Search for: All records

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 the 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. 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. 

Micro-Raman spectroscopy has become an important tool in probing thermophysical properties in functional materials. Localized heating by the focused Raman excitation laser beam can produce both stress and local nonequilibrium phonons in the material. Here, we investigate the effects of hot optical phonons in the Raman spectra of molybdenum disulfide and distinguish them from those caused by thermally induced compressive stress, which causes a Raman frequency blue shift. We use a thermomechanical analysis to correct for this stress effect in the equivalent lattice temperature extracted from the measured Raman peak shift. When the heating Gaussian laser beam is reduced to 0.71  μm, the corrected peak shift temperature rise is 17% and 8%, respectively, higher than those determined from the measured peak shift and linewidth without the stress correction, and 32% smaller than the optical phonon temperature rise obtained from the anti-Stokes to Stokes intensity ratio. This nonequilibrium between the hot optical phonons and the lattice vanishes as the beam width increases to 1.53 μm. Much less pronounced than those reported in prior micro-Raman measurements of suspended graphene, this observed hot phonon behavior agrees with a first-principles based multitemperature model of overpopulated zone-center optical phonons compared to other optical phonons in the Brillouin zone and acoustic phonons of this prototypical transition metal dichalcogenide. The findings provide detailed insight into the energy relaxation processes in this emerging electronic and optoelectronic material and clarify an important question in micro-Raman measurements of thermal transport in this and other two-dimensional materials. 

Boron arsenide (BAs) is a covalent semiconductor with a theoretical intrinsic thermal conductivity approaching 1300 W/m K. The existence of defects not only limits the thermal conductivity of BAs significantly but also changes its pressure-dependent thermal transport behavior. Using both picosecond transient thermoreflectance and femtosecond time-domain thermoreflectance techniques, we observed a non-monotonic dependence of thermal conductivity on pressure. This trend is not caused by the pressure-modulated phonon–phonon scattering, which was predicted to only change the thermal conductivity by 10%–20%, but a result of several competing effects, including defect–phonon scattering and modification of structural defects under high pressure. Our findings reveal the complexity of the defect-modulated thermal behavior under pressure.

 

Atmospheric nitrogen fixation using a photocatalytic system is a promising approach to produce ammonia. However, most of the recently explored photocatalysts for N 2 fixation are in the powder form, suffering from agglomeration and difficulty in the collection and leading to unsatisfactory conversion efficiency. Developing efficient film catalysts for N 2 photofixation under ambient conditions remains challenging. Herein, we report the efficient photofixation of N 2 over a periodic WS 2 @TiO 2 nanoporous film, which is fabricated through a facile method that combines anodization, E-beam evaporation, and chemical vapor deposition (CVD). Oxygen vacancies are introduced into TiO 2 nanoporous films through Ar annealing treatment, which plays a vital role in N 2 adsorption and activation. The periodic WS 2 @TiO 2 nanoporous film with an optimized WS 2 content shows highly efficient photocatalytic performance for N 2 fixation with an NH 3 evolution rate of 1.39 mmol g −1 h −1 , representing one of the state-of-the-art catalysts.