High hardness and high crack resistance are usually mutually exclusive in glass materials. Through the aerodynamic levitation and laser melting technique, we prepared a series of magnesium aluminosilicate glasses with a constant MgO content, and found a striking enhancement of both hardness and crack resistance with increasing Al2O3. The crack resistance of the magnesium aluminosilicate glass is about five times higher than that of the binary alumina‐silica glass for the similar [Al]/([Al] + [Si]) molar ratio (around 0.6). For the selected magnesium aluminosilicate glass with R = 0.32, when subjected to isothermal treatment at 1283K, we observed a further drastic enhancement of both hardness and crack resistance by extending the heating time. Based on the structural analyses, we propose an atomic‐scale model to explain the mechanism of synergetic enhancement in hardness and crack resistance for the magnesium aluminosilicate glasses and glass‐ceramics.

Through a chemo-mechanical milling process, we prepared a highly conductive (1.1 × 10 À 3 S · cm À 1 ) amorphous 0.5AgI · 0.5 Ag 3 PS 4 conductor, which is much higher than that of pure amorphous Ag 3 PS 4 (8.5 × 10 À 4 S · cm À 1 ). Detailed structural characterizations indicate that compared to the ionic conductivity of the amorphous Ag 3 PS 4 conductor, the enhancement can be ascribed to the formation of mixed polymeric anions {[PS 4 ] m I n } around Ag + ions. Through heat-treatment at 370°C for 20 minutes, the room temperature ionic conductivity of the 0.5AgI · 0.5 Ag 3 PS 4 conductor is further enhanced by about 4 times. This enhancement can be ascribed to the following two aspects: 1) the existence of residual amorphous phase with higher ionic conductivity; 2) the connection of the fast ionic conductive interfaces between the deposited Ag 7 PS 6 nanocrystals and the residual amorphous phase. This work reveals the key roles of both disorder and interface in improving the ionic conductivity of solid-state electrolytes.

Overcoming the brittleness of glass materials has always been one of the most important scientific questions in the field of materials physics. Herein, we selected a silica (SiO2) crystal, a silica glass, a sapphire (Al2O3) crystal, an amorphous alumina film, and a CaO⋅Al2O3 (CA) glass as the research objects. Detailed characterization was performed on two kinds of macromechanical properties, i.e., hardness and crack resistance. Combined with their density, bond density, bond energy density, and other structural features, we systematically investigated the structural origin and physics mechanism of hardness and crack resistance in a single phase material. The structural origin of the inverse relationship between hardness and crack resistance is ascribed to the facts that the bond density in a single phase material is generally positively correlated with the hardness while usually negatively correlated with the crack resistance. The discovery of simultaneously high hardness and high crack resistance in a CA glass revealed the key way to break through the inverse relationship between hardness and crack resistance, i.e., to develop the materials with the capability of self-adaptive structural adjustment, thus dissipating as much energy as possible upon external impact. These findings pave the way to the development of “scratchproof” and “unbreakable” transparent window materials such as a mobile phone screen glass.