Selective visualization of multiple organic components in small-angle X-ray scattering (SAXS) studies remains a major challenge in complex soft matter systems due to limited electron density contrast. Here, we introduce contrast-engineered polymeric nanoparticles (PNPs) as organic probes for multicomponent SAXS imaging. Well-defined, monomodal cationic PNPs prepared by polymerization-induced self-assembly (PISA) were loaded with the iodine-containing molecule 1,4-diiodobenzene, increasing particle electron density while preserving particle size, morphology, colloidal stability, and surface properties. Incorporation of iodine increased the PNP scattering 2 signal by 57%, improving signal-to-noise ratios and expanding the experimental parameter space for SAXS imaging. To demonstrate the capabilities of the contrast-engineered nanoparticles, they were used to study the flow-induced alignment and spinning of cellulose nanofibril (CNF) filaments. The PNPs were used as spatially resolved tracers to simultaneously visualize and distinguish between sheath flows. The measurements showed that the gelling stream remains confined near the channel walls and does not penetrate the detaching sheath or CNF core, clarifying how the flow architecture supports filament formation. These findings establish contrastengineered polymer nanoparticles as versatile organic probes for SAXS and demonstrate a general strategy for resolving transport, segregation, and spatial organization in multicomponent soft matter systems.

X-rays are commonly used in imaging experiments due to their penetration power, which enables non-destructive resolution of internal structures in samples that are opaque to visible light. Time-resolved X-ray tomography is the state-of-the-art method for obtaining volumetric 4D (3D + time) information by rotating the sample and acquiring projections from different angular viewpoints over time. This method enables studies to address a plethora of research questions across various scientific disciplines. However, it has several limitations, such as incompatibility with single-shot experiments, challenges in rotating complex sample environments that restrict the achievable rotation speed or range, and the introduction of centrifugal forces that can affect the sample's dynamics. These limitations can hinder and even preclude the study of certain dynamics. Here, we present an implementation of an alternative approach, X-ray multi-projection imaging (XMPI), which eliminates the need for sample rotation. Instead, the direct incident X-ray beam is split into beamlets using beam splitting X-ray optics. These beamlets intersect at the sample position from different angular viewpoints, allowing multiple projections to be acquired simultaneously. We commissioned this setup at the ForMAX beamline at MAX IV, the first operational diffraction-limited storage ring. We present projections acquired from two different sample systems – fibers under mechanical load and particle suspension in multiphase flow – with distinct spatial and temporal resolution requirements. We demonstrate the capabilities of the ForMAX XMPI setup using the detector's full analog-to-digital converter range for the relevant sample-driven spatiotemporal resolutions: (i) at least 12.5 kHz frame rates with 4 µm pixel sizes (fibers) and (ii) 40 Hz acquisitions with 1.3 µm pixel sizes (multiphase flows). The presented setup and results form the basis for a permanent XMPI endstation at ForMAX, offering flexibility to adapt to the spatiotemporal requirements of the studied dynamics.

Multiphase flows where particles, bubbles, or droplets are suspended in a fluid govern critical processes in biology, medicine, materials processing, and geophysics. However, observing their microscale dynamics in opaque systems has remained a fundamental challenge. We present Synchrotron X-ray Multi-Projection Imaging (XMPI), a novel approach enabling four-dimensional (3D + time) tracking of microparticles in visibly opaque suspension flows without requiring sample rotation. By capturing simultaneous projections from multiple angles using beam-split X-rays at synchrotron facilities, we resolve instantaneous particle positions and trajectories in opaque fluids such as blood. We demonstrate the potential of XMPI through individual particle tracking velocimetry (3D PTV) in dilute conditions, as well as multi-projection image velocimetry in dense suspensions. The methodology provides otherwise inaccessible experimental validation for particle-resolved computational fluid dynamics models and allows, e.g., observation of inertial focusing effects and microstructural dynamics relevant to suspension rheology and biomedical flows. This work paves the way for high-resolution, time-resolved 4D imaging of complex multiphase flows across a range of scientific and industrial applications. Combining XMPI with recent AI-supported 4D reconstruction algorithms opens a new spatiotemporal frontier for high-speed, rotation-free microtomography.

ABSTRACT Nano‐sized hydrogel drug carriers with tailored hydro‐ and lipophilicity are designed and their encapsulation and structure‐forming capabilities investigated in real‐time. These nano‐carriers are built from cellulose and peptide hydrogels in tandem with a nano‐stacked interwoven design and alternating hydro‐ and lipophilicity, thus enabling tuning of the lipophilicity of the carrier mesh for drugs of complementary lipophilicities. This allows for a variety of therapeutic applications, based on the nanoproperties of the hydrogel. Time‐resolved and in situ grazing incidence x‐ray scattering studies confirm the design and hydro‐ and lipophilicities of the fiber‐hydrogel composite and conclude their ability for carrying drugs of complementary properties site specific. This approach allows for a novel way of understanding the functionality of drug carriers using photon‐based approach.

Even at very low concentrations, the rheology of dispersions of charged semiflexible nanofibers differs from the rheology of the pure liquid, given the fiber charge, morphology, and interactions. At the nanoscale, the thermal motion of fibers is driven by the collective motion of the solvent molecules, but to what extent does the fiber presence and motion affect the self-diffusion of the liquid molecules? By studying the self-diffusion of water in dilute nanofiber dispersions using experiments and simulations, we can show that the interplay of fiber charge and motion on water mobility is more significant than the effect of the excluded volume caused by the charged particles.

Shoe press belts contribute significantly to the overall dewatering performance in the press section of a paper machine. Within the shoe press nip, the press belt faces a dynamic and multidimensional load that mainly leads to a compression of the structure. As this will cause a loss in void volume, knowledge of the dynamic compression characteristics of shoe press belts is crucial for optimized dewatering. A novel method was developed to examine the dynamic compression characteristics of grooved polyurethane press belts. Therefore, an experimental setup allowing realistic boundary conditions to test specimens was placed in a servo-hydraulic testing machine. Press belt specimens with different matrix material formulations and groove patterns were tested under varying load rates equivalent to different paper machine operational speeds. The results showed an evident sensitivity of the dynamic compression stiffness to the operational speed of the paper machine. This behavior was seen to be more sensitive to changes in the matrix material formulation than to adaptions of the groove pattern. As a result, the compression of the press belt within a shoe press nip is not only influenced by the peak pressure within the shoe press nip but also depends on the operational speed of the paper machine.

A novel concept of nano-scaled interwoven templates for drug delivery with alternating hydro- and lipophilicity properties is introduced. They are built from cellulose and peptide hydrogel in tandem, and characterized by a nano-stacked interwoven design, thus enabling for tuning the lipophilicity in the mesh nano-domains in which drug candidates of complementary lipophilicities can be embedded. This allows for low-dose-controlled consumption and therapeutic applications. Time-resolved and in-situ grazing incidence X-ray scattering studies confirm the design of the therapeutic nano-paper and create conditions suitable for the drug storage of complementary properties. The molecular design has the potential of a locally controlled, site-specific drug release on a beyond-nanomolar scale. Generalized, the design may contribute to facile developments of personalized medicine.

The water dynamics in a nanocomposite film that consists of the electrically conductive poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and cellulose nanofibrils (CNFs) have been investigated during three cycles of exposure to low and high relative humidity (RH = 5% and 85%, respectively) using quasi-elastic neutron scattering (QENS). The obtained dynamical structure factors are transformed into the imaginary part of the dynamic susceptibility to better differentiate between the individual relaxation processes. In a humid environment, two different water species are present inside the films: fast-moving bulk water and slow-moving hydration water. During the first cycle, a large amount of hydration water enhances the polymer chain mobility, eventually leading to irreversible structural rearrangements within the film. In the subsequent cycles, we observed a release of all bulk water and portions of hydration water upon drying, along with an uptake of both water species in a humid environment. The relaxation times of hydration water diffusion as a function of momentum transfer can be described by a jump-diffusion model. The obtained jump lengths, residence times, and diffusion coefficients of hydration water suggest a change in the hydration layer upon drying: water molecules around hydrophobic groups are released from the film, while the hydrogen bonds between water and hydrophilic groups are sufficiently strong to keep these molecules inside the films, even in a dry state. The QENS results can be correlated to the structural and conductive properties. In the dry state, the low hydration water content and the absence of bulk water allow for improved wetting of the CNFs by PEDOT:PSS, which eventually increases the electrical conductivity of the films.

Cellulose Nanofibrils (CNFs), highly present in nature, can be used as building blocks for future sustainable materials, including strong and stiff filaments. A rheo-optical flow-stop technique is used to conduct experiments to characterize the CNFs by studying Brownian dynamics through the CNFs’ birefringence decay after stop. As the experiments produce large quantities of data, we reduce their dimensionality using Principal Component Analysis (PCA) and exploit the possibility of visualizing the reduced data in two ways. First, we plot the principal components (PCs) as time series, and by training LSTM networks assigned for each PC time series with the data before the flow stop, we predict the behavior after the flow stop (Bragone et al., 2024). Second, we plot the first PCs against each other to create clusters that give information about the different CNF materials and concentrations. Our approach aims at classifying the CNF materials to varying concentrations by applying unsupervised machine learning algorithms, such as k-means and Gaussian Mixture Models (GMMs). Finally, we analyze the Autocorrelation Function (ACF) and the Partial Autocorrelation Function (PACF) of the first principal component, detecting seasonality in lower concentrations.

Efficient mechanical dewatering in paper manufacturing is essential for reducing energy consumption and enhancing operational efficiency. Practical observations indicate that press felt and roll cover structures significantly influence dewatering performance. While previous studies have focused on micro-scale stress variations at the paper web-press felt interface, this study extends the analysis to the press felt-roll cover interface. Using a custom dynamic compression setup, we investigate how different groove patterns impact press felt dewatering. The results show that macro-scale stress variations play a crucial role, with controlled mechanical inhomogeneities enhancing felt permeability. Through multivariate regression analysis, an optimized groove pattern is identified that improves dewatering by approximately 7 % under highly dynamic pressing conditions. These findings offer valuable insights into optimizing press felt and roll cover interactions, providing a methodology to enhance nip dewatering efficiency. The study highlights the need to tailor groove patterns to specific press felts to ensure optimal water flow under saturated conditions. This research contributes to improving paper machine performance by maximizing water removal while reducing energy consumption, supporting both economic and environmental sustainability in the industry.

Spray deposition is a rapid and facile technique for coating surfaces on a large scale. The quality of these coatings can be improved via post‐treatment. One example is solvent annealing, a well‐known strategy to enhance the conductivity of polymeric electrode materials using organic solvents. Herein, the annealing of sprayed poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS)‐based electrodes via solvent spray deposition in a single roll‐to‐roll setup is reported. The annealing rates of three solvents, namely dimethyl sulfoxide (DMSO), isopropanol (IPA), and methanol (MeOH), depending on the spray time and sprayed volume, are evaluated and correlated with structural changes. The results show that the applied method reduces the sheet resistance ( R s ) of pure PEDOT:PSS films by 82% using DMSO and of cellulose‐based silver nanowire‐PEDOT:PSS electrodes by 50% using MeOH. This approach allows for the facile and effective combination of fabrication and quality enhancement of sprayed, conductive polymer films using only one piece of equipment. This approach makes the overall production process of organic electrodes faster and cheaper and therefore the usage of sustainable materials and fabrication methods more attractive for the industry.

In many industrial applications, nonwoven fibre networks are facilitated to operate under partly saturated conditions, allowing for filtration, liquid absorption and liquid transport. Resolving the governing liquid distribution in loaded polyamide-6 (PA6) fibre networks using X-ray computed micro-tomography is a challenge due to the similar X-ray attenuation coefficients of water and PA6 and limitations in using background subtraction techniques if the network is deformed, which will be the case if subjected to compression. In this work, we developed a method using a potassium iodide solution in water to enhance the liquid’s attenuation coefficient without modifying the water’s rheological properties. Therefore, we studied the evolving liquid distribution in loaded and partly saturated PA6 fibre networks on the microscale. Increasing the external load applied to the network, we observed an exponential decrease in air content while the liquid content was constant, increasing the overall saturation with increasing network strain. Furthermore, the microstructural properties created by the punch-needle process in the manufacturing of the network significantly influenced the out-of-plane liquid distribution. The method has been proven helpful in understanding the results of adaptions in both the fibre network design and manufacturing process, allowing for investigating the resulting liquid distribution on a microscale.

Cellulose is a natural polymer with great properties such as high optical transparency and mechanical strength, flexibility, and biodegradability. Hence, cellulose-based foils are suitable for the replacement of synthetic polymers as substrate materials in organic electronics. This article reports the fabrication of ultrathin, free-standing cellulose foils by spraying aqueous 2,2,6,6-tetramethylpiperidine-1-oxyl-nanocellulose (TEMPO) fibrils ink layer-by-layer on a hot substrate using a movable spray nozzle. The resulting foils are only 2 +/- 1 mu m in thickness with an average basis weight of 1.9 g m-2, which ranges in the same scale as the world's thinnest paper. The suitability of these ultra-thin nanocellulose foils as a sustainable substrate material for organic electronic applications is demonstrated by testing the foils resistance against organic solvents. Furthermore, silver nanowires (AgNWs) and the blend poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) are integrated into the foils, and the foils are molded into 3D paper structures in order to create conductive, paper-based building blocks for organic electronics. This article reports the fabrication of free-standing cellulose foils via layer-by-layer spray deposition. The foils are 2 mu m thin with an average basis weight of 1.9 g m-2, which ranges in the same scale as the world's thinnest paper. By integrating conductive nanoparticles and polymers, these foils become 3D, lightweight, functional components of individual shapes, suitable for organic electronics. image

An experimental method was developed to examine the dynamic compression properties of structured polyurethane composites used as press belts within a shoe press of a paper machine. The objective was to investigate the influences of the geometrical surface structure and the matrix material composition on the compression properties. Two polyurethane formulations were tested under varying specimen conditions. The results show that the dynamic compression modulus increases with the applied load rate and that temperature and water saturation reduce the influence of dynamic effects on the compression modulus. Furthermore, it was observed that modifications of the matrix material have a more significant impact on the dynamic compression modulus than adaptions in the geometrical structure. This is addressed to the relatively small variations in possible surface designs. Finally, a rate-sensitivity index is introduced to quantify the tested specimens' rate-sensitive behaviour.

The diffusion and interaction dynamics of charged nanoparticles (NPs) within charged polymer networks are crucial for understanding various biological and biomedical applications. Using a combination of coarse-grained molecular dynamics simulations and experimental diffusion studies, we investigate the effects of the NP size, relative surface charge density (ζ), and concentration on the NP permeation length and time. We propose a scaling law for the relative diffusion of NPs with respect to concentration and ζ, highlighting how these factors influence the NP movement within the network. The analyses reveal that concentration and ζ significantly affect NP permeation length and time, with ζ being critical, as critical as concentration. This finding is corroborated by controlled release experiments. Further, we categorize NP dynamics into sticking, sliding, and bouncing regimes, demonstrating how variations in ζ, concentration, and NP size control these behaviors. Through normalized attachment time (NAT) analyses, we elucidate the roles of electrostatic interactions, steric hindrance, and hydrodynamic forces in governing NP dynamics. These insights provide guidance for optimizing NP design in targeted drug delivery and advanced material applications, enhancing our understanding of NP behavior in complex environments.

The colloidal layer formation on porous materials is a crucial step for printing and applying functional coatings, which can be used to fabricate anticounterfeiting paper. The deposition of colloidal layers and subsequent thermal treatment allows for modifying the hydrophilicity of the surface of a material. In the present work, wood-based colloidal inks are applied by spray deposition on spray-deposited porous cellulose nanofibrils (CNF) films. The surface modification by thermal annealing of the fabricated colloid-cellulose hybrid thin films is investigated in terms of layering and hydrophobicity. The polymer colloids in the inks are core-shell nanoparticles with different sizes and glass transition temperatures (T-g), thus enabling different and low thermal treatment temperatures. The ratio between the core polymers, poly(sobrerol methacrylate) (PSobMA), and poly(-butyl methacrylate) (PBMA) determines the T-g and hence allows for tailoring of the T-g. The layer formation of the colloidal inks on the porous CNF layer depends on the imbibition properties of the CNF layer which is determined by their morphology. The water adhesion of the CNF layer decreases due to the deposition of the colloids and thermal treatment except for the colloids with a size smaller than the void size of the porous CNF film. In this case, the colloids are imbibed into the CNF layer when T-g of the colloids is reached and the polymer chains transit in a mobile phase. Tailored aggregate and nanoscale-embedded hybrid structures are achieved depending on the colloid properties. The imbibition of these colloids into the porous CNF films is verified with grazing incidence small-angle X-ray scattering. This study shows a route for tuning the nanoscale structure and macroscopic physicochemical properties useful for anticounterfeiting paper.

As the quest for more sustainable and environmentally friendly materials has increased in the last decades, cellulose nanofibrils (CNFs), abundant in nature, have proven their capabilities as building blocks to create strong and stiff filaments. Experiments have been conducted to characterize CNFs with a rheo-optical flow-stop technique to study the Brownian dynamics through the CNFs’ birefringence decay after stop. This paper aims to predict the initial relaxation of birefringence using Principal Component Analysis (PCA) and Long Short-Term Memory (LSTM) networks. By reducing the dimensionality of the data frame features, we can plot the principal components (PCs) that retain most of the information and treat them as time series. We employ LSTM by training with the data before the flow stops and predicting the behavior afterward. Consequently, we reconstruct the data frames from the obtained predictions and compare them to the original data.

The advent of diffraction-limited storage rings (DLSRs) has boosted the brilliance or coherent flux by one to two orders of magnitude with respect to the previous generation. One consequence of this brilliance enhancement is an increase in the flux density or number of photons per unit of area and time, which opens new possibilities for the spatiotemporal resolution of X-ray imaging techniques. This paper studies the time-resolved microscopy capabilities of such facilities by benchmarking the ForMAX beamline at the MAX IV storage ring. It is demonstrated that this enhanced flux density using a single harmonic of the source allows micrometre-resolution time-resolved imaging at 2000 tomograms per second and 1.1 MHz 2D acquisition rates using the full dynamic range of the detector system.

In the context of global climate change, the demand for new functional materials that are sustainable and environmentally friendly is rapidly increasing. Cellulose and lignin are the two most abundant raw materials in nature, and are ideal components for functional materials. The hydrophilic interface and easy film-forming properties of cellulose nanofibrils make them excellent candidates for natural biopolymer templates and network structures. Lignin is a natural UV-shielding material, as it contains a large number of phenolic groups. In this work, we have applied two routes for spray deposition of hybrid films with different laminar structures using surface-charged cellulose nanofibrils and water-based colloidal lignin particles. As the first route, we prepare stacked colloidal lignin particles and cellulose nanofibrils hybrid film through a layer-by-layer deposition. As the second route, we spray-deposite premixed colloidal lignin particles and cellulose nanofibrils dispersion to prepare a mixed hybrid film. We find that cellulose nanofibrils act as a directing agent to dominate the arrangement of the colloidal lignin particles in a mixed system. Additionally, cellulose nanofibrils eliminate the agglomerations and thus increase the visible light transparency while retaining the UV shielding ability. Our research on these colloidal lignin and cellulose nanofibril hybrid films provides a fundamental understanding of using colloidal lignin nanoparticles as functional material on porous cellulose-based materials, for example on fabrics.

We demonstrate a framework of interpreting data from x-ray photon correlation spectroscopy experiments with the aid of numerical simulations to describe nanoscale dynamics in soft matter. This is exemplified with the transport of passive tracer gold nanoparticles in networks of charge-stabilized cellulose nanofibers. The main structure of dynamic modes in reciprocal space could be replicated with a simulated system of confined Brownian motion, a digital twin, allowing for a direct measurement of important effective material properties describing the local environment of the tracers.