Multiplexed lock-in thermography.

Many modern measurement methods for heat transfer work in the frequency domain. A certain average temperature rise in the sample is unavoidable if the sample can only be heated, e.g., by an intensity modulated light source. This average temperature rise influences the measured thermal properties because they are, in general, temperature dependent. Here, we explore square waves and multiplexed sine waves with the goal of reducing the average temperature rise. We apply these signals to lock-in thermography and show the feasibility of a simultaneous measurement at multiple frequencies. In addition, we propose the use of the Goertzel algorithm to efficiently extract individual spectral components from the temperature signal.

Tunable Thermoelastic Anisotropy in Hybrid Bragg Stacks with Extreme Polymer Confinement.

Controlling thermomechanical anisotropy is important for emerging heat management applications such as thermal interface and electronic packaging materials. Whereas many studies report on thermal transport in anisotropic nanocomposite materials, a fundamental understanding of the interplay between mechanical and thermal properties is missing, due to the lack of measurements of direction-dependent mechanical properties. In this work, exceptionally coherent and transparent hybrid Bragg stacks made of strictly alternating mica-type nanosheets (synthetic hectorite) and polymer layers (polyvinylpyrrolidone) were fabricated at large scale. Distinct from ordinary nanocomposites, these stacks display long-range periodicity, which is tunable down to angstrom precision. A large thermal transport anisotropy (up to 38) is consequently observed, with the high in-plane thermal conductivity (up to 5.7 W m-1 K-1 ) exhibiting an effective medium behavior. The unique hybrid material combined with advanced characterization techniques allows correlating the full elastic tensors to the direction-dependent thermal conductivities. We, therefore, provide a first analysis on how the direction-dependent Young's and shear moduli influence the flow of heat.

Direct Measurement of the In-Plane Thermal Diffusivity of Semitransparent Thin Films by Lock-In Thermography: An Extension of the Slopes Method.

We present an extension of the well-known slopes method for characterization of the in-plane thermal diffusivity of semitransparent polymer films. We introduce a theoretical model which considers heat losses due to convection and radiation mechanisms, as well as semitransparency of the material to the exciting laser heat source (visible range) and multiple reflections at the film surfaces. Most importantly, a potential semitransparency of the material in the IR detection range is also considered. We prove by numerical simulations and by an asymptotic expansion of the surface temperature that the slopes method is also valid for any semitransparent film in the thermally thin regime. Measurements of the in-plane thermal diffusivity performed on semitransparent polymer films covering a wide range of absorption coefficients (to the exciting wavelength and in the IR detection range of our IR camera) validate our theoretical findings.

Ordered Particle Arrays via a Langmuir Transfer Process: Access to Any Two-Dimensional Bravais Lattice.

We demonstrate how to directly transform a close-packed hexagonal colloidal monolayer into nonclose-packed particle arrays of any two-dimensional symmetry at the air/water interface. This major advancement in the field of nanoparticle self-assembly is based on a simple one-dimensional stretching step in combination with the particle array orientation. Our method goes far beyond existing strategies and allows access to all possible two-dimensional Bravais lattices. A key element of our work is the possibility to macroscopically stretch a particle array in a truly one-dimensional manner, which has not been possible up to now. We achieve this by stretching the nanoparticle array at an air/water interface during the transfer process. The degree of stretching is simply controlled by the wettability of the transfer substrate. To retain the symmetry of the transferred structure, the capillary forces upon drying have to be circumvented. We demonstrate two concepts based on thermal fixation for this. It allows for the first time to fabricate nonclose-packed, nonhexagonal colloidal monolayers on a macroscopic length scale.

Computing the 3D Radial Distribution Function from Particle Positions: An Advanced Analytic Approach.

The radial distribution function, g( r), is ubiquitously used to analyze the internal structure of particulate systems. However, experimentally derived particle coordinates are always confined to a finite sample volume. This poses a particular challenge on computing g( r): Once the radial distance, r, extends beyond the sample boundaries in at least one dimension, substantial deviations from the true g( r) function can occur. State of the art algorithms for g( r) mitigate this issue for instance by using artificial periodic boundary conditions. However, ignoring the finite nature of the sample volume distorts g( r) significantly. Here, we present a simple, analytic algorithm for the computation of g( r) in finite samples. No additional assumptions about the sample are required. The key idea is to use an analytic solution for the intersection volume between a spherical shell and the sample volume. In addition, we discovered a natural upper bound for the radial distance that only depends on sample size and shape. This analytic approach will prove to be invaluable for the quantitative analysis of the increasing amount of experimentally derived tomography data.

Thermal transport in binary colloidal glasses: Composition dependence and percolation assessment.

The combination of various types of materials is often used to create superior composites that outperform the pure phase components. For any rational design, the thermal conductivity of the composite as a function of the volume fraction of the filler component needs to be known. When approaching the nanoscale, the homogeneous mixture of various components poses an additional challenge. Here, we investigate binary nanocomposite materials based on polymer latex beads and hollow silica nanoparticles. These form randomly mixed colloidal glasses on a sub-µm scale. We focus on the heat transport properties through such binary assembly structures. The thermal conductivity can be well described by the effective medium theory. However, film formation of the soft polymer component leads to phase segregation and a mismatch between existing mixing models. We confirm our experimental data by finite element modeling. This additionally allowed us to assess the onset of thermal transport percolation in such random particulate structures. Our study contributes to a better understanding of thermal transport through heterostructured particulate assemblies.

Low Thermal Conductivity through Dense Particle Packings with Optimum Disorder.

Heat transport plays a critical role in modern batteries, electrodes, and capacitors. This is caused by the ongoing miniaturization of such nanotechnological devices, which increases the local power density and hence temperature. Even worse, the introduction of heterostructures and interfaces is often accompanied by a reduction in thermal conductivity, which can ultimately lead to the failure of the entire device. Surprisingly, a fundamental understanding of the governing heat transport processes even in simple systems, such as binary particle mixtures is still missing. This contribution closes this gap and elucidates how strongly the polydispersity of a model particulate system influences the effective thermal conductivity across such a heterogeneous system. In a combined experimental and modeling approach, well-defined mixtures of monodisperse particles with varying size ratios are investigated. The transition from order to disorder can reduce the effective thermal conductivity by as much as ≈50%. This is caused by an increase in the thermal transport path length and is governed by the number of interparticle contact points. These results are of general importance for many particulate and heterostructured materials and will help to conceive improved device layouts with more reliable heat dissipation or conservation properties in the future.

Circular Dichroism of Chiral Nematic Films of Cellulose Nanocrystals Loaded with Plasmonic Nanoparticles.

In the search for induced chiral plasmonic activity, cholesteric films formed by cellulose nanocrystals have attracted great interest as potential hosts for plasmonic nanoparticles. Circular dichroism (CD) spectra of the composite films exhibit two peaks, one of which is ascribed to the cholesteric host and the other one to plasmonic chiroptical activity of the plasmonic nanoparticles. Here we report the results of comprehensive studies of extinction and CD properties of composite films formed by different types of cellulose nanocrystals and different types of plasmonic nanoparticles. We show that the second peak in the CD spectra acquired using CD spectrometers appears as the result of the local reduction of the CD signal of the host material, due to excessive absorption by the nanoparticles, and thus it cannot be interpreted as induced plasmonic chiroptical activity. Instead, we propose an alternative way to measure CD spectra of plasmonic cholesteric films by using Mueller matrix transmission ellipsometry. The results of this study are important for ongoing research in the field of chiral plasmonics and for the optical characterization of a broad range of chiral nematic nanostructured materials.