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Cement is one of the most produced materials in the world. A major player in greenhouse gas emissions, it is the main binding agent in concrete, to which it provides a cohesive strength that rapidly increases during setting. Understanding how such cohesion emerges has been a major obstacle to advances in cement science and technology. Here, we combine computational statistical mechanics and theory to demonstrate how cement cohesion results from the organization of interlocked ions and water, progressively confined in nano-slits between charged surfaces of Calcium-Silicate-Hydrates. Due to the water/ions interlocking, dielectric screening is drastically reduced and ionic correlations are proven significantly stronger than previously thought, dictating the evolution of the nano-scale interactions during cement hydration. By developing a quantitative analytical prediction of cement cohesion based on Coulombic forces, we reconcile a novel fundamental understanding of cement hydration with the fully atomistic description of the solid cement paste and open new paths for science and technologies of construction materials.
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The spontaneous permeation of overlay is a critical factor affecting the mechanical link of layer-to-layer interfaces. This work mainly studies the possibility of improving the interlayer bonding of 3D printed structures by increasing the spontaneous permeation of overlay. A polycarboxylate superplasticizer with high slump retention (TSRS) are employed to control the spontaneous permeation of cement-based materials. The rheological properties, micro-structure and interlayer bonding strength of printed structures with TSRS polymers are analyzed. Results indicate that fluidity is the key factor affecting the spontaneous permeation of cement-based materials. Properly improving the fluidity retention of cement-based materials can promote the spontaneous permeation of overlay, which fills part of the air-void systems of layer-to-layer interfaces, increases the mechanical interlocking and interlayer bonding strength of printed structures.
Capillary effects such as imbibition-drying cycles impact the mechanics of granular systems over time. A multiscale poromechanics framework was applied to cement paste, that is the most common building material, experiencing broad humidity variations over the lifetime of infrastructure. First, the liquid density distribution at intermediate to high relative humidities is obtained using a lattice gas density functional method together with a realistic nano-granular model of cement hydrates. The calculated adsorption/desorption isotherms and pore size distributions are discussed and compare well to nitrogen and water experiments. The standard method for pore size distribution determination from desorption data is evaluated. Then, the integration of the Korteweg liquid stress field around each cement hydrate particle provided the capillary forces at the nanoscale. The cement mesoscale structure was relaxed under the action of the capillary forces. Local irreversible deformations of the cement nano-grains assembly were identified due to liquid-solid interactions. The spatial correlations of the nonaffine displacements extend to a few tens of nm. Finally, the Love-Weber method provided the homogenized liquid stress at the micronscale. The homogenization length coincided with the spatial correlation length nonaffine displacements. Our results on the solid response to capillary stress field suggest that the micronscale texture is not affected by mild drying, while local irreversible deformations still occur. These results pave the way towards understanding capillary phenomena induced stresses in heterogeneous porous media ranging from construction materials, hydrogels to living systems.
Physicists become acquainted with special functions early in their studies. Consider our perennial model, the harmonic oscillator, for which we need Hermite functions, or the Laguerre functions in quantum mechanics. Here we choose a particular number theoretical function, the Riemann zeta function and examine its influence in the realm of physics and also how physics may be suggestive for the resolution of one of mathematics most famous unconfirmed conjectures, the Riemann Hypothesis. Does physics hold an essential key to the solution for this more than hundred-year-old problem? In this work we examine numerous models from different branches of physics, from classical mechanics to statistical physics, where this function plays an integral role. We also see how this function is related to quantum chaos and how its pole-structure encodes when particles can undergo Bose-Einstein condensation at low temperature. Throughout these examinations we highlight how physics can perhaps shed light on the Riemann Hypothesis. Naturally, our aim could not be to be comprehensive, rather we focus on the major models and aim to give an informed starting point for the interested Reader.
By generalizing the traditional concept of heat dQ and work dW to also include their time-dependent irreversible components d_{i}Q and d_{i}W allows us to express them in terms of the instantaneous internal temperature T(t) and pressure P(t), whereas the conventional form uses the constant values T_{0} and P_{0} of the medium. This results in an extremely useful formulation of non-equilibrium thermodynamics so that the first law turns into the Gibbs fundamental relation and the Clausius inequality becomes an equality ointdQ(t)/T(t)equiv0 in all cases, a quite remarkable but unexpected result. We determine the irreversible components d_{i}Qequivd_{i}W and discuss how they can be determined to obtain the generalized dW(t) and dQ(t).
Integration of semiconducting transition metal dichalcogenides (TMDs) into functional optoelectronic circuitries requires an understanding of the charge transfer across the interface between the TMD and the contacting material. Here, we use spatially resolved photocurrent microscopy to demonstrate electronic uniformity at the epitaxial graphene/molybdenum disulfide (EG/MoS2) interface. A 10x larger photocurrent is extracted at the EG/MoS2 interface when compared to metal (Ti/Au) /MoS2 interface. This is supported by semi-local density-functional theory (DFT), which predicts the Schottky barrier at the EG/MoS2 interface to be ~2x lower than Ti/MoS2. We provide a direct visualization of a 2D material Schottky barrier through combination of angle resolved photoemission spectroscopy with spatial resolution selected to be ~300 nm (nano-ARPES) and DFT calculations. A bending of ~500 meV over a length scale of ~2-3 micrometer in the valence band maximum of MoS2 is observed via nano-ARPES. We explicate a correlation between experimental demonstration and theoretical predictions of barriers at graphene/TMD interfaces. Spatially resolved photocurrent mapping allows for directly visualizing the uniformity of built-in electric fields at heterostructure interfaces, providing a guide for microscopic engineering of charge transport across heterointerfaces. This simple probe-based technique also speaks directly to the 2D synthesis community to elucidate electronic uniformity at domain boundaries alongside morphological uniformity over large areas.
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