A customizable digital holographic microscope.

We propose a compact, portable, and low-cost holographic microscope designed for the characterization of micrometric particles suspended in a liquid. This system is built around a commercial optical microscope by substituting its illumination source (a light-emitting diode) with a collimated laser beam. Similarly, a quartz flow cell replaces the microscope glass slide using a 3D-printed custom mount. With the hardware presented in this paper, the holographic imaging of the electromagnetic fields emitted by the particles that intercept the laser beam achieves a resolution close to that of optical microscopes but with a greater depth of field. Several morphological and optical features can be extracted from the holograms, including particle projected section, aspect ratio, and extinction cross-section. Additionally, we introduce a remote system control that enables users to process the acquired holograms on a remote computational device. This work provides a comprehensive description of the methodology of image processing in holographic microscopy and a series of validation measurements conducted using calibrated particles. This technique is suitable for the characterization of airborne particles found in snow, firn, and ice; here we report experimental results obtained from Alpine ice cores.

Refractive Index of Supercooled Water Down to 230.3 K in the Wavelength Range between 534 and 675 nm.

Knowledge of the refractive index of water in the deeply supercooled metastable liquid state is important, for example, for an accurate description of optical reflection and refraction processes occurring in clouds. However, a measurement of both the temperature and wavelength dependence of the refractive index under such extreme conditions is challenging. Here, we employ Raman spectroscopy in combination with microscopic water jets in vacuum to obtain the refractive index of supercooled water to a lowest temperature of 230.3 K. While our approach is based on the analysis of Mie resonances in Raman spectra measured by using a single excitation wavelength at 532 nm, it allows us to obtain the refractive index in a wide visible wavelength range from 534 to 675 nm. Because of a direct link between the refractive index and density of water, our results provide a promising approach to help improve our understanding of water's anomalous behavior.

Near field scattering for samples under forced flow.

We describe a light scattering technique for characterizing colloidal samples under constant flow. It exploits the properties of speckles in the deep Fresnel region-the so-called near field speckles-providing absolute scattering measurements of the static form factor of the sample, as described extensively by Mazzoni et al. [Rev. Sci. Instrum. 84, 043704 (2013)] for static samples. We exploit a strongly astigmatic beam for illuminating the scattering volume with a light sheet a few microns thick. This largely improves the sensitivity of the method to small signals. Moreover, by flowing the sample in the direction perpendicular to the light sheet, the transit times are reduced to a minimum, allowing for fast measurements. We tested the instrument with suspensions of calibrated colloidal polystyrene spheres with a size comparable to the light wavelength. In particular, we recovered the static form factors of suspensions of spherical particles and the phase lag of the zero-angle scattering amplitude, which both compare well to Mie theory predictions. We then applied the method to colloidal fractal aggregates of sub-wavelength particles and measured their fractal dimension. The instrument is designed to be operational in continuous flow analysis systems.

Erratum: Shrinking of Rapidly Evaporating Water Microdroplets Reveals their Extreme Supercooling [Phys. Rev. Lett. 120, 015501 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.120.015501.

Shrinking of Rapidly Evaporating Water Microdroplets Reveals their Extreme Supercooling.

The fast evaporative cooling of micrometer-sized water droplets in a vacuum offers the appealing possibility to investigate supercooled water-below the melting point but still a liquid-at temperatures far beyond the state of the art. However, it is challenging to obtain a reliable value of the droplet temperature under such extreme experimental conditions. Here, the observation of morphology-dependent resonances in the Raman scattering from a train of perfectly uniform water droplets allows us to measure the variation in droplet size resulting from evaporative mass losses with an absolute precision of better than 0.2%. This finding proves crucial to an unambiguous determination of the droplet temperature. In particular, we find that a fraction of water droplets with an initial diameter of 6379±12 nm remain liquid down to 230.6±0.6 K. Our results question temperature estimates reported recently for larger supercooled water droplets and provide valuable information on the hydrogen-bond network in liquid water in the hard-to-access deeply supercooled regime.

Hyperspectral imaging with deformable gratings fabricated with metal-elastomer nanocomposites.

We report the fabrication and characterization of a simple and compact hyperspectral imaging setup based on a stretchable diffraction grating made with a metal-polymer nanocomposite. The nanocomposite is produced by implanting Ag clusters in a poly(dimethylsiloxane) film by supersonic cluster beam implantation. The deformable grating has curved grooves and is imposed on a concave cylindrical surface, thus obtaining optical power in two orthogonal directions. Both diffractive and optical powers are obtained by reflection, thus realizing a diffractive-catoptric optical device. This makes it easier to minimize aberrations. We prove that, despite the extended spectral range and the simplified optical scheme, it is actually possible to work with a traditional CCD sensor and achieve a good spectral and spatial resolution.

Single particle extinction and scattering optical method unveils in real time the influence of the blood components on polymeric nanoparticles.

Here we report the quantitative in situ characterization of size distribution evolution of polymeric nanoparticles incubated in murine serum, filtered and unfiltered murine blood. We used an analytical optical approach, named Single Particle Extinction and Scattering (SPES), which relies on the measurements of two independent parameters of single particles. SPES is based on a robust self-reference interference optical scheme which allows a rejection of the spurious signals coming from the background caused by the medium. We employed polystyrene nanoparticles as reference system and polydisperse poly(lactic-co-glycolic acid) nanoparticles. Our results demonstrate that SPES can be used for carrying out ex vivo analysis of nanoparticles to evaluate the modifications that NPs undergo in vivo following different routes of entry. Conversely, Dynamic Light Scattering is not able to provide reliable results for these systems due to the presence of the biological components in solution.

Do protein crystals nucleate within dense liquid clusters?

Protein-dense liquid clusters are regions of high protein concentration that have been observed in solutions of several proteins. The typical cluster size varies from several tens to several hundreds of nanometres and their volume fraction remains below 10(-3) of the solution. According to the two-step mechanism of nucleation, the protein-rich clusters serve as locations for and precursors to the nucleation of protein crystals. While the two-step mechanism explained several unusual features of protein crystal nucleation kinetics, a direct observation of its validity for protein crystals has been lacking. Here, two independent observations of crystal nucleation with the proteins lysozyme and glucose isomerase are discussed. Firstly, the evolutions of the protein-rich clusters and nucleating crystals were characterized simultaneously by dynamic light scattering (DLS) and confocal depolarized dynamic light scattering (cDDLS), respectively. It is demonstrated that protein crystals appear following a significant delay after cluster formation. The cDDLS correlation functions follow a Gaussian decay, indicative of nondiffusive motion. A possible explanation is that the crystals are contained inside large clusters and are driven by the elasticity of the cluster surface. Secondly, depolarized oblique illumination dark-field microscopy reveals the evolution from liquid clusters without crystals to newly nucleated crystals contained in the clusters to grown crystals freely diffusing in the solution. Collectively, the observations indicate that the protein-rich clusters in lysozyme and glucose isomerase solutions are locations for crystal nucleation.

Mapping the transverse coherence of the self amplified spontaneous emission of a free-electron laser with the heterodyne speckle method.

The two-dimensional single shot transverse coherence of the Self-Amplified Spontaneous Emission of the SPARC_LAB Free-Electron Laser was measured through the statistical analysis of a speckle field produced by heterodyning the radiation beam with a huge number of reference waves, scattered by a suspension of particles. In this paper we report the measurements and the evaluation of the transverse coherence along the SPARC_LAB undulator modules. The measure method was demonstrated to be precise and robust, it does not require any a priori assumptions and can be implemented over a wide range of wavelengths, from the optical radiation to the x-rays.

Colloidal aggregation in microgravity by critical Casimir forces.

By using the critical Casimir force, we study the attractive strength dependent aggregation of colloids with and without gravity by means of near field scattering. Significant differences were seen between microgravity and ground experiments, both in the structure of the formed fractal aggregates as well as in the kinetics of growth. In microgravity purely diffusive aggregation is observed. By using the continuously variable particle interaction potential we can for the first time experimentally relate the strength of attraction between the particles and the structure of the aggregates.