Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics.
Understanding the glass transition requires getting the picture of the dynamical processes that intervene in it. Glass-forming liquids show a characteristic decoupling of relaxation processes when they are cooled down towards the glassy state. The faster (βJG) process is still under scrutiny, and its full explanation necessitates information at the microscopic scale. To this aim, nuclear γ-resonance time-domain interferometry (TDI) has been utilized to investigate 5-methyl-2-hexanol, a hydrogen-bonded liquid with a pronounced βJG process as measured by dielectric spectroscopy. TDI probes in fact the center-of-mass, molecular dynamics at scattering-vectors corresponding to both inter- and intra-molecular distances. Our measurements demonstrate that, in the undercooled liquid phase, the βJG relaxation can be visualized as a spatially-restricted rearrangement of molecules within the cage of their closest neighbours accompanied by larger excursions which reach out at least the inter-molecular scale and are related to cage-breaking events. In-cage rattling and cage-breaking processes therefore coexist in the βJG relaxation.
Tardigrades are microscopic animals that survive desiccation by inducing biostasis. To survive drying tardigrades rely on intrinsically disordered CAHS proteins that form gels. However, the sequence features and mechanisms underlying gel formation and the necessity of gelation for protection have not been demonstrated. Here we report a mechanism of gelation for CAHS D similar to that of intermediate filaments. We show that gelation restricts molecular motion, immobilizing and protecting labile material from the harmful effects of drying. In vivo, we observe that CAHS D forms fiber-like condensates during osmotic stress. Condensation of CAHS D improves survival of osmotically shocked cells through at least two mechanisms: reduction of cell volume change and reduction of metabolic activity. Importantly, condensation of CAHS D is reversible and metabolic rates return to control levels after CAHS condensates are resolved. This work provides insights into how tardigrades induce biostasis through the self-assembly of CAHS gels.
Residual stresses are well-known companions of all glassy materials. They affect and, in many cases, even strongly modify important material properties like the mechanical response and the optical transparency. The mechanisms through which stresses affect such properties are, in many cases, still under study, and their full understanding can pave the way to a full exploitation of stress as a primary control parameter. It is, for example, known that stresses promote particle mobility at small length scales, e.g., in colloidal glasses, gels, and metallic glasses, but this connection still remains essentially qualitative. Exploiting a preparation protocol that leads to colloidal glasses with an exceptionally directional built-in stress field, we characterize the stress-induced dynamics and show that it can be visualized as a collection of “flickering,” mobile regions with linear sizes of the order of ≈20 particle diameters (≈2 μm here) that move cooperatively, displaying an overall stationary but locally ballistic dynamics.
When a liquid is cooled to produce a glass its dynamics, dominated by the structural relaxation, become very slow, and at the glass-transition temperature Tg its characteristic relaxation time is about 100 s. At slightly elevated temperatures (~1.2 Tg) however, a second process known as the Johari-Goldstein relaxation, βJG, decouples from the structural one and remains much faster than it down to Tg. While it is known that the βJG-process is strongly coupled to the structural relaxation, its dedicated role in the glass-transition remains under debate. Here we use an experimental technique that permits us to investigate the spatial and temporal properties of the βJG relaxation, and give evidence that the molecules participating in it are highly mobile and spatially connected in a system-spanning, percolating cluster. This correlation of structural and dynamical properties provides strong experimental support for a picture, drawn from theoretical studies, of an intermittent mosaic structure in the deeply supercooled liquid phase.
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