of about 3%–5%. This work extends defect engineering to 2D materials for achieving TR.

Electrical and thermal conductivities of reduced graphene oxide/polystyrene composites

The author reports an experimental study of electrical and thermal transport in reduced graphene oxide (RGO)/polystyrene (PS) composites. The electrical conductivity (σ) of RGO/PS composites with different RGO concentrations at room temperature shows a percolation behavior with the percolation threshold of ∼0.25 vol. %. Their temperature-dependent electrical conductivity follows Efros-Shklovskii variable range hopping conduction in the temperature range of 30–300 K. The thermal conductivity (κ) of composites is enhanced by ∼90% as the concentration is increased from 0 to 10 vol. %. The thermal conductivity of composites approximately linearly increases with increasing temperature from 150 to 300 K. Composites with a higher concentration show a stronger temperature dependence in the thermal conductivity.