We use X-Ray Photon Correlation Spectroscopy to investigate the structural relaxation process in a metallic glass on the atomic length scale. We report evidence for a dynamical crossover between the supercooled liquid phase and the metastable glassy state, suggesting different origins of the relaxation process across the transition. Furthermore, using different cooling rates we observe a complex hierarchy of dynamic processes characterized by distinct aging regimes. Strong analogies with the aging dynamics of soft glassy materials, such as gels and concentrated colloidal suspensions, point at stress relaxation as a universal mechanism driving the relaxation dynamics of out-of-equilibrium systems.PACS numbers: 64.70.pe,65.60.+a,64.70.pv Glasses are usually defined as liquids that are trapped in a metastable state from which they slowly evolve toward the corresponding equilibrium phase [1,2]. Although aging is known since centuries, a clear picture of the dynamics in the glassy state is still missing [3,4]. Most of the experimental information available on aging concerns macroscopic quantities, such as viscosity or elastic moduli [5][6][7][8][9][10][11], or focuses on dielectric relaxation [12][13][14][15][16][17], a quantity that is often difficult to relate directly to the particle-level dynamics. From these measurements, a characteristic time for the evolution towards equilibrium can be extracted, but no direct information on the connection between aging and the underlying microscopic dynamics is available. By contrast, a full understanding of aging requires a detailed description of the particle-level dynamics, and in particular of the structural relaxation time τ , the characteristic time for a system to rearrange its structure on the length scale of its constituents. While the structural relaxation has been widely investigated in the liquid phase, only a few studies report on the behaviour of τ below the glass transition temperature, T g [14-16, 18]. Molecular dynamics simulations show that τ increases linearly or sub-linearly with the waiting time, t w , and suggest the possibility of rescaling the measured quantities on a single master curve (time-waiting time superposition principle) [18]. Studies in this direction, however, have led to debated results [5,12,13,17,19]. Consequently, several key questions remain unanswered: what is the fate of the structural relaxation process when the system falls out of equilibrium in the glassy state? How does it depend on the thermal history and the waiting time? What physical mechanism is responsible for structural relaxation? Here, we address these questions by presenting an experimental investigation of the structural relaxation on the atomic length scale in a metallic glass former, in both the supercooled liquid and the glassy state, as a function of temperature and waiting time, and for different thermal histories. We use X-Ray Photon Correlation Spectroscopy (XPCS) to study Mg 65 Cu 25 Y 10 , a well-known glass former with a relatively low T g ∼ 405 K and a st...

The dynamic properties of nanoparticles suspended in a supercooled glass forming liquid are studied by x-ray photon correlation spectroscopy. While at high temperatures the particles undergo Brownian motion the measurements closer to the glass transition indicate hyperdiffusive behavior. In this state the dynamics is independent of the local structural arrangement of nanoparticles, suggesting a cooperative behavior governed by the near-vitreous solvent.

Still very little is known on the relaxation dynamics of glasses at the microscopic level due to the lack of experiments and theories. It is commonly believed that glasses are in a dynamical arrested state, with relaxation times too large to be observed on human time scales. Here we provide the experimental evidence that glasses display fast atomic rearrangements within a few minutes, even in the deep glassy state. Following the evolution of the structural relaxation in a sodium silicate glass, we find that this fast dynamics is accompanied by the absence of any detectable aging, suggesting a decoupling of the relaxation time and the viscosity in the glass. The relaxation time is strongly affected by the network structure with a marked increase at the mesoscopic scale associated with the ion-conducting pathways. Our results modify the conception of the glassy state and asks for a new microscopic theory.

We present x-ray photon correlation spectroscopy measurements of the atomic dynamics in a Zr 67 Ni 33 metallic glass, well below its glass transition temperature. We find that the decay of the density fluctuations can be well described by compressed, thus faster than exponential, correlation functions which can be modeled by the well-known Kohlrausch-Williams-Watts function with a shape exponent β larger than one. This parameter is furthermore found to be independent of both waiting time and wave-vector, leading to the possibility to rescale all the correlation functions to a single master curve. The dynamics in the glassy state is additionally characterized by different aging regimes which persist in the deep glassy state. These features seem to be universal in metallic glasses and suggest a nondiffusive nature of the dynamics. This universality is supported by the possibility of describing the fast increase of the structural relaxation time with waiting time using a unique model function, independently of the microscopic details of the system.

Nowadays powerful X-ray sources like synchrotrons and free-electron lasers are considered as ultimate tools for probing microscopic properties in materials. However, the correct interpretation of such experiments requires a good understanding on how the beam affects the properties of the sample, knowledge that is currently lacking for intense X-rays. Here we use X-ray photon correlation spectroscopy to probe static and dynamic properties of oxide and metallic glasses. We find that although the structure does not depend on the flux, strong fluxes do induce a non-trivial microscopic motion in oxide glasses, whereas no such dependence is found for metallic glasses. These results show that high fluxes can alter dynamical properties in hard materials, an effect that needs to be considered in the analysis of X-ray data but which also gives novel possibilities to study materials properties since the beam can not only be used to probe the dynamics but also to pump it.

We present a new method to extract the intermediate scattering function from series of coherent diffraction patterns taken with 2D detectors. Our approach is based on analyzing speckle patterns in terms of photon statistics. We show that the information obtained is equivalent to the conventional technique of calculating the intensity autocorrelation function. Our approach represents a route for correlation spectroscopy on ultrafast timescales at X-ray free-electron laser sources.

Since its first experimental demonstration in 1999, coherent diffractive imaging (CDI) has been applied to image a broad range of samples using advanced synchrotron radiation, X-ray free-electron lasers, high harmonic generation and electrons. Here, the first experimental demonstration of cryogenic CDI for quantitative three-dimensional imaging of whole frozen-hydrated cells is reported. As a proof of principle, the three-dimensional mass density of the sub-cellular organization of a Neospora caninum cell is determined based on its natural contrast.

Predictive knowledge of ion transport in electrolytes which bridges microscopic and macroscopic length scales is imperative to design new ion conductors and to simulate device performance. Here, we employed a...