Equilibrium and non-equilibrium concentration fluctuations in a critical binary mixture

When a macroscopic concentration gradient is present across a binary mixture, long-ranged non-equilibrium concentration fluctuations (NCF) appear as a consequence of the coupling between the gradient and spontaneous equilibrium velocity fluctuations. Long-ranged equilibrium concentration fluctuations (ECF) may be also observed when the mixture is close to a critical point. Here we study the interplay between NCF and critical ECF in a near critical mixture aniline/cyclohexane in the presence of a vertical concentration gradient. To this aim, we exploit a commercial optical microscope and a simple, custom-made, temperature-controlled cell to obtain simultaneous static and dynamic scattering information on the fluctuations. We first characterise the critical ECF at fixed temperature $T$ above the upper critical solution temperature $T_{c}$, in the wide temperature range $T-T_{c}\in[0.1,30]$ $^{o}$C. In this range, we observe the expected critical scaling behaviour for both the scattering intensity and the mass diffusion coefficient and we determine the critical exponents $\gamma$, $\nu$ and $\eta$, which are found in agreement with the 3D Ising values. We then study the system in the two-phase region ($T<T_{c}$). In particular, we characterise the interplay between ECF and NCF when the mixture, initially at a temperature $T_{i}$, is rapidly brought to a temperature $T_{f}>T_{i}$. During the transient, a vertical diffusive mass flux is present that causes the onset of NCF, whose amplitude vanishes with time, as the flux goes to zero. We also study the time dependence of the equilibrium scattering intensity $I_{eq}$, of the crossover wave-vector $q_{co}$ and of the diffusion coefficient $D$ during diffusion and find that all these quantities exhibit an exponential relaxation enslaved to the diffusive kinetics.Comment: 11 pages, 4 figure

Dark Field Differential Dynamic Microscopy enables the accurate characterization of the roto-translational dynamics of bacteria and colloidal clusters

Micro- and nanoscale objects with anisotropic shape are key components of a variety of biological systems and inert complex materials, and represent fundamental building blocks of novel self-assembly strategies. The time scale of their thermal motion is set by their translational and rotational diffusion coefficients, whose measurement may become difficult for relatively large particles with small optical contrast. Here we show that Dark Field Differential Dynamic Microscopy is the ideal tool for probing the roto-translational Brownian motion of shape anisotropic particles. We demonstrate our approach by successful application to aqueous dispersions of non-motile bacteria and of colloidal aggregates of spherical particles

Dynamic scaling for the growth of non-equilibrium fluctuations during thermophoretic diffusion in microgravity

Diffusion processes are widespread in biological and chemical systems, where they play a fundamental role in the exchange of substances at the cellular level and in determining the rate of chemical reactions. Recently, the classical picture that portrays diffusion as random uncorrelated motion of molecules has been revised, when it was shown that giant non-equilibrium fluctuations develop during diffusion processes. Under microgravity conditions and at steady-state, non-equilibrium fluctuations exhibit scale invariance and their size is only limited by the boundaries of the system. In this work, we investigate the onset of non-equilibrium concentration fluctuations induced by thermophoretic diffusion in microgravity, a regime not accessible to analytical calculations but of great relevance for the understanding of several natural and technological processes. A combination of state of the art simulations and experiments allows us to attain a fully quantitative description of the development of fluctuations during transient diffusion in microgravity. Both experiments and simulations show that during the onset the fluctuations exhibit scale invariance at large wave vectors. In a broader range of wave vectors simulations predict a spinodal-like growth of fluctuations, where the amplitude and length-scale of the dominant mode are determined by the thickness of the diffuse layer.Comment: To appear in Scientific Report

Correcting artifacts from finite image size in Differential Dynamic Microscopy

Differential Dynamic Microscopy (DDM) analyzes traditional real-space microscope images to extract information on sample dynamics in a way akin to light scattering, by decomposing each image in a sequence into Fourier modes, and evaluating their time correlation properties. DDM has been applied in a number of soft-matter and colloidal systems. However, objects observed to move out of the microscope's captured field of view, intersecting the edges of the acquired images, can introduce spurious but significant errors in the subsequent analysis. Here we show that application of a spatial windowing filter to images in a sequence before they enter the standard DDM analysis can reduce these artifacts substantially. Moreover, windowing can increase significantly the accessible range of wave vectors probed by DDM, and may further yield unexpected information, such as the size polydispersity of a colloidal suspension

Differential dynamic microscopy microrheology of soft materials: A tracking-free determination of the frequency-dependent loss and storage moduli

Particle-tracking microrheology (PT-μr) exploits the thermal motion of embedded particles to probe the local mechanical properties of soft materials. Despite its appealing conceptual simplicity, PT-μr requires calibration procedures and operating assumptions that constitute a practical barrier to its wider application. Here we demonstrate differential dynamic microscopy microrheology (DDM-μr), a tracking-free approach based on the multiscale, temporal correlation study of the image intensity fluctuations that are observed in microscopy experiments as a consequence of the translational and rotational motion of the tracers. We show that the mechanical moduli of an arbitrary sample are determined correctly over a wide frequency range provided that the standard DDM analysis is reinforced with an iterative, self-consistent procedure that fully exploits the multiscale information made available by DDM. Our approach to DDM-μr does not require any prior calibration, is in agreement with both traditional rheology and diffusing wave spectroscopy microrheology, and works in conditions where PT-μr fails, providing thus an operationally simple, calibration-free probe of soft materials

Giant fluctuations and structural effects in a flocking epithelium

We thank S Henkes for useful discussions. FGia and RC acknowledge funding from the Italian Ministry of University and Scientific Research (MIUR) under the program Futuro in Ricerca—Project ANISOFT (RBFR125H0M) and from Regione Lombardia and CARIPLO foundation under the joint action Avviso congiunto per l'incremento dell'attrattivitá del sistema ricerca lombardo e della competitivitá dei ricercatori candidati su strumenti ERC—Project 2016-0998. CM, SC and GS acknowledge funding from Associazione Italiana per la Ricerca sul Cancro (AIRC 10168 and 18621), MIUR, the Italian Ministry of Health, Ricerca Finalizzata (RF0235844), Worldwide Cancer Research (AICR-14-0335), and the European Research Council (Advanced-ERC-268836). CM was also supported by Fondazione Umberto Veronesi and SC by an AIRC fellowship. FGin acknowledges support from the Marie Curie Career Integration Grant (CIG) PCIG13-GA-2013-618399, and wish to thank the University of Milan and LibrOsteria for their hospitality while this work was underway.Peer reviewedPostprin

Correction: Equilibrium gels of low-valence DNA nanostars: a colloidal model for strong glass formers

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Protein sizing with Differential Dynamic Microscopy

Introduced more than fifty years ago, dynamic light scattering is routinely used to determine the size distribution of colloidal suspensions, as well as of macromolecules in solution, such as proteins, nucleic acids, and their complexes. More recently, differential dynamic microscopy has been proposed as a way to perform dynamic light scattering experiments with a microscope, with much less stringent constraints in terms of cleanliness of the optical surfaces, but a potentially lower sensitivity due to the use of camera-based detectors. In this work, we push bright-field differential dynamic microscopy beyond known limits and show it to be sufficiently sensitive to size small macromolecules in diluted solutions. By considering solutions of three different proteins (Bovine Serum Albumin, Lysozyme, and Pepsin), we accurately determine the diffusion coefficient and hydrodynamic radius of both single proteins and small protein aggregates down to concentrations of a few milligrams per milliliter. In addition, we present preliminary results showing unexplored potential for the determination of virial coefficients. Our results are in excellent agreement with the ones obtained in parallel with a state-of-the-art commercial dynamic light scattering setup, showing that differential dynamic microscopy represents a valuable alternative for rapid, label-free protein sizing with an optical microscope