Silica-Inspired Aerogel Thermal Metamaterials with Gradient Porosity: High-Temperature-Induced Pore Sintering Evolution via Nanoindentation

Localized densification of nanoporous silica under combined mechanical compression and elevated temperature involves coupled pore collapse, skeletal rearrangement, and thermally activated sintering. Clarifying how local pre-compression regulates these processes is important for understanding the surface and near-surface densification of nanoporous silica and related porous materials. In this study, the microscopic sintering behavior of a silica-inspired aerogel-like nanoporous model under the coupling of non-uniform local stress and high-temperature fields (indentation depths of 50–150 Å and temperatures of 298–1800 K) was systematically investigated using molecular dynamics simulations combined with a three-dimensional (3D) topological recognition algorithm (probe sphere method and DBSCAN clustering). The results indicate that the sintering densification of the silica-inspired aerogel model exhibits significant pore-size dependence and a “depth-temperature inverse relationship”: the local pre-compression induced by the 150 Å indentation facilitates thermally activated atomic rearrangement and shifts the onset of densification to a lower temperature, leading to an early bimodal splitting of the pore size distribution at 1300 K, accompanied by a significant jump in the elastic modulus from 3.0 to 10.07 GPa. In contrast, the 50 Å shallow region requires heating to 1800 K to achieve an equivalent densification effect. Furthermore, topological analysis quantitatively reveals the phase transition process of the pore network from connected to isolated: taking 1300 K as an example, the number of connected pore clusters decreases from the initial 86 to 70 (at 1000 ps), marking the fracture of the connected network; subsequently, the number of isolated pores surges to 4861, and the residual connected framework is severely fragmented into 136 micro-clusters. Based on the above microstructural and topological evolution data, a four-stage thermo-mechanical synergistic evolution process of the silica-inspired aerogel model is summarized. These findings provide quantitative fundamental data that conceptually supports the design of functional gradient structures with alternating “dense-thermally-conductive” and “porous-thermally-insulating” layers within a single continuous aerogel matrix; such structures may be realized in the future through strategies such as arrayed nanoindentation combined with high-temperature sintering.