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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 utilize pump-probe microscopy to distinguish four 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 also demonstrates that even nominally homogeneous pigments present remarkable, and useful, heterogeneity in pump-probe microscopy.

In optical experiments, shutters are devices that open or close a path of light. They are often used to limit the duration of light exposure onto a target or onto a detector in order to reduce possible light-induced damage. Many commercial shutters are available for different applications - some provide very fast opening and closing times, some can handle large optical powers, and others allow for fail-safe operation. Many of these devices are costly and offer limited control options. Here we provide an open-source design for a low-cost, general purpose shutter system based on ubiquitous servo motors that are connected to an Arduino-based controller. Several shutters can be controlled by one controller, further reducing system cost. The state of the shutters can be controlled via a display built into the controller, by serial commands via USB, or by electrical control lines. The use of a microcontroller makes the shutter controller adaptable - only control options that are used need to be included, and the design accommodates a selection of display and servo options. We provide designs for all required components, including 3D print files for the servo holders and cases, software for the Arduino, libraries for serial communication (C and python), and example graphical user interfaces for testing.

Cadmium sulfide (CdS) pigments have degraded in several well-known paintings, but the mechanisms of degradation 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 artificially aged by exposure to high relative humidity (RH) and ultraviolet (UV) light. 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. The observed degradation by pump-probe microscopy occurred through the conversion from CdS into CdSO4.xH2O, verified by both FTIR (Fourier-transform infrared) and XPS (X-ray photoelectron spectroscopy) experiment.

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 is 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 exemplary 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., Comment: 12 pages, 4 figures

Pump-probe microscopy is an emerging nonlinear imaging technique based on high repetition rate lasers and fast intensity modulation. Here we present new methods for pump-probe microscopy that keep the beam intensity constant and instead modulate the inter-pulse time delay, the relative polarization, or the pulse length. These techniques can improve image quality for samples that have poor heat dissipation or long-lived radiative states, and can selectively address nonlinear interactions in the sample. We experimentally demonstrate this approach and point out the advantages over conventional intensity modulation.

We present a new imaging method for pump-probe microscopy that explores non-collinear excitation. This method (crossed-beam pump-probe microscopy, or CBPM) can significantly improve the axial resolution when imaging through low-NA lenses, providing an alternative way for depth resolved, large field-of-view imaging. We performed a proof-of-concept demonstration, characterized CBPM's resolution using different imaging lenses, and measured an enhanced axial resolution for certain types of low-NA lenses., Comment: 9 pages, 6 figures

We study ultra-broadband slow light in a warm Rubidium vapor cell. By working between the D1 and D2 transitions, we find a several-nm window centered at 788.4 nm in which the group index is highly uniform and the absorption is small (<1%). We demonstrate that we can control the group delay by varying the temperature of the cell, and observe a tunable fractional delay of 18 for pulses as short as 250 fs (6.9 nm bandwidth) with a fractional broadening of only 0.65 and a power leakage of 55%. We find that a simple theoretical model is in excellent agreement with the experimental results. Using this model, we discuss the impact of the pulse's spectral characteristics on the distortion it incurs during propagation through the vapor., Comment: The first two authors contributed equally to this work