arXiv subjects

Andrei Fluerasu

Publications and source records attributed to Andrei Fluerasu.

At least 19 recordsLinked to original sources

arXiv2026

Probing Non-Equilibrium Grain Boundary Dynamics with XPCS and Domain-Adaptive Machine Learning

Grain-boundary (GB) dynamics control the stability, mechanical, and functional response of nanocrystalline materials, but direct experimental access to their slow non-equilibrium motion has been limited. Here we establish X-ray photon correlation spectroscopy (XPCS), combined with domain-adaptive machine learning, as a quantitative probe of GB dynamics. Temperature- and grain-size-dependent two-time XPCS measurements in nanocrystalline silicon reveal pronounced departures from time-translation invariance, showing that GB relaxation can remain far from equilibrium over experimental timescales. However, direct extraction of quantitative physical information from these high-dimensional, noisy fluctuation maps faces a significant challenge. To overcome this barrier, we develop a semi-supervised learning framework that transfers physical parameter labels from continuum simulations to unlabeled experimental XPCS maps through domain-adaptive representation alignment. This AI-augmented approach enables the extraction of key kinetic parameters, including bulk diffusivity, GB stiffness, and effective GB concentration, directly from experimental XPCS measurements. Our results show how machine learning can transform indirect fluctuation signals into quantitative materials dynamics, providing a general route to study non-equilibrium defect motion in solids.

cond-mat.mtrl-sci↗

arXiv2025

Heterogeneous dynamics in a polymer solution revealed through measurement of ultraslow convection

Understanding solution-phase aggregation and dynamics in complex fluids is critical for material processing, yet widely used dynamic light scattering (DLS) fails for strongly attenuating systems such as conjugated polymers. We use X-ray photon correlation spectroscopy (XPCS) to probe the dynamics of a polymer, PM7, in toluene, revealing unexpected oscillations in the autocorrelation function that show vertical flow during measurement. Despite the relatively low X-ray absorption, measured flow velocities scale with X-ray beam power and suggest convective transport. Our analyses reveal both mobile and static scatterers that together produce oscillatory, heterodyne features in the measured correlation functions. Finite element simulations predict flow velocities much larger than observed, suggesting that entanglements of the aggregates slow their motion. These results provide a direct measurement of ultra-slow convection and highlight the need to explicitly account for even modest beam heating in interpreting XPCS results. Moreover, the observation of distinct scatterer populations underscores the structural complexity of conjugated polymer solutions.

cond-mat.soft↗

arXiv2025

Metastable short-range charge order in superconducting CuxTiSe2

In a vast array of materials, including cuprates, transition metal dichalcogenides (TMDs) and rare earth tritellurides, superconductivity is found in the vicinity of short-range charge density wave (CDW) order. The crossover from long-range to short-range charge order often occurs as quenched disorder is introduced, yet it is unclear how this disorder disrupts the CDW. Here, using x-ray photon correlation spectroscopy (XPCS), we investigate the prototypical TMD superconductor CuxTiSe2 and show that disorder induces substantial CDW dynamics. We observe CDW phase fluctuations on a timescale of minutes to hours above the nominal transition temperature while the order parameter amplitude remains finite. These long timescale fluctuations prevent the system from finding the global free energy minimum upon cooling and ultimately traps it in a short-range ordered metastable state. Our findings demonstrate how correlated disorder can give rise to a distinct mechanism of domain formation that may be advantageous to the emergence of superconductivity.

cond-mat.str-el↗

arXiv2024

Quantum Imaging with X-rays

Quantum imaging encompasses a broad range of methods that exploit the quantum properties of light to capture information about an object. One such approach involves using a two-photon quantum state, where only one photon interacts with the object being imaged while its entangled partner carries spatial or temporal information. To implement this technique, it is necessary to generate specific quantum states of light and detect photons at the single-photon level. While this method has been successfully demonstrated in the visible electromagnetic spectrum, extending it to X-rays has faced significant challenges due to the difficulties in producing a sufficient rate of X-ray photon pairs and detecting them with adequate resolution. Here, we demonstrate record high rates of correlated X-ray photon pairs produced via a spontaneous parametric down-conversion process and we employ these photons to perform quantum correlation imaging of several objects, including a biological sample (E. cardamomum seedpod). Notably, we report an unprecedented detection rate of about 6,300 pairs per hour and the observation of energy anti-correlation for the X-ray photon pairs. We also present a detailed analysis of the properties of the down-converted X-ray photons, as well as a comprehensive study of the correlation imaging formation, including a study of distortions and corrections. These results mark a substantial advancement in X-ray quantum imaging, expanding the possibilities of X-ray quantum optical technologies, and illustrating the pathway towards enhancing biological imaging with reduced radiation doses.

quant-ph↗

arXiv2024

Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid

Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) -- directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation.

cond-mat.soft↗

arXiv2024

In situ coherent X-ray scattering reveals polycrystalline structure and discrete annealing events in strongly-coupled nanocrystal superlattices

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and X-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in situ in their native chemical environments, thus extending the reach of high-resolution coherent X-ray characterization to the benefit of a much wider range of physical systems.

cond-mat.mtrl-sci↗

arXiv2023

Imaging of X-ray Pairs in a Spontaneous Parametric Down-Conversion Process

Spontaneous parametric down-conversion is a vital method for generating correlated photon pairs in the visible and near-infrared spectral regions; however, its extension to X-ray frequencies has faced substantial barriers. Here, we present an advancement in correlated X-ray pair generation and detection by employing a two-dimensional pixelated detector to obtain the first direct image of the pair distribution. Our study explores and directly visualizes the down-conversion process, revealing the characteristic ring structure of coincident photon pairs and demonstrating robust spatial correlations. A significant finding is the observation of energy anti-correlation, achieved at an unprecedented rate of approximately 4,100 pairs/hour, far exceeding previous reports in the literature. We believe these results represent a significant leap in X-ray quantum imaging, unlocking the potential for enhanced imaging of biological materials with reduced doses and broadening the applicability of X-ray quantum optical technologies.

physics.optics↗

arXiv2023

Dichotomic Aging Behaviour in a Colloidal Glass

An unexpected dichotomic long time aging behaviour is observed in a glassy colloidal clay suspension investigated by X-Ray Photon Correlation Spectroscopy and Dynamic Light Scattering. In the long time aging regime the intensity autocorrelations are non-exponential, following the Kohlrausch-Williams-Watts functional form with exponent bQ. We show that for spontaneously aged samples a stretched behaviour (\beta_Q < 1) is always found. Surprisingly a compressed exponent (\beta_Q > 1) appears only when the system is rejuvenated by application of a shear field. In both cases the relaxation times scale as Q^{-1}. These observations shed light on the origin of compressed exponential behaviour and helps in classifying previous results in the literature on anomalous dynamics.

cond-mat.soft↗

arXiv2023

Coherent X-ray Spectroscopy Elucidates Nanoscale Dynamics of Plasma-Enhanced Thin-Film Growth

Sophisticated thin film growth techniques increasingly rely on the addition of a plasma component to open or widen a processing window, particularly at low temperatures. However, the addition of the plasma into the growth environment also complicates the surface dynamical evolution. Taking advantage of continued increases in accelerator-based X-ray source brilliance, this real-time study uses X-ray Photon Correlation Spectroscopy (XPCS) to elucidate the nanoscale surface dynamics during Plasma-Enhanced Atomic Layer Deposition (PE-ALD) of an epitaxial indium nitride film. XPCS examines the evolution of the coherent X-ray scattering speckle pattern, which is a fingerprint of the unique sample microstructure at each moment in time. In PE-ALD, ultrathin films are synthesized from repeated cycles of alternating self-limited surface reactions induced by temporally-separated pulses of material precursor and plasma reactant, allowing the influence of each on the evolving morphology to be examined. During the heteroepitaxial 3D growth examined here, sudden changes in surface structure during initial film growth, consistent with numerous overlapping stress-relief events, are observed. When the film becomes continuous, the nanoscale surface morphology abruptly becomes long-lived with correlation time spanning the period of the experiment. Throughout the growth experiment, there is a consistent repeating pattern of correlations associated with the cyclic growth process, which is modeled as transitions between different surface states. The plasma exposure does not simply freeze in a structure that is then built upon in subsequent cycles, but rather there is considerable surface evolution during all phases of the growth cycle.

cond-mat.mtrl-sci↗

arXiv2023

Local step-flow dynamics in thin film growth with desorption

Desorption of deposited species plays a role in determining the evolution of surface morphology during crystal growth when the desorption time constant is short compared to the time to diffuse to a defect site, step edge or kink. However, experiments to directly test the predictions of these effects are lacking. Novel techniques such as \emph{in-situ} coherent X-ray scattering can provide significant new information. Herein we present X-ray Photon Correlation Spectroscopy (XPCS) measurements during diindenoperylene (DIP) vapor deposition on thermally oxidized silicon surfaces. DIP forms a nearly complete two-dimensional first layer over the range of temperatures studied (40 - 120 $^{\circ}$C), followed by mounded growth during subsequent deposition. Local step flow within mounds was observed, and we find that there was a terrace-length-dependent behavior of the step edge dynamics. This led to unstable growth with rapid roughening ($\beta>0.5$) and deviation from a symmetric error-function-like height profile. At high temperatures, the grooves between the mounds tend to close up leading to nearly flat polycrystalline films. Numerical analysis based on a 1 + 1 dimensional model suggests that terrace-length dependent desorption of deposited ad-molecules is an essential cause of the step dynamics, and it influences the morphology evolution.

cond-mat.mtrl-sci↗

arXiv2022

Exploring Nanofibrous Networks with X-ray Photon Correlation Spectroscopy

Nanofibrous networks are the foundation and natural building strategy for all life forms on our planet. Apart from providing structural integrity to cells and tissues, they also provide a porous scaffold allowing transport of substances, where the resulting properties rely on the nanoscale network structure. Recently, there has been a great deal of interest in extracting and reassembling biobased nanofibers to create sustainable, advanced materials with applications ranging from high-performance textiles to artificial tissues. However, achieving structural control of the extracted nanofibers is challenging as it is strongly dependent on the extraction methods and source materials. Furthermore, the small nanofiber cross-sections and fast Brownian dynamics make them notoriously difficult to characterize in dispersions. In this work, we study the diffusive motion of spherical gold nanoparticles in semi-dilute networks of cellulose nanofibers (CNFs) using X-ray Photon Correlation Spectroscopy (XPCS). We find that the motion becomes increasingly subdiffusive with higher CNF concentration, where the dynamics can be decomposed into several superdiffusive relaxation modes in reciprocal space. Using simulations of confined Brownian dynamics in combination with simulated XPCS-experiments, we observe that the dynamic modes can be connected to pore sizes and inter-pore transport properties in the network. The demonstrated analytical strategy by combining experiments using tracer particles with a digital twin may be the key to understand nanoscale properties of nanofibrous networks.

cond-mat.soft↗

arXiv2020

Measurement of Ehrlich-Schwoebel barrier contribution to the self-organized formation of ordered surface patterns on Ge(001)

Normal incidence 1 keV Ar$^+$ ion bombardment leads to amorphization and ultrasmoothing of Ge at room temperature, but at elevated temperatures the Ge surface remains crystalline and is unstable to the formation of self-organized nanoscale patterns of ordered pyramid-shaped pits. The physical phenomenon distinguishing the high temperature patterning from room temperature ultrasmoothing is believed to be a surface instability due to the Ehrlich-Schwoebel barrier for diffusing vacancies and adatoms, which is not present on the amorphous material. This real-time GISAXS study compares smoothing of a pre-patterned Ge sample at room temperature with patterning of an initially flat Ge sample at an elevated temperature. In both experiments, when the nanoscale structures are relatively small in height, the average kinetics can be explained by a linear theory. The linear theory coefficients, indicating surface stability or instability, were extracted for both experiments. A comparison between the two measurements allows estimation of the contribution of the Ehrlich-Schwoebel barrier to the self-organized formation of ordered nanoscale patterns on crystalline Ge surfaces.

cond-mat.mtrl-sci↗

arXiv2020

Nanoscale dynamics during self-organized ion beam patterning of Si: I. Ar$^+$ Bombardment

Coherent grazing-incidence small-angle X-ray scattering is used to investigate the average kinetics and the fluctuation dynamics during self-organized nanopatterning of silicon by Ar$^+$ bombardment at 65$^{\circ}$ polar angle. At early times, the surface behavior can be understood within the framework of linear theory. The transition away from the linear theory behavior is observed in the dynamics through the intensity correlation function. It quickly evolves to exhibit stretched exponential decay on short length scales and compressed exponential decay on length scales corresponding the dominant structural length scale - the ripple wavelength. The correlation times also peak strongly at the ripple length scale. This behavior has notable similarities but also significant differences with the phenomenon of de Gennes narrowing. Overall, this dynamics behavior is found to be consistent with simulations of a nonlinear growth model.

cond-mat.mtrl-sci↗

arXiv2020

Nanoscale dynamics during self-organized ion beam patterning of Si: II. Kr$^+$ Bombardment

Despite extensive study, fundamental understanding of self-organized patterning by broad-beam ion bombardment is still incomplete and controversial. Understanding the nanopatterning of elemental semiconductors, particularly silicon, is both foundational for the broader field and of intrinsic scientific and technological interest itself. This is the second component of a two-part investigation of the kinetics and fluctuation dynamics of self-organized nanoscale ripple development on silicon during 1 keV Ar$^+$ (Part I) and Kr$^+$ bombardment. Here, it's found that the ion-enhanced viscous flow relaxation is essentially equal for Kr$^+$-induced patterning as previously found for Ar$^+$ patterning. The magnitude of the surface curvature dependent roughening rate in the early stage kinetics is larger for Kr$^+$ than for Ar$^+$, qualitatively consistent with expectations for erosive and mass redistributive contributions to the initial surface instability. As with the Ar$^+$ case, fluctuation dynamics in the late stage show a peak in correlation time at the length scale corresponding to the dominant structural feature on the surface -- the ripples. Analogy is made to the phenomenon of de Gennes narrowing in liquids, but significant differences are also pointed out. Finally, it's shown that speckle motion during the surface evolution can be analyzed to determine spatial inhomogeneities in erosion rate and ripple velocity on the surface. This allows the direction and speed of ripple motion to be measured in real time, a unique capability for measuring these fundamental parameters outside the specialized environment of FIB/SEM systems.

cond-mat.mtrl-sci↗

arXiv2020

de Gennes Narrowing and the Relationship Between Structure and Dynamics in Self-Organized Ion Beam Nanopatterning

Investigating the relationship between structure and dynamical processes is a central goal in condensed matter physics. Perhaps the most noted relationship between the two is the phenomenon of de Gennes narrowing, in which relaxation times in liquids are proportional to the scattering structure factor. Here a similar relationship is discovered during the self-organized ion beam nanopatterning of silicon using coherent x-ray scattering. However, in contrast to the exponential relaxation of fluctuations in classic de Gennes narrowing, the dynamic surface exhibits a wide range of behaviors as a function of length scale, with a compressed exponential relaxation at lengths corresponding to the dominant structural motif - self-organized nanoscale ripples. These behaviors are reproduced in simulations of a nonlinear model describing the surface evolution. We suggest that the compressed exponential behavior observed here is due to the morphological persistence of the self-organized surface ripple patterns which form and evolve during ion beam nanopatterning.

cond-mat.mes-hall↗

arXiv2018

Coherent X-ray measurement of step-flow propagation during growth on polycrystalline thin film surfaces

The properties of artificially grown thin films are strongly affected by surface processes during growth. Coherent X-rays provide an approach to better understand such processes and fluctuations far from equilibrium. Here we report results for vacuum deposition of C$_{60}$ on a graphene-coated surface investigated with X-ray Photon Correlation Spectroscopy in surface-sensitive conditions. Step-flow is observed through measurement of the step-edge velocity in the late stages of growth after crystalline mounds have formed. We show that the step-edge velocity is coupled to the terrace length, and that there is a variation in the velocity from larger step spacing at the center of crystalline mounds to closely-spaced, more slowly propagating steps at their edges. The results extend theories of surface growth, since the behavior is consistent with surface evolution driven by processes that include surface diffusion, the motion of step-edges, and attachment at step edges with significant step-edge barriers.

cond-mat.mtrl-sci↗

arXiv2012

Dynamics in dense hard-sphere colloidal suspensions

The dynamic behavior of a hard-sphere colloidal suspension was studied by X-ray Photon Correlation Spectroscopy and Small Angle X-ray Scattering over a wide range of particle volume fractions. The short-time mobility of the particles was found to be smaller than that of free particles even at relatively low concentrations, showing the importance of indirect hydrodynamic interactions. Hydrodynamic functions were derived from the data and for moderate particle volume fractions (> 0.40) there is a good agreement with earlier many-body theory calculations by Beenakker and Mazur [C.W.J. Beenakker and P. Mazur, Physica A 120, 349 (1984)]. Important discrepancies appear at higher concentrations, above ~0.40, where the hydrodynamic effects are overestimated by the Beenakker-Mazur theory, but predicted accurately by an accelerated Stokesian dynamics algorithm developed by Banchio and Brady [A.J. Banchio and J. F. Brady, J. Chem. Phys. 118, 10323 (2003)]. For the relaxation rates, good agreement was also found between the experimental data and a scaling form predicted by Mode Coupling Theory. In the high concentration range, with the fluid suspensions approaching the glass transition, the long-time diffusion coefficient was compared with the short-time collective diffusion coefficient to verify a scaling relation previously proposed by Segre and Pusey [P.N. Segre and P.N. Pusey, Phys. Rev. Lett. 77, 771 (1996)]. We discuss our results in view of previous experimental attempts to validate this scaling law [L. Lurio et al., Phys. Rev. Lett. 84, 785 (2000)]

cond-mat.soft↗

arXiv2010

Slow dynamics in an azopolymer molecular layer studied by x-ray photon correlation spectroscopy

We report the results of X-ray photon correlation spectroscopy (XPCS) experiments on Langmuir Blodgett multilayers of a photosensitive azo-polymer. Time correlation functions have been measured at different temperatures and momentum transfers (q) and under different illumination conditions (darkness, UV or visible). The correlation functions are well described by the Kohlrausch-Williams-Watts (KWW) form with relaxation times that are proportional to q^-1, which in other systems have been explained in terms of intermittent rearrangements [L. Cipelletti et al., Phys. Rev. Lett. 84, 2275-2278 (2000)] or random dipolar interactions within an elastic medium [J.- P. Bouchaud and E. Pitard, Eur. Phys. J. E 6, 231-236 (2001)]. The characteristic relaxation times follow the well known Vogel-Fulcher-Tammann law describing the temperature dependence of the bulk viscosity of this polymer. UV photoperturbation accelerates the relaxation dynamics, in qualitative agreement with the fluidification effect of UV photo-perturbation previously observed by surface rheometry, and is used to drive the system out of equilibrium. Transient dynamics is characterized, by the variance chi of the two-times correlation functions. A clear peak in chi appears at a well defined time tau_C which scales with q^-1 and with the ageing time, in a similar fashion as previously reported in colloidal suspensions [O. Dauchot et al., Phys. Rev. Lett. 95, 265701 (2005)]. From an accurate analysis of the correlation functions we could demonstrate a temperature dependent cross-over from KWW compressed to simple exponential behaviour, which is modified by the fluidification due to the optical pumping of the cis-trans isomerisation of the side-chain azobenzene group.

cond-mat.soft↗