We present the design and construction of a custom neutron-transparent sample environment for in situ moisture-dependent neutron dark-field imaging (NDFI) experiments for the imaging facilities at the Paul Scherrer Institute (PSI), Villigen, Switzerland. This simple setup, combined with a moisture generator, features a continuous flow system to ensure a constant homogeneous flow of humid air to manipulate the sample's moisture conditions at room temperature. To facilitate neutron dark-field imaging measurements, the chamber has a slim design to maximize the sample-detector distance scanning range. The chamber can maintain static or dynamic relative humidity conditions, allowing for humidity cycles. Beyond moisture-dependent studies, the system's versatility allows its utilization in any type of gas stream-dependent study. This technical note details the engineering considerations, construction process, and validation of this sample environment.

The complexity of condensed matter arises from emergent behaviors that cannot be understood by investigating individual constituents in isolation. While traditional condensed-matter approaches, developed primarily for ideal crystalline solids, have provided important insights into symmetry, order, and electronic structure, they fall short in describing the rich, multiscale organization of hierarchical and soft materials. These systems exhibit structural correlations across multiple length and time scales, often governed by nonlinear interactions that span from molecular to macroscopic domains. This review explores how the convergence of emerging experimental and computational strategies is redefining our ability to characterize and model such systems. We outline how multimodal techniques, combining scattering, imaging, and spectroscopy, can map structural order and dynamics across scales, with methods such as small-angle scattering tensor tomography, dark-field imaging, and ultrafast spectroscopies, providing unprecedented spatiotemporal resolution. On the computational front, machine learning approaches such as graph neural networks, neural operators, and physics-informed models, offer powerful tools to connect disparate scales and uncover hidden correlations in high-dimensional data. These advancements have the potential to close the gap between structure and function in complex materials, thereby addressing one of the Grand Challenges of contemporary material science: understanding and engineering multiscale architectures whose emergent properties underpin the behavior of next-generation functional materials, biological systems, and adaptive technologies.

There has been a recent surge of interest in biobased foams for applications ranging from building sustainability (insulation) to biomedicine, pharmaceutics, and electronics (scaffolds), with nanocellulose-based foams being particularly promising due to their porous and low-density structure. This study compares the production energy, structure, and properties of foams made from TEMPO-oxidized lignocellulose nanofibers (FTOLCNF) derived from unbleached wood pulp, and TEMPO-oxidized cellulose nanofibers (FTOCNF) from bleached cellulose pulp. Additionally, the incorporation of tannic acid (TA) as a biobased additive is explored for its ability to enhance the mechanical strength of FTOLCNF, contributing to improved performance. This builds upon the inherent advantages of FTOLCNF, which not only demonstrate superior structural integrity and load-bearing capacity (specific Young’s modulus of 37.4 J g–1, compared to 16.4 J g–1 for TOCNF) but also exhibit a higher yield during production due to the minimal processing required for unbleached pulp. Furthermore, FTOLCNF production requires about 18% less cumulative energy than FTOCNF (27 vs 33 MJ kg–1), largely owing to the energy-efficient preparation of TOLCNF from unbleached wood pulp. FTOLCNF also have a significantly lower cumulative energy demand (CED) compared to fossil-based alternatives like expanded polystyrene (EPS) and polyurethane (PU), highlighting their reduced environmental impact. Despite their lightweight nature, FTOLCNF exhibit competitive compressive strength, making them viable candidates for eco-friendly applications across various industries. Overall, this study demonstrates that FTOLCNF are an attractive alternative to other bio- and fossil-based foams, offering a balance of energy efficiency, higher yield, mechanical performance, and sustainability.

Nanocellulose is a promising alternative to fossil-derived materials, but its development is hindered by a limited understanding of cellulose–water interactions. Herein, quasielastic neutron scattering (QENS) is used to investigate how hydration and temperature affect the localized rotations in cellulose nanocrystals (CNC) and the diffusion of mobile water. QENS reveals that the C6 hydrogens and the C6 OH in the surface regions of CNC exhibit an isotropic rotation. The extracted mean square displacement shows that hydration enhances the overall hydrogen mobility in the cellulose chains. The mobile water diffusion at 270 K is unaffected by cellulose and consistent with diffusion of supercooled bulk water. At 310 K, the diffusion slows compared to bulk water, consistent with water diffusing on the CNC surface. Decoupling of the translational and rotational motion provides insight into the local cellulose–water motions. The localized motions of the nondiffusing water are found to be coupled with cellulose at 310 K, indicating a more complex dynamics at higher temperature. These findings provide new insights into how hydration modulates hydrogen mobility in cellulose, highlighting the interplay between water diffusion and molecular motion.

Superinsulating nanofibrillar cellulose foams have the potential to replace fossil-based insulating materials, but the development is hampered by the moisture-dependent heat transport and the lack of direct measurements of phonon transport. Here, inelastic neutron scattering is used together with wide angle X-ray scattering (WAXS) and small angle neutron scattering to relate the moisture-dependent structural modifications to the vibrational dynamics and phonon transport and scattering of cellulose nanofibrils from wood and tunicate, and wood cellulose nanocrystals (W-CNC). The moisture interacted primarily with the disordered regions in nanocellulose, and WAXS showed that the crystallinity and coherence length increased as the moisture content increased. The phonon population derived from directional-dependent phonon density of states (GDOS) increased along the cellulose chains in W-CNC between 5 and 8 wt% D₂O, while the phonon population perpendicular to the chains remained relatively unaffected, suggesting that the effect of increased crystallinity and coherence length on phonon transport is compensated by the moisture-induced swelling of the foam walls. Frequency scaling in the low-energy GDOS showed that materials based on hygroscopic and semicrystalline nanocellulose falls in between the predicted behavior for solids and liquids. Phonon-engineering of hygroscopic biopolymer-based insulation materials is promoted by the insights on the moisture-dependent phonon transport.

We have produced foams from cellulose nanofibrils from upcycled cotton (upCNF) and wood (wCNF) through unidirectional (UIT) and multidirectional ice-templating (MIT) and investigated the structural humidity response through in-situ WAXS, SAXS, and micro tomography (μCT) between 10 and 95 % relative humidity (RH). The upCNF and wCNF WAXS patterns displayed a shape- and position shift as the RH was increased, with a compression in the (200) direction and an elongation in the (004) direction. The average separation distance extracted from the 1D SAXS patterns revealed no significant change for the upCNF foams regardless of RH and processing route, while a significant increase was observed for the wCNF foams. The μCT measurements of the upCNF foams showed a slight shift in macropore distribution towards larger pores between 50 and 80 % RH which can be attributed to the weakening and partial disintegration of the pore wall as more moisture is introduced. The humidity-induced structural alterations of the upCNF foam were significantly lower compared to the wCNF foams, confirming our claim of upCNF being more moisture resistant than wCNF foams.

Understanding ion diffusion mechanisms in layered materials is critical for advancing next-generation battery technologies. Using the well-characterized Na_xCoO₂ (NCO) system as a model platform, we investigated the temperature-dependent diffusion properties across a broad compositional range (x = 0.33 − 0.89) using muon spin relaxation (μ⁺SR). Unexpected low-temperature internal magnetic field fluctuations were observed, systematically varying with Na content and appearing well before the onset of long-range diffusion. These fluctuations are attributed to phonon-assisted local Na motion, as suggested by a systematic increase in A with x, concurrent with a decreasing activation energy. The diffusion coefficient was calculated based on the crystal structure using a tailored diffusion model accounting for two inequivalent Na sites, yielding values consistent with those found in other layered battery materials. This work highlights the crucial role of phonon-coupled diffusion mechanisms in enabling ion transport at the microscopic scale, providing new insights into ion dynamics in layered solid-state conductors and their relevance to sodium-ion battery technology.

The assertion of intrinsic material properties based on measured experimental data is being challenged by emerging sample synthesis protocols, which opens new avenues for discovering novel functionalities. In this study, we revisit one of the most widely studied strongly correlated materials of the early 2000s, Na𝑥⁢CoO2 (NCO). Leveraging the sensitivity of muon spin rotation and relaxation (𝜇+⁢SR) measurements, we discern significant differences between NCO samples synthesized via conventional solid-state reaction (SSR) and our electrochemical reaction (ECR) approach. Contrary to SSR-synthesized Na0.7⁢CoO2, which exhibits a nonmagnetic ground state, our ECR-derived sample showcases an antiferromagnetic (AF) order from 𝑥≥0.7, challenging established phase boundaries. We attribute the observed magnetic phenomena in ECR-NCO to long-range order of Na-ions and/or vacancies, as well as the inherent flexibility of the crystal framework. Our study holds implications for tailoring and optimization of next-generation devices based on layered materials.

Biopolymer-based functional materials are essential for reducing the carbon footprint and providing high-quality lightweight materials suitable for packaging and thermal insulation. Here, cellulose nanocrystals (CNCs) were efficiently upcycled from post-consumer cotton clothing by TEMPO-mediated oxidation and HCl hydrolysis with a yield of 62% and combined with wood cellulose nanofibrils (CNFs) to produce anisotropic foams by unidirectional freeze-casting followed by freeze drying (FD) or supercritical-drying (SCD). Unidirectional freeze-casting resulted in foams with aligned macropores irrespective of the drying method, but the particle packing in the foam wall was significantly affected by how the ice was removed. The FD foams showed tightly packed and aligned CNC and CNF particles while the SCD foams displayed a more network-like structure in the foam walls. The SCD compared to FD foams had more pores smaller than 300 nm and higher specific surface area but they were more susceptible to moisture-induced shrinkage, especially at relative humidities (RH) > 50%. The FD and SCD foams displayed low radial thermal conductivity, and the FD foams displayed a higher mechanical strength and stiffness in compression in the direction of the aligned particles. Better understanding how drying influences the structural, thermal, mechanical and moisture-related properties of foams based on repurposed cotton is important for the development of sustainable nanostructured materials for various applications.

Strongly correlated electron materials are often characterized by competition and interplay of multiple quantum states. For example, in high-temperature cuprate superconductors unconventional superconductivity, spin- and charge-density wave orders coexist. A key question is whether competing states coexist on the atomic scale or if they segregate into distinct regions. Using X-ray diffraction, we investigate the competition between charge order and superconductivity in the archetypal cuprate La_2−xBa_xCuO₄, around x = 1/8-doping, where uniaxial stress restores optimal 3D superconductivity at σ_3D ≈ 0.06 GPa. We find that the charge order peaks and the correlation length along the stripe are strongly reduced up to σ_3D. Upon the increase of stress beyond this point, no further changes were observed. Simultaneously, the charge order onset temperature only shows a modest decrease. Our findings suggest that optimal 3D superconductivity is not linked to the absence of charge stripes but instead requires their arrangement into smaller regions. Our results provide insight into the length scales over which the interplay between superconductivity and charge order takes place.