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Zhongming Li, Kyle Aleshire, Masaru Kuno , and Gregory V. Hartland, “Super-Resolution Far-Field Infrared Imaging by Photothermal Heterodyne Imaging,” J. Phys. Chem. B, 2017, 121, 8838–8846

Abstract: Infrared (IR) imaging provides chemical-specific information without the need for exogenous labels. Conventional far-field IR imaging techniques are diffraction limited, which means an effective spatial resolution of >5 μm with currently available optics. In this article, we present a novel far-field IR imaging technique based on photothermal heterodyne imaging (IR-PHI). In our version of IR-PHI, an IR pump laser excites the sample, causing a small temperature rise that is detected by a counterpropagating visible probe beam. Images and spectra of several different types of soft matter systems (polystyrene beads, thin polymer films, and single Escherichia coli bacterial cells) are presented to demonstrate the sensitivity and versatility of the technique. Importantly, the spatial resolution in the IR-PHI measurements is determined by the visible probe beam: a spatial resolution of 0.3 μm was achieved with a 0.53 μm probe wavelength and a high numerical aperture focusing objective. This is the highest spatial resolution reported to date for far-field IR imaging. Analysis of the experiments shows that for polymer beads in a dry environment, the magnitude of the IR-PHI signal is determined by the scattering cross section of the nano-object at the probe wavelength. This is in contrast to conventional PHI experiments in a heat-transfer medium, where the signal scales as the absorption cross section. This different scaling can be understood through the optical theorem. Our analysis also shows that both thermal expansion and changes in the refractive index of the material are important and that these two effects, in general, counteract each other.

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