Brillouin and Raman scattering spectroscopy are established techniques for the nondestructive contactless and label-free readout of mechanical, chemical and structural properties of condensed matter. Brillouin-Raman investigations currently require separate measurements and a site-matching approach to obtain complementary information from a sample.Here we demonstrate a new concept of fully scanning multimodal micro-spectroscopy for simultaneous detection of Brillouin and Raman light scattering in an exceptionally wide spectral range, from fractions of GHz to hundreds of THz. It yields an unprecedented 150 dB contrast, which is especially important for the analysis of opaque or turbid media such as biomedical samples, and a spatial resolution on sub-cellular scale. We report the first applications of this new multimodal method to a range of systems, from a single cell to the fast reaction kinetics of a curing process, and the mechano-chemical mapping of highly scattering biological samples.

Light scattering spectra on aqueous solutions of trehalose were recorded in a wide frequency range combining the use of a double monochromator and a multipass Fabry-Perot interferometer. Experimental results indicate the presence of a slow relaxation mode related to the solute dynamics, which is clearly separated from the solvent one. The spectral analysis reveals the existence of two separate solvent relaxation processes assigned to hydrating and bulk water molecules. The picosecond dynamics of water molecules directly interacting with the solute (proximal water) is consistently delayed with the corresponding relaxation time increase is about 5-6 times compared to the bulk. The slowing down induced by the sugar on the water dynamics mainly involves a restricted hydration layer constituted of 16-18 water molecules. These results improve our knowledge about the influence of carbohydrates on the fast rearrangement dynamics of water and may serve as a model to gain important insight on basic solvation properties of other biorelevant systems in aqueous media.

Brillouin scattering has been used to measure the dynamic structure factor of glycerol as a function of temperature from the high temperature liquid to the glassy state. Our investigation aims at understanding the number and the nature of the relaxation processes active in this prototype glass forming system in the high frequency region. The associated character of glycerol is reflected by a rather simple relaxations pattern, while the contributions coming from intra-molecular channels are negligible in the GHz frequency region. The temperature behavior of the characteristic frequency and lifetime of the longitudinal acoustic modes is analyzed, suggesting that a phenomenological model which only includes the structural (α) process and the unrelaxed viscosity is able to catch the leading contributions to the dynamics of the density fluctuations. This ansatz is also supported by a combined analysis of light and inelastic x-ray scattering spectra. The temperature dependence of the characteristic time of the α-process, τα, obtained by a full-spectrum analysis conforms to the α-scale universality, i.e. the values τα revealed by different experimental techniques are proportional the ones to the others. The non-erogodicity parameter smoothly decreases on increasing the temperature, and no signature of the cusp-like behavior predicted by the idealized mode coupling theory and observed in other glass-formers is found in glycerol.

We report a detailed analysis of the dynamic structure factor of glassy sorbitol by using inelastic X-ray scattering and previously measured light scattering data [B. Ruta, G. Monaco, F. Scarponi, and D. Fioretto, Philos. Mag. 88, 3939 (2008)]. The thus obtained knowledge on the density-density fluctuations at both the mesoscopic and macroscopic length scale has been used to address two debated topics concerning the vibrational properties of glasses. The relation between the acoustic modes and the universal boson peak (BP) appearing in the vibrational density of states of glasses has been investigated, also in relation with some recent theoretical models. Moreover, the connection between the elastic properties of glasses and the slowing down of the structural relaxation process in supercooled liquids has been scrutinized. For what concerns the first issue, it is here shown that the wave vector dependence of the acoustic excitations can be used, in sorbitol, to quantitatively reproduce the shape of the boson peak, supporting the relation between BP and acoustic modes. For what concerns the second issue, a proper study of elasticity over a wide spatial range is shown to be fundamental in order to investigate the relation between elastic properties and the slowing down of the dynamics in the corresponding supercooled liquid phase.

Depolarized Rayleigh scattering (DRS) spectra of glucose aqueous solutions measured from 0.01 to 1000 cm −1 reveal the presence of two distinct relaxation processes, in addition to the intermolecular Raman modes of the water network. The slow relaxation process with a characteristic time of tens of picoseconds is due to the glucose rotational diffusion and is spectrally separated from the fast relaxation process at picosecond time scales commonly attributed to the hydrogen-bond lifetime; this latter time clearly increases with increase in glucose concentration. This suggests the formation of stable sugar hydration shells where the water dynamics is slower than the bulk. The destructuring effect on the tetrahedral hydrogen bonding of water induced by the sugar is also clearly evidenced when comparing the intermolecular Raman spectra at different molar ratios.

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