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For multi-layered 2D materials, although its c-axis has a much lower thermal conductivity than the a-axis, its phonon mean free path has been confirmed to be very long, e.g., in the order of 100s nm at room temperature for multi-layered graphene. An anisotropic specific heat concept has been proposed in the past to explain this very long mean free path. This work carries out detailed atomistic modeling to quantify the anisotropic specific heat concept and reports the discovery of anisotropic temperatures in multi-layered 2D materials under ultrafast surface heating. Extremely fast c-phonon energy transport is discovered, and the non-Fourier effect is observed for both a-phonons and c-phonons. The energy coupling factor between these two modes of phonons is determined to be in the order of 1016 W K−1 m−3, with the specific number depending on the structure location. The anisotropic temperature concept is also quantitatively confirmed based on the lattice Boltzmann method simulation. The anisotropic temperature concept does not violate the physics that temperature is a scalar; rather, it is developed to distinguish the temperatures of phonons that travel in different directions. This concept is universally applicable to other 2D materials to describe the heat conduction in the in-plane and out-of-plane directions that feature different interatomic bonds. 

The temperature coefficient of resistivity (θT) of carbon-based materials is a critical property that directly determines their electrical response upon thermal impulses. It could have metal- (positive) or semiconductor-like (negative) behavior, depending on the combined temperature dependence of electron density and electron scattering. Its distribution in space is very difficult to measure and is rarely studied. Here, for the first time, we report that carbon-based micro/nanoscale structures have a strong non-uniform spatial distribution of θT. This distribution is probed by measuring the transient electro-thermal response of the material under extremely localized step laser heating and scanning, which magnifies the local θT effect in the measured transient voltage evolution. For carbon microfibers (CMFs), after electrical current annealing, θT varies from negative to positive from the sample end to the center with a magnitude change of >130% over <1 mm. This θT sign change is confirmed by directly testing smaller segments from different regions of an annealed CMF. For micro-thick carbon nanotube bundles, θT is found to have a relative change of >125% within a length of ∼2 mm, uncovering strong metallic to semiconductive behavior change in space. Our θT scanning technique can be readily extended to nm-thick samples with μm scanning resolution to explore the distribution of θT and provide a deep insight into the local electron conduction. 

The thermophysical properties of 1D micro/nanoscale materials could differ significantly from those of their bulk counterparts due to intensive energy carrier scattering by structures. This work provides an in-depth review of cutting-edge techniques employed for transient characterization of thermophysical properties at the micro/nanoscale scale. In terms of transient excitation, step Joule heating, step laser heating, pulsed laser heating, and frequency domain amplitude-modulated laser heating are covered. For thermal probing, electrical and Raman scattering-based physical principles are used. These techniques enable the measurement of thermal conductivity, thermal diffusivity, and specific heat from the sub-mm level down to the atomic level (single-atom thickness). This review emphasizes the advantages of these techniques over steady state techniques and their physics, challenges, and potential applications, highlighting their significance in unraveling the intricate thermal transport phenomena to the atomic level of 1D materials. 

Abstract Partial laser treatment is introduced to carbon‐based microfibers to generate excellent photon sensing capability without bias. This treatment brings about a Seebeck coefficient distribution along the sample's length, out of which a photovoltage with no external bias is generated and sensed. Using a line‐shaped laser spot, carbon microfiber (CMF), graphene microfiber (GMF), and graphene aerogel fiber (GAF) are investigated for their response to µm‐scale photon irradiation. A higher sensitivity for the incident photon is found for the GAF with no position sensitivity. More Seebeck coefficient variation is also observed for the GAF considering the amount of laser power used for the laser treatment. A weaker Seebeck coefficient spatial variation is observed for the GMF compared with the GAF. However, its photovoltage shows an abrupt magnitude change from the laser‐treated region to the non‐treated one. Despite the low spatial variation of the Seebeck coefficient for the CMF, it features an excellent and accurate position‐sensitive photoresponse with polarization change over a distance of ≈100 µm. Such unique capability prompts novel applications in using partially annealed CMF for sensing the position of optical beams at the microscale. 

Abstract This work reports the dynamic behaviors of graphene aerogel (GA) microfibers during and after continuous wave (CW) laser photoreduction. The reduction results in one‐order of magnitude increase in the electrical conductivity. The experimental results reveal the exact mechanisms of photoreduction as it occurs: immediate photochemical removal of oxygen functional groups causing a sharp decrease in electrical resistance and subsequent laser heating that facilitates thermal rearrangement of GO sheets towards more graphene‐like domains. X‐ray and Raman spectroscopy analysis confirm that photoreduction removes virtually all oxygen and nitrogen containing functional groups. Interestingly, a dynamic period immediately following the end of laser exposure shows a slow, gradual increase in electrical resistance, suggesting that a proportion of the electrical conductivity enhancement from photoreduction is not permanent. A two‐part experiment monitoring the resistance changes in real‐time before and after photoreduction is conducted to investigate this critical period. The thermal diffusivity evolution of the microfiber is tracked and shows an improvement of 277 % after all photoreduction experiments. A strong linear coherency between thermal diffusivity and electrical conductivity is also uncovered. This is the first known work to explore both the dynamic electrical and thermal evolution of a GO‐based aerogel during and after photoreduction.