Determining and imaging the thermal properties at the nanoscale is a demanding experimental challenge. So far, virtually any techniques used to image nanoscale thermal properties require to position the sample in contact with voluminous probes that act as undesirable thermal sinks and dramatically affect the measurements, in spite of poor interfacial thermal resistivity. Thermoreflectance, a contactless technique in which thermal conductivity is measured by optically probing the heat-induced changes in a sample, is extensively used for measuring the macroscopic and microscopic thermal properties of solids, but, so far, has been limited by diffraction in its applicability at the nanoscale. Here, we present near-field scanning thermoreflectance imaging (NeSTRI), a new scanning probe technique in which an aperture-type near-field optical microscope at sub-wavelength resolution is used to contactlessly determine the thermoreflectance of thin films. As a case study, NeSTRI is here applied to multilayer graphene thin films on glass substrates. Thermal conductivity of micrometre-size multilayer graphene platelets is determined and is consistent with previous macroscopic predictions. We also find that the thermal conductivity is locally higher at specific crystallographic edges of multilayer graphene platelets, which is indicative of the spatial resolution of our method. NeSTRI is uniquely suited to understanding the thermal properties of a large class of nanostructured and nanoscale systems.
Photothermal deflection (PTD) has been frequently utilized to measure the thermal properties of thin solid films on a substrate. In the models commonly used to interpret PTD data, the substrate is assumed to be an ideal thermal insulator. This assumption poses important restrictions on the reliability of these thermal measurements and limits the possibility to use PTD for also measuring the specific heat of the samples. Simultaneous knowledge of specific heat and thermal diffusivity is necessary to determine the thermal conductivity of thin solid films. In this work, we calculated the phase and amplitude of the PTD signal at the two opposites sides (film-side and substrate-side) of a thin-film substrate system. We find that, on both sides, the phases of the PTD signal primarily depend on the thermal diffusivity of the thin film, while the amplitudes primarily depend on the specific heat. By using the phases and amplitudes at the two sides, we show that the accuracy of thermal conductivity measurements by PTD can be dramatically improved. We validate our theoretical model by measuring, in a scanning PTD apparatus, the thermal properties of gold thin films, which are in excellent agreement with, and improve on, existing data from the literature.
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