No Arabic abstract
We review the Raman shift method as a non-destructive optical tool to investigate the thermal conductivity and demonstrate the possibility to map this quantity with a micrometer resolution by studying thin film and bulk materials for thermoelectric applications. In this method, a focused laser beam both thermally excites a sample and undergoes Raman scattering at the excitation spot. The temperature dependence of the phonon energies measured is used as a local thermometer. We discuss that the temperature measured is an effective one and describe how the thermal conductivity is deduced from single temperature measurements to full temperature maps, with the help of analytical or numerical treatments of heat diffusion. We validate the method and its analysis on 3- and 2-dimensional single crystalline samples before applying it to more complex Si-based materials. A suspended thin mesoporous film of phosphorus-doped laser-sintered Si78Ge22 nanoparticles is investigated to extract the in-plane thermal conductivity from the effective temperatures, measured as a function of the distance to the heat sink. Using an iterative multigrid Gauss-Seidel algorithm the experimental data can be modelled yielding a thermal conductivity of 0.1 W/m K after normalizing by the porosity. As a second application we map the surface of a phosphorus-doped 3-dimensional bulk-nanocrystalline Si sample which exhibits anisotropic and oxygen-rich precipitates. Thermal conductivities as low as 11 W/m K are found in the regions of the precipitates, significantly lower than the 17 W/m K in the surrounding matrix. The present work serves as a basis to more routinely use the Raman shift method as a versatile tool for thermal conductivity investigations, both for samples with high and low thermal conductivity and in a variety of geometries.
We use a spatially resolved, direct spectroscopic probe for electronic structure with an additional sensitivity to chemical compositions to investigate high-quality single crystal samples of La_{1/4}Pr_{3/8}Ca_{3/8}MnO_{3}, establishing the formation of distinct insulating domains embedded in the metallic host at low temperatures. These domains are found to be at least an order of magnitude larger in size compared to previous estimates and exhibit memory effects on temperature cycling in the absence of any perceptible chemical inhomogeneity, suggesting long-range strains as the probable origin.
We present a novel high resolution contactless technique for thermal conductivity determination and thermal field mapping based on creating a thermal distribution of phonons using a heating laser, while a second laser probes the local temperature through the spectral position of a Raman active mode. The spatial resolution can be as small as $300$ nm, whereas its temperature accuracy is $pm 2$ K. We validate this technique investigating the thermal properties of three free-standing single crystalline Si membranes with thickness of 250, 1000, and 2000 nm. We show that for 2-dimensional materials such as free-standing membranes or thin films, and for small temperature gradients, the thermal field decays as $T(r) propto ln(r)$ in the diffusive limit. The case of large temperature gradients within the membranes leads to an exponential decay of the thermal field, $T propto exp[-A cdot ln(r)]$. The results demonstrate the full potential of this new contactless method for quantitative determination of thermal properties. The range of materials to which this method is applicable reaches far beyond the here demonstrated case of Si, as the only requirement is the presence of a Raman active mode.
The excitonic recombinations in hexagonal boron nitride (hBN) are investigated with spatially resolved cathodoluminescence spectroscopy in the UV range. Cathodoluminescence images of an individual hBN crystallite reveals that the 215 nm free excitonic line is quite homogeneously emitted along the crystallite whereas the 220 nm and 227 nm excitonic emissions are located in specific regions of the crystallite. Transmission electron microscopy images show that these regions contain a high density of crystalline defects. This suggests that both the 220 nm and 227 nm emissions are produced by the recombination of excitons bound to structural defects.
Low dimensional systems, nanowires, in particular, have exhibited excellent optical and electronic properties. Understanding the thermal properties in semiconductor nanowires is very important for their applications in their electronic devices. In the present study, the thermal conductivity of a freestanding silicon nanowire (NW) is estimated employing the Raman spectroscopy. The advantage of this technique is that the light source (laser) can be used both as heating and excitation source. The variations of the first-order Raman peak position of the freestanding silicon NW with respect to temperature and laser power are carried out. A critical analysis of effective laser power absorbed by exposed silicon NW, the detailed Raman study along with the concept of longitudinal heat distribution in silicon NW, the thermal conductivity of the freestanding silicon NW of 112 nm diameter is estimated to be ~53 W/m.K.
We investigate temperature dependent thermal conductivity k(T) in a single Ge nanowire (NW) using Optothermal Raman Spectroscopy which utilizes the temperature dependence of Raman lines as a local probe for temperature. The experiment was done from 300 K to above 700 K, a temperature range in which thermal conductivity of single NWs has been explored rarely. The thermal conductivity of Ge NWs (grown by vapor liquid solid mechanism), at around room temperature were observed to lie in the range 1.8 to 4.2 W/m.K for diameters between 50 to 110 nm. The thermal conductivity at a given temperature was found to follow a linear dependence on NW diameter, suggesting that the low magnitude of k(T) is determined by diffused scattering of phonons from the surface of NWs that reduces it severely from its bulk value. k(T) shows approximately 1/T behavior which arises from the Umklapp processes. The quantitative estimation of errors arising from the Optothermal measurement and methods to mitigate them has been discussed. We also suggest a quick way to estimate approximately the thermal conductivity of Ge and Si NWs using the above observations.