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We study the conductive heat transport through calcium silicate hydrate (C-S-H) and organically cross-linked C-S-H via experiments, micromechanical homogenization theory, and molecular simulations. We find that C-S-H's intrinsic thermal conductivity falls below its amorphous limit when cross-linked with short-chain organosilanes. The observed reduction correlates with the alkyl chain length of the bis-organosilane molecule. To understand the underlying fundamental molecular processes accountable for such a reduction, we construct realistic molecular structures of cross-linked C-S-H and validate them against the spectroscopic and pycnometery measurements. The atomistic simulations indicate that the reduction in the contribution of propagons (propagating heat carriers) and diffusons (diffusive heat carriers) to heat transport, and the amplification of locons (localized vibrational modes), are the main driving factors allowing to limit the heat conduction in C-S-H. Presented findings offer new potential directions to nanoengineering novel admixtures for cement composites and resilient lightweight cementitious mesostructures for thermally efficient building envelopes. 

Organic–inorganic hybrids have found increasing applications for thermal management across various disciplines. Such materials can achieve thermal conductivities below the so-called “amorphous limit” of their constituents’ thermal conductivity. Despite their technological significance, a complete understanding of the origins of this thermal conductivity reduction remains elusive in these materials. In this paper, we develop a prototypical cross-linked organic–inorganic layered system, to investigate the spectral origins of its sub-amorphous thermal conductivity. Initially, we study the atomic structure of the model and find that besides polymer chain length, the relative drift of the layers governs the reduction in computed basal spacing, in agreement with experimental measurements. We, subsequently, find that organic cross-linking results in up to 40% reduction in thermal conductivity compared to inorganic samples. An in-depth investigation of vibrational modes reveals that this reduction is the result of reduced mode diffusivities, which in turn is a consequence of a vibrational mismatch between the organic and inorganic constituents. We also show that the contribution of propagating modes to the total thermal conductivity is not affected by organic cross-linking. Our approach paves the path toward a physics-informed analysis and design of a wide range of multifunctional hybrid nanomaterials for thermal management applications among others. 

Context.Blazars exhibit strong variability across the entire electromagnetic spectrum, including periods of high-flux states commonly known as flares. The physical mechanisms in blazar jets responsible for flares remain poorly understood to date. Aims.Our aim is to better understand the emission mechanisms during blazar flares using X-ray polarimetry and broadband observations from the archetypical TeV blazar Mrk 421, which can be studied with higher accuracy than other blazars that are dimmer and/or located farther away. Methods.We studied a flaring activity from December 2023 that was characterized from radio to very high-energy (VHE;E > 0.1 TeV) gamma rays with MAGIC,Fermi-LAT,Swift,XMM-Newton, and several optical and radio telescopes. These observations included, for the first time for a gamma-ray flare of a blazar, simultaneous X-ray polarization measurements with IXPE, in addition to optical and radio polarimetry data. We quantify the variability and correlations among the multi-band flux and polarization measurements, and describe the varying broadband emission within a theoretical scenario constrained by the polarization data. Results.We find substantial variability in both X-rays and VHE gamma rays throughout the campaign, with the highest VHE flux above 0.2 TeV occurring during the IXPE observing window, and exceeding twice the flux of the Crab Nebula. However, the VHE and X-ray spectra are on average softer, and the correlation between these two bands is weaker than those reported in the previous flares of Mrk 421. IXPE reveals an X-ray polarization degree significantly higher than that at radio and optical frequencies, similar to previous results for Mrk 421 and other high synchrotron peaked blazars. Differently to past observations, the X-ray polarization angle varies by ∼100° on timescales of days, and the polarization degree changes by more than a factor of 4. The highest X-ray polarization degree, analyzed in 12 h time intervals, reaches 26 ± 2%, around which an X-ray counter-clockwise hysteresis loop is measured withXMM-Newton. It suggests that the X-ray emission comes from particles close to the high-energy cutoff, hence possibly probing an extreme case of the Turbulent Extreme Multi-Zone model for which the chromatic trend in the polarization may be more pronounced than theoretically predicted. We model the broadband emission with a simplified stratified jet model throughout the flare. The polarization measurements imply an electron distribution in the X-ray emitting region with a very high minimum Lorentz factor ($$ \gamma\prime_{\mathrm{min}}\gtrsim10^4 $$), which is expected in electron-ion plasma, as well as a variation of the emitting region size of up to a factor of 3 during the flaring activity. We find no correlation between the fluxes and the evolution of the model parameters, which indicates a stochastic nature of the underlying physical mechanism that likely explains the lack of a tight X-ray/VHE correlation during this flaring activity. Such behavior would be expected in a highly turbulent electron-ion plasma crossing a shock front.