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Carbon-based black pigments, a widely used class of pigments, are difficult to differentiate with the noninvasive techniques currently used in cultural heritage science. We use pump-probe microscopy, coupled with a support vector machine, to distinguish common carbon-based black pigments as pure pigments, as two-component black pigment mixtures, and as a mixture of a black and a colorful pigment. This work showcases the potential of pump-probe microscopy to spatially differentiate carbon-based black pigments, which would have interesting applications to works of art. 

Abstract Cadmium sulfide (CdS) pigments have degraded in several well-known artworks, but the influence of pigment properties and environmental conditions on the degradation process have yet to be fully understood. Traditional non-destructive analysis techniques primarily focus on macroscopic degradation, whereas microscopic information is typically obtained with invasive techniques that require sample removal. Here, we demonstrate the use of pump-probe microscopy to nondestructively visualize the three-dimensional structure and degradation progress of CdS pigments in oil paints. CdS pigments, reproduced following historical synthesis methods, were reproduced as oil paints and artificially aged by exposure to high relative humidity and light. The degradation of CdS to CdSO₄·xH₂O was confirmed by both FTIR (Fourier-transform infrared) and XPS (x-ray photoelectron spectroscopy) experiments. During the degradation process, optical pump-probe microscopy was applied to track the degradation progress in single grains, and volumetric imaging revealed early CdS degradation of small particles and on the surface of large particles. This indicates that the particle dimension influences the extent and evolution of degradation of historical CdS. In addition, the pump-probe signal decrease in degraded CdS is observable before visible changes to the eye, demonstrating that pump-probe microscopy is a promising tool to detect early-stage degradation in artworks. 

Pump-probe microscopy of melanin in tumors has been proposed to improve diagnosis of malignant melanoma, based on the hypothesis that aggressive cancers disaggregate melanin structure. However, measured signals of melanin are complex superpositions of multiple nonlinear processes, which makes interpretation challenging. Polarization control during measurement and data fitting are used to decompose signals of melanin into their underlying molecular mechanisms. We then identify the molecular mechanisms that are most susceptible to melanin disaggregation and derive false-coloring schemes to highlight these processes in biological tissue. We demonstrate that false-colored images of a small set of melanoma tumors correlate with clinical concern. More generally, our systematic approach of decomposing pump-probe signals can be applied to a multitude of different samples.