arXiv subjects

Daniele Fioretto

Publications and source records attributed to Daniele Fioretto.

12 recordsLinked to original sources

arXiv2024

Consensus Statement on Brillouin Light Scattering Microscopy of Biological Materials

Brillouin Light Scattering (BLS) spectroscopy is a non-invasive, non-contact, label-free optical technique that can provide information on the mechanical properties of a material on the sub-micron scale. Over the last decade it has seen increased applications in the life sciences, driven by the observed significance of mechanical properties in biological processes, the realization of more sensitive BLS spectrometers and its extension to an imaging modality. As with other spectroscopic techniques, BLS measurements not only detect signals characteristic of the investigated sample, but also of the experimental apparatus, and can be significantly affected by measurement conditions. The aim of this consensus statement is to improve the comparability of BLS studies by providing reporting recommendations for the measured parameters and detailing common artifacts. Given that most BLS studies of biological matter are still at proof-of-concept stages and use different--often self-built--spectrometers, a consensus statement is particularly timely to assure unified advancement.

physics.optics↗

arXiv2021

Brillouin imaging in turbid samples: the removal of multiple scattering contribution

We provide a new analytic expression and an innovative experimental method to isolate the effect of multiple scattering (MS) in Brillouin investigation of highly turbid media. On the one hand, an analytic model is given to describe the spectrum in case of ill-defined exchanged wave-vector. On the other hand, a new experimental method, named Polarization Gated Brillouin Spectroscopy (PG-BS), is proposed for selecting the MS contribution through light polarization. Both experimental and analytic methods are tested against a benchmark material, milk, demonstrating their capability to extract reliable micro-mechanical parameters even in highly turbid materials till now inaccessible to in-depth Brillouin scattering investigation.

physics.optics↗

arXiv2020

Monitoring the refractive index of tissue models using light scattering spectroscopy

In this work, we report the application of Raman microspectroscopy for analysis of the refractive index of a range of tissue phantoms. Using both a custom-developed setup with visible laser source and a commercial micro-spectrometer with near infrared laser, we measured the Raman spectra of gelatin hydrogels at various concentrations. By building a calibration curve from measured refractometry data and Raman scattering intensity for different vibrational modes of the hydrogel, we determined the refractive indices of the gels from their Raman spectra, with approximately the same accuracy as that of refractometry measurements with an Abbe refractometer. This work highlights the importance of a correlative approach through Brillouin-Raman microspectroscopy for the mechano-chemical analysis of biologically relevant samples.

physics.bio-ph↗

arXiv2020

On the actual spatial resolution of Brillouin Imaging

Brillouin imaging is an emerging optical elastography technique able to generate maps of the mechanical properties at microscale, with great potential in biophysical and biomedical fields. A key parameter is its spatial resolution, which is usually identified with that of the confocal microscope coupled to the Brillouin interferometer. Conversely, here we demonstrate that the mean free path of acoustic phonons plays a major role in defining the resolution, especially for high numerical aperture confocal setups. Surprisingly, the resolution of elastography maps may even deteriorate when decreasing the scattering volume.

physics.optics↗

arXiv2019

Brillouin-derived viscoelastic parameters of hydrogel tissue models

Many problems in mechanobiology urgently require characterisation of the micromechanical properties of the fibrous proteins of cells and tissues. Brillouin light scattering has been proposed as a new optical elastography technique to meet this need, but the information contained in the Brillouin spectrum is still a matter of debate. Here we investigate this question using gelatin as a model system in which the macroscopic physical properties can be manipulated to mimic all the relevant biological states of matter, ranging from the liquid to the gel and the glassy phase. We demonstrate that Brillouin spectroscopy is a powerful tool to reveal both the elastic and viscous properties of biomaterials that are central to their biological functions.

physics.bio-ph↗

arXiv2019

Brillouin Light Scattering: Applications in Biomedical Sciences

Brillouin spectroscopy and imaging are emerging techniques in analytical science, biophotonics and biomedicine. They are based on Brillouin light scattering from acoustic waves or phonons in the GHz range, providing a nondestructive contactless probe of the mechanics on a micro-scale. Novel approaches and applications of these techniques to the field of biomedical sciences are discussed highlighting the theoretical foundations and experimental methods that have been developed to date, acknowledging that this is a fast moving field and a comprehensive account of the relevant literature is critically assessed here.

physics.bio-ph↗

arXiv2013

Depolarized light scattering and dielectric response of a peptide dissolved in water

The density and orientational relaxation of bulk water can be separately studied by depolarized light scattering (DLS) and dielectric spectroscopy (DS), respectively. Here we ask the question of what are the leading collective modes responsible for polarization anisotropy relaxation (DLS) and dipole moment relaxation (DS) of solutions involving mostly hydrophobic solute-water interfaces. We study, by atomistic molecular dynamics simulations, the dynamics and structure of hydration water interfacing N-Acetyl-leucine-methylamide (NALMA) dipeptide. The DLS response of the solution is consistent with three relaxation processes: bulk water, rotations of single solutes, and collective dipole-induced-dipole polarizability of the solutes, with the time-scale of 130-200 ps. No separate DLS response of the hydration shell has been identified by our simulations. Density fluctuations of the hydration layer, which largely contribute to the response, do not produce a dynamical process distinct from bulk water. We find that the structural perturbation of the orientational distribution of hydration waters by the dipeptide solute is quite significant and propagates 3-5 hydration layers into the bulk. This perturbation is still below that produced by hydrated globular proteins. Despite this structural perturbation, there is little change in the orientational dynamics of the hydration layers, compared to the bulk, as probed by both single-particle orientational dynamics and collective dynamics of the dipole moment of the shells. There is a clear distinction between the perturbation of the interfacial structure by the solute-solvent interaction potential and the perturbation of the interfacial dynamics by the corresponding forces.

cond-mat.soft↗

arXiv2013

Stress-induced modification of the boson peak scaling behavior

The scaling behavior of the so-called boson peak in glass-formers and its relation to the elastic properties of the system remains a source of controversy. Here, the boson peak in a binary reactive mixture is measured by Raman scattering (i) on cooling the unreacted mixture well below its glass transition temperature and (ii) after quenching to very low temperature the mixture at different times during isothermal polymerization. These different paths to the glassy phase are able to generate glasses with different amounts of residual stresses, as evidenced by the departure of the elastic moduli from a Cauchy-like relationship. We find that the scaling behavior of the boson peak with the properties of the elastic medium --- as measured by the Debye frequency --- holds for states in which the system is able to release internal stress and breaks down in the presence of residual stresses. These findings provide new insight into the boson peak behavior and are able to reconcile the apparently conflicting results presented in literature.

cond-mat.soft↗

arXiv2008

A molecular dynamics study of chemical gelation in a patchy particle model

We report event-driven molecular dynamics simulations of the irreversible gelation of hard ellipsoids of revolution containing several associating groups, characterizing how the cluster size distribution evolves as a function of the extent of reaction, both below and above the gel point. We find that in a very large interval of values of the extent of reaction, parameter-free mean-field predictions are extremely accurate, providing evidence that in this model the Ginzburg zone near the gel point, where non-mean field effects are important, is very limited. We also find that the Flory's hypothesis for the post-gelation regime properly describes the connectivity of the clusters even if the long-time limit of the extent of reaction does not reach the fully reacted state. This study shows that irreversibly aggregating asymmetric hard-core patchy particles may provide a close realization of the mean-field model, for which available theoretical predictions may help control the structure and the connectivity of the gel state. Besides chemical gels, the model is relevant to network-forming soft materials like systems with bioselective interactions, functionalized molecules and patchy colloids.

cond-mat.soft↗

arXiv2007

On the origin of the $λ$-transition in liquid Sulphur

Developing a novel experimental technique, we applied photon correlation spectroscopy using infrared radiation in liquid Sulphur around $T_λ$, i.e. in the temperature range where an abrupt increase in viscosity by four orders of magnitude is observed upon heating within few degrees. This allowed us - overcoming photo-induced and absorption effects at visible wavelengths - to reveal a chain relaxation process with characteristic time in the ms range. These results do rehabilitate the validity of the Maxwell relation in Sulphur from an apparent failure, allowing rationalizing the mechanical and thermodynamic behavior of this system within a viscoelastic scenario.

cond-mat.dis-nn↗

arXiv2003

Density fluctuations in the intermediate glass-former glycerol: a Brillouin light scattering study

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, $τ_α$, obtained by a full-spectrum analysis conforms to the $α$-scale universality, i.e. the values $τ_α$ 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.

cond-mat.soft↗

arXiv2002

Can experiments select the configurational component of excess entropy?

We introduce an experimental method of assessing the vibrational and configurational components of the excess entropy of a liquid over crystal, based on a joined investigation of dynamic and thermodynamic properties as a function of temperature and pressure. We analyze light scattering, dielectric, calorimetric and dilatometric measurements of three prototype glass formers, orthoterphenyl, salol, and glycerol. In all cases we find that about 70% of the excess entropy is configurational in nature.

cond-mat.soft↗