Μm Length Scale Research Articles

Optical Properties of H-Bonded Heterotriangulene Supramolecular Polymers: Charge-Transfer Excitations Matter.

H-bonded N-heterotriangulene (NHT) supramolecular polymers offer a nice playground to explore the nature and dynamics of electronic excitations in low-dimensional organic nanostructures. Here, we report on a comprehensive molecular modeling of the excited-state electronic structure and optical properties of model NHT stacks, highlighting the important role of intermolecular charge-transfer (CT) excitations in shaping their optical absorption and emission lineshapes. Most importantly, we show that the coupling between the local and CT excitations, modulated by the electric fields induced by the presence of polar amide groups forming H-bonded arrays along the stacks, significantly increases the resulting hybrid exciton bandwidth. We discuss these findings in the context of the efficient transport of singlet excitons over the μm length scale reported experimentally on individual self-assembled nanofibers with molecular-scale diameter.

Viscoelastic properties of the equine hoof wall

The equine hoof wall has outstanding impact resistance, which enables high-velocity gallop over hard terrain with minimum damage. To better understand its viscoelastic behavior, complex moduli were determined using two complementary techniques: conventional (∼5 mm length scale) and nano (∼1 µm length scale) dynamic mechanical analysis (DMA). The evolution of their magnitudes was measured for two hydration conditions: fully hydrated and ambient. The storage modulus of the ambient hoof wall was approximately 400 MPa in macro-scale experiments, decreasing to ∼250 MPa with hydration. In contrast, the loss tangent decreased for both hydrated (∼0.1–0.07) and ambient (∼0.04–0.01) conditions, over the frequency range of 1–10 Hz. Nano-DMA indentation tests conducted up to 200 Hz showed little frequency dependence beyond 10 Hz. The loss tangent of tubular regions showed more hydration sensitivity than in intertubular regions, but no significant difference in storage modulus was observed. Loss tangent and effective stiffness were higher in indentations for both hydration levels. This behavior is attributed to the hoof wall's hierarchical structure, which has porosity, functionally graded aspects, and material interfaces that are not captured at the scale of indentation. The hoof wall's viscoelasticity characterized in this work has implications for the design of bioinspired impact-resistant materials and structures. Statement of significanceThe outer wall of horse hooves evolved to withstand heavy impacts during gallop. While previous studies have measured the properties of the hoof wall in slowly changing conditions, we wanted to quantify its behavior using experiments that replicate the quickly changing forces of impact. Since the hoof wall's structure is complex and contributes to its overall performance, smaller scale experiments were also performed. The behavior of the hoof wall was within the range of other biological materials and polymers. When hydrated, it becomes softer and can dissipate more energy. This work improves our understanding of the hoof's function and allows for more accurate simulations that can account for different impact speeds.

Rapid subsurface analysis of frequency-domain thermoreflectance images with K-means clustering

K-means clustering analysis is applied to frequency-domain thermoreflectance (FDTR) hyperspectral image data to rapidly screen the spatial distribution of thermophysical properties at material interfaces. Performing FDTR while raster scanning a sample consisting of 8.6 μm of doped-silicon (Si) bonded to a doped-Si substrate identifies spatial variation in the subsurface bond quality. Routine thermal analysis at select pixels quantifies this variation in bond quality and allows assignment of bonded, partially bonded, and unbonded regions. Performing this same routine thermal analysis across the entire map, however, becomes too computationally demanding for rapid screening of bond quality. To address this, K-means clustering was used to reduce the dimensionality of the dataset from more than 20 000 pixel spectra to just K=3 component spectra. The three component spectra were then used to express every pixel in the image through a least-squares minimized linear combination providing continuous interpolation between the components across spatially varying features, e.g., bonded to unbonded transition regions. Fitting the component spectra to the thermal model, thermal properties for each K cluster are extracted and then distributed according to the weighting established by the regressed linear combination. Thermophysical property maps are then constructed and capture significant variation in bond quality over 25 μm length scales. The use of K-means clustering to achieve these thermal property maps results in a 74-fold speed improvement over explicit fitting of every pixel.

Controlling the roll-to-helix transformation in electron-beam-patterned gel-based micro-ribbons.

Helix formation has been of ongoing interest because of its role in both natural and synthetic materials systems. It has been extensively studied in gel-based ribbons where swelling anisotropies drive out-of-plane bending. In contrast to approaches based on photolithography or mechanical bilayer construction, we use electron-beam patterning to create microscale ribbons at ∼1-100 μm length scales in pure homopolymer precursor films of poly(acrylic acid) (PAA). The radiation chemistry creates a ribbon comprising a crosslinked hydrophobic top layer and a hydrophilic gel bottom layer with a continuous through-thickness variation in between. The classic roll-to-helix transition occurs as the ribbon aspect ratio increases. Notably, we see examples of single-loop rolls, multi-loop rolls, minimal-pitch helices, plus a transition structure comprising both helical and roll-like features. Finite-element modelling recapitulates key aspects of these conformations. Increasing the pH from below to above the PAA pKa increases the out-of-plane bending to the extent that the ribbons plastically deform and nonminimal-pitch helices form across a wide range of aspect ratios and irradiation conditions. The nonminimal pitch is caused by an in-plane anisotropy associated with the plastic deformation. We mimic this anisotropy by patterning ribbons comprising micro-tiles separated by gaps which receive electron exposure due to proximity effects. We observe a transition from roll to helix to tube with increasing gap angle. The chirality is completely determined by the gap orientation (±θ). However, in contrast to established approaches to generate in-plane anisotropies based on mechanical properties, finite-element modelling indicates that anisotropic through-thickness swelling of the gap material plays a dominant role in helix formation and suggests that this micro-composite ribbon behaves like a rigid origami metamaterial where deformation at the creases (the gaps) between structural elements controls the shape shifting.

Targeted micro-heterogeneity in bioinks allows for 3D printing of complex constructs with improved resolution and cell viability.

Three-dimensional bioprinting is an evolving versatile technique for biomedical applications. Ideal bioinks have complex micro-environment that mimic human tissue, allow for good printing quality and provide high cell viability after printing. Here we present two strategies for enhancing gelatin-based bioinks heterogeneity on a 1-100µm length scale resulting in superior printing quality and high cell viability. A thorough spatial and micro-mechanical characterization of swollen hydrogel heterogeneity was done using multiple particle tracking microrheology. When poly(vinyl alcohol) is added to homogeneous gelatin gels, viscous inclusions are formed due to micro-phase separation. This phenomenon leads to pronounced slip and superior printing quality of complex 3D constructs as well as high human hepatocellular carcinoma (HepG2) and normal human dermal fibroblast (NHDF) cell viability due to reduced shear damage during extrusion. Similar printability and cell viability results are obtained with gelatin/nanoclay composites. The formation of polymer/nanoclay clusters reduces the critical stress of gel fracture, which facilitates extrusion, thus enhancing printing quality and cell viability. Targeted introduction of micro-heterogeneities in bioinks through micro-phase separation is an effective technique for high resolution 3D printing of complex constructs with high cell viability. The size of the heterogeneities, however, has to be substantially smaller than the desired feature size in order to achieve good printing quality.

4D printing of Metal-Reinforced double network granular hydrogels

Recent developments in soft actuation demand for resilient, responsive materials with locally varying compositions that are sufficiently stiff to exhibit significant actuation forces. Hydrogels are inherently responsive to certain stimuli. Yet, they typically suffer from a stiffness-toughness compromise such that those that are soft and show adequate flexibility display limited actuation forces. This compromise can be partially addressed if hydrogels are formulated as double networks. However, their involved processing prevents controlled variations in the local composition. The composition of hydrogels can be varied down to the 100 µm length scale through 3D printing. A wide range of hydrogels can be 3D printed if formulated as microparticles. Yet, the resulting granular hydrogels are soft. They can be reinforced with a percolating hydrogel network, resulting in double network granular hydrogels (DNGHs) that, however, are rather brittle. Here, we introduce 3D printable metal-reinforced DNGHs (mrDNGHs) that combine three seemingly contradictory traits: stiffness, toughness, and processability. Our mrDNGHs can bear loads up to 3 MPa while displaying a fracture energy up to 12 MJ·m−3, a value exceeding that of any of the previously 3D printed hydrogels at least 20-fold. We leverage the different degrees of swelling of the mrDNGHs to 3D print shape morphing structures.

Real‐time Observation of Macroscopic Helical Morphologies under Optical Microscope: A Curious Case of π–π Stacking Driven Molecular Self‐assembly of an Organic Gelator Devoid of Hydrogen Bonding

AbstractSupramolecular assemblies such as tubules/helix/double helix/helical tape etc. are usually submicron objects preventing direct observation under optical microscope. Chiral‐pure form of these assemblies is important for potential applications. Herein, we report a rare phenomenon wherein a DMSO gel of a simple terpyridine derivative [(4‐CNPhe)4PyTerp] produced macroscopic helical morphologies (μm length scale) which could be observed under optical microscope, formation of which could be monitored by optical videography, stable enough to withstand acidic vapour, robust enough to display reversible gel↔sol in response to acidic and ammonia vapour and sturdy enough to be maneuvered with a needle. These properties appeared to be unique to the title compound as the other related derivatives failed to display such assembly structures. SXRD and MD simulation studies suggested that weak interactions (π‐π stacking) played a crucial role in the self‐assembly process.

Real-time Observation of Macroscopic Helical Morphologies under Optical Microscope: A Curious Case of π-π Stacking Driven Molecular Self-assembly of an Organic Gelator Devoid of Hydrogen Bonding.

Supramolecular assemblies such as tubules/helix/double helix/helical tape etc. are usually submicron objects preventing direct observation under optical microscope. Chiral-pure form of these assemblies is important for potential applications. Herein, we report a rare phenomenon wherein a DMSO gel of a simple terpyridine derivative [(4-CNPhe)4PyTerp] produced macroscopic helical morphologies (μm length scale) which could be observed under optical microscope, formation of which could be monitored by optical videography, stable enough to withstand acidic vapour, robust enough to display reversible gel↔sol in response to acidic and ammonia vapour and sturdy enough to be maneuvered with a needle. These properties appeared to be unique to the title compound as the other related derivatives failed to display such assembly structures. SXRD and MD simulation studies suggested that weak interactions (π-π stacking) played a crucial role in the self-assembly process.

Modeling and mechanical perturbations reveal how spatially regulated anchorage gives rise to spatially distinct mechanics across the mammalian spindle.

During cell division, the spindle generates force to move chromosomes. In mammals, microtubule bundles called kinetochore-fibers (k-fibers) attach to and segregate chromosomes. To do so, k-fibers must be robustly anchored to the dynamic spindle. We previously developed microneedle manipulation to mechanically challenge k-fiber anchorage, and observed spatially distinct response features revealing the presence of heterogeneous anchorage (Suresh et al., 2020). How anchorage is precisely spatially regulated, and what forces are necessary and sufficient to recapitulate the k-fiber's response to force remain unclear. Here, we develop a coarse-grained k-fiber model and combine with manipulation experiments to infer underlying anchorage using shape analysis. By systematically testing different anchorage schemes, we find that forces solely at k-fiber ends are sufficient to recapitulate unmanipulated k-fiber shapes, but not manipulated ones for which lateral anchorage over a 3 μm length scale near chromosomes is also essential. Such anchorage robustly preserves k-fiber orientation near chromosomes while allowing pivoting around poles. Anchorage over a shorter length scale cannot robustly restrict pivoting near chromosomes, while anchorage throughout the spindle obstructs pivoting at poles. Together, this work reveals how spatially regulated anchorage gives rise to spatially distinct mechanics in the mammalian spindle, which we propose are key for function.

Chemorepellent-Loaded Nanocarriers Promote Localized Interference of Escherichia coli Transport to Inhibit Biofilm Formation.

To mitigate antimicrobial resistance, we developed polymeric nanocarrier delivery of the chemorepellent signaling agent, nickel, to interfere with Escherichia coli transport to a surface, an incipient biofilm formation stage. The dynamics of nickel nanocarrier (Ni NC) chemorepellent release and induced chemorepellent response required to effectively modulate bacterial transport for biofilm prevention were characterized in this work. Ni NCs were fabricated with the established Flash NanoPrecipitation method. NC size was characterized with dynamic light scattering. Measured with a zincon monosodium salt colorimetric assay, NC nickel release was pH-dependent, with 62.5% of total encapsulated nickel released at pH 7 within 0-15 min, competitive with rapid E. coli transport to the surface. Confocal laser scanning microscopy of E. coli (GFP-expressing) biofilm growth dynamics on fluorescently labeled Ni NC coated glass coupled with a theoretical dynamical criterion probed the biofilm prevention outcomes of NC design. The Ni NC coating significantly reduced E. coli attachment compared to a soluble nickel coating and reduced E. coli biomass area by 61% compared to uncoated glass. A chemical-in-plug assay revealed Ni NCs induced a chemorepellent response in E. coli. A characteristic E. coli chemorepellent response was observed away from the Ni NC coated glass over 10 μm length scales effective to prevent incipient biofilm surface attachment. The dynamical criterion provided semiquantitative analysis of NC mechanisms to control biofilm and informed optimal chemorepellent release profiles to improve NC biofilm inhibition. This work is fundamental for dynamical informed design of biofilm-inhibiting chemorepellent-loaded NCs promising to mitigate the development of resistance and interfere with the transport of specific pathogens.

Long-range interconnected nanoporous Co/Ni/C composites as bifunctional electrocatalysts for long-life rechargeable zinc-air batteries

Zinc–air batteries are considered to be a promising candidate for use as a sustainable power source, due to their higher energy density and more economical features. However, it is necessary to design efficient and durable electrocatalysts, especially the durability, for bifunctional oxygen reduction (ORR) and oxygen evolution reactions (OER). Therefore, it is imperative to developing reliable zinc-air batteries with long-lasting cycle lifetime. Herein, we report long-range interconnected nanoporous Co/Ni/C composites in µm-length scale as highly active and stable bifunctional electrocatalysts for long-life rechargeable zinc-air batteries. The composite catalysts consist of N and S co-doped hollow carbon and carbon-encapsulated CoNi alloy nanoparticles, which serve as catalytically active sites for the ORR/OER. Meanwhile, the long-range interconnected nanoporous carbon structure in µm-length scale favors fast ion and electron transfer during the reactions, and can prevent the catalyst deterioration against nanoparticles collapse and agglomerate into large ones during the long-term battery operation. As a result, compared to the commercial precious metal-based catalysts, the Co/Ni/C composite catalysts exhibit a significantly improved stability towards the ORR/OER with small activity decay after 100 h/10 h of operation under chronoamperometric polarization. Especially, the resulting zinc-air battery demonstrates remarkable cycling stability exceeding 620 h and 430 h at 5 and 10 mA cm−2, respective.

Transient Anomalous Diffusion MRI in Excised Mouse Spinal Cord: Comparison Among Different Diffusion Metrics and Validation With Histology.

Neural tissue is a hierarchical multiscale system with intracellular and extracellular diffusion compartments at different length scales. The normal diffusion of bulk water in tissues is not able to detect the specific features of a complex system, providing nonlocal, diffusion measurement averaged on a 10-20 μm length scale. Being able to probe tissues with sub-micrometric diffusion length and quantify new local parameters, transient anomalous diffusion (tAD) would dramatically increase the diagnostic potential of diffusion MRI (DMRI) in detecting collective and sub-micro architectural changes of human tissues due to pathological damage. In DMRI, the use of tAD parameters quantified using specific DMRI acquisition protocols and their interpretation has often aroused skepticism. Although the derived formulas may accurately fit experimental diffusion-weighted data, the relationships between the postulated dynamical feature and the underlying geometrical structure remains elusive, or at most only suggestive. This work aimed to elucidate and validate the image contrast and information that can be obtained using the tAD model in white matter (WM) through a direct comparison between different diffusion metrics and histology. Towards this goal, we compared tAD metrics extracted from pure subdiffusion (α-imaging) and super-pseudodiffusion (γ-imaging) in excised mouse spinal cord WM, together with T2 and T2* relaxometry, conventional (normal diffusion-based) diffusion tensor imaging (DTI) and q-space imaging (QSI), with morphologic measures obtained by optical microscopy, to determine which structural and topological characteristics of myelinated axons influenced tAD contrast. Axon diameter (AxDiam), the standard deviation of diameters (SDax.diam), axonal density (AxDens) and effective local density (ELD) were extracted from optical images in several WM tracts. Among all the diffusion parameters obtained at 9.4 T, γ-metrics confirmed a strong dependence on magnetic in-homogeneities quantified by R2* = 1/T2* and showed the strongest associations with AxDiam and ELD. On the other hand, α-metrics showed strong associations with SDax.diam and was significantly related to AxDens, suggesting its ability to quantify local heterogeneity degree in neural tissue. These results elucidate the biophysical mechanism underpinning tAD parameters and show the clinical potential of tAD-imaging, considering that both physiologic and pathologic neurodegeneration translate into alterations of WM morphometry and topology.

Influence of pia-arachnoid complex on the indentation response of porcine brain at different length scales

Brain tissues are surrounded by two tightly adhering thin membranes known as the pia-arachnoid complex (PAC), which is pivotal in regulating brain mechanical response upon mechanical impact. Despite the crucial role of PAC as a structural damper protecting the brain, its mechanical contribution has received minimal attention. In this work, the mechanical contribution of PAC on brain tissues against mechanical loading is characterized by using a custom-built indentation apparatus. The indentation responses of the isolated and PAC-overlaid brains are quantitatively compared at different length scales and strain rates. Results show that PAC substantially affects the indentation response of brain tissues at micro- and macro-scales and provides better protection against mechanical impact at a relatively small (μm) length scale. The modulus of the PAC-overlaid brain shows a threefold stiffening at the microscale compared with that of the isolated brain (with instantaneous shear modulus distribution means of 0.85 ± 0.14 kPa versus 2.64 ± 0.43 kPa at the strain rate of 0.64 s−1 and 1.40 ± 0.31 kPa versus 4.02 ± 0.51 at 1.27 s−1). These findings indicate that PAC seriously affects the mechanical response of brain tissues, especially at the microscale, and may have important implications for the studies of brain injury.

Hierarchical Self-Assembly of Metal-Ion-Modulated Chitosan Tubules.

Soft materials such as gels or biological tissues can develop via self-assembly under chemo-mechanical forces. Here, we report the instantaneous formation of soft tubular structures with a two-level hierarchy by injecting a mixture of inorganic salt and chitosan (CS) solution from below into a reactor filled with alkaline solution. Folding and wrinkling instabilities occur on the originally smooth surface controlled by the salt composition and concentration. Liesegang-like precipitation patterns develop on the outer surface on a μm length scale in the presence of calcium chloride, while the precipitate particles are distributed evenly in the bulk as corroborated by X-ray μ-CT. On the other hand, barium hydroxide precipitates out only in the thin outer layer of the CS tubule when barium chloride is introduced into the CS solution. Independent of the concentration of the weakly interacting salt, an electric potential gradient across the CS membrane develops, which vanishes when the pH difference between the two sides of the membrane diminishes.

On the significance of interfacial chemistry on the strength of fly ash-cement composites

Despite the large number of studies on supplementary cementitious materials, the underlying physicochemical interfacial processes that govern their strength remain obscure. To address this knowledge gap, this paper strives to establish a relation between the chemical composition of fly ash (FA) at the molecular level and the macroscopic compressive strength in cement hydrates-FA composites. We develop a multiscale modeling framework that links the fundamental physicochemical attributes of calcium silicate hydrate (C-S-H)-FA interfaces across molecular (~1 nm), mesoscopic (~100 nm), and microscopic (~10 μm) length scales. We observe that FA's chemical composition affects the interfacial properties across all scales. FAs with higher network-modifier cation concentration show stronger molecular and mesoscale interfacial properties and statistically significant higher macroscopic compressive strength. This is particularly interesting for Class F FA, where early-age reactivity is negligible.

Nondestructive characterization of nanoporous alumina films using terahertz scattering imaging

Ordered nanoporous (NP) alumina (Al 2 O 3 ) films were grown on Al substrates through a two-step electrochemical anodization process. The morphology as well as the roughness are characterized by terahertz (THz) reflectometry and scattering imaging. In particular, we show that before the second anodization, irregular surface morphology of the NP Al 2 O 3 films leads to significant THz scattering, whereas the far more homogeneous films following the second anodization show far less scattering. The regularity of the surface morphology is not readily ascertained using visible-light optical microscopy. The THz results are corroborated by field-emission scanning electron microscopy (SEM) and atomic-force microscopy (AFM), both of which are time-consuming, not easy to operate, and can only provide the local characterization of NP Al 2 O 3 films on Al substrate. THz-based techniques allow for the nondestructive characterization of the surface morphology of the entire NP Al 2 O 3 films on the 10–100 μm length scale important for a range of applications while providing information over macroscopic scan areas, and obviate the need for sample preparation required by other common surface-morphology characterization techniques. • Terahertz scattering imaging is applied to characterize the homogeneity of nanoporous alumina films after anodization. • Irregular surface morphology of nanoporous alumina films observed in terahertz images is corroborated by FE-SEM and AFM. • The stratigraphy and thickness of nanoporous alumina films are obtained nondestructively based on terahertz images. • Terahertz imaging may provide a reliable nondestructive and contactless modality to evaluate the quality of nanoporous films.

Millimeter-Wave Bat for Mapping and Quantifying Micromotions in Full Field of View.

Echolocating bats possess remarkable capability of multitarget spatial localization and micromotion sensing in a full field of view (FFOV) even in cluttered environments. Artificial technologies with such capability are highly desirable for various fields. However, current techniques such as visual sensing and laser scanning suffer from numerous fundamental problems. Here, we develop a bioinspired concept of millimeter-wave (mmWave) full-field micromotion sensing, creating a unique mmWave Bat (“mmWBat”), which can map and quantify tiny motions spanning macroscopic to μm length scales of full-field targets simultaneously and accurately. In mmWBat, we show that the micromotions can be measured via the interferometric phase evolution tracking from range-angle joint dimension, integrating with full-field localization and tricky clutter elimination. With our approach, we demonstrate the capacity to solve challenges in three disparate applications: multiperson vital sign monitoring, full-field mechanical vibration measurement, and multiple sound source localization and reconstruction (radiofrequency microphone). Our work could potentially revolutionize full-field micromotion monitoring in a wide spectrum of applications, while may inspiring novel biomimetic wireless sensing systems.

On improving the accuracy of self-calibrated stereo digital image correlation system

Stereo digital image correlation (stereo DIC), a full-field deformation measurement technique, is increasingly being used to resolve strains at µm-length scale by using microscope-like imaging systems. Self calibration of these imaging systems is more cost-effective and convenient than the conventional target-based calibration. Though the use of self-calibrated stereo DIC systems has already been reported, less attention has been paid to improving the accuracy of these systems. In the present work, we improve the accuracy of a self-calibrated stereo DIC system, which is composed of two full-frame DSLR cameras coupled to macro lenses and is used for testing ASTM E8M sub-sized flat dog-bone specimens. First, we collect the images of two of the speckled test specimens that subtend an angle of 12° between them using an f/25 aperture. Our image-collection strategy leads to a convergent imaging configuration with viewpoints that range from −45° to 45° across two perpendicular directions. Next, we process the collected images in a commercial photogrammetric calibration software by using more than nine image points for computing each object point. We validate our findings on a rigid-body motion test and a uniaxial tensile experiment, and we observe an excellent agreement between the stereo-DIC measurements and the ground truth. Using our findings, the reprojection error of self calibration is improved from 0.3 pixel to 0.1 pixel. The error in the stereo-DIC strain measurements is always less than 3.4% with the improvements made to self calibration, whereas it is as large as 7.6% without them.

Pt2AuCuNiSn, a new noble metal single-phase high entropy alloy

A new single-phase noble metal high entropy alloy, Pt2AuCuNiSn, has been obtained at comparatively low temperatures by a solid-state reaction. A Rietveld refinement gave a satisfactory description of the X-ray diffraction data, showing that the compound crystallizes with space group Fm3¯m, where only one Wyckoff site is occupied. In bulk samples, SEM/EDX measurements gave no indication for chemical inhomogeneities on a μm length scale. Temperature dependent in situ diffraction measurements using high energy (λ ​= ​0.1204 ​Å) radiation up to 875 ​K show several transient phases upon heating a mixture of the elements, consistent with results of DSC measurements. The parameter describing the variability of the radii of the constituent atoms, δr, is uncommonly large (δr ​= ​8.7%) and maybe the origin of the instability of this alloy at high temperatures.

Multi-scale quantification and modeling of aged nanostructured silicon-based composite anodes

Advanced anode material designs utilizing dual phase alloy systems like Si/FeSi2 nano-composites show great potential to decrease the capacity degrading and improve the cycling capability for Lithium (Li)-ion batteries. Here, we present a multi-scale characterization approach to understand the (de-)lithiation and irreversible volumetric changes of the amorphous silicon (a-Si)/crystalline iron-silicide (c-FeSi2) nanoscale phase and its evolution due to cycling, as well as their impact on the proximate pore network. Scattering and 2D/3D imaging techniques are applied to probe the anode structural ageing from nm to μm length scales, after up to 300 charge-discharge cycles, and combined with modeling using the collected image data as an input. We obtain a quantified insight into the inhomogeneous lithiation of the active material induced by the morphology changes due to cycling. The electrochemical performance of Li-ion batteries does not only depend on the active material used, but also on the architecture of its proximity.