Despite its significance in both fundamental science and industrial applications,the glass-forming tran-sition in the Al_(2)O_(3)-Y_(2)O_(3)(AY)refractory system is not yet fully understood due to the elusive structur...Despite its significance in both fundamental science and industrial applications,the glass-forming tran-sition in the Al_(2)O_(3)-Y_(2)O_(3)(AY)refractory system is not yet fully understood due to the elusive structure evolution upon cooling.Here,atomic-scale structural changes in AY-bearing melts with different compo-sitions and temperatures are tracked by employing in situ high-energy synchrotron X-ray diffraction and empirical potential structure refinement simulation.We find that the glass-forming abilities(GFA)of AY-bearing melts are intriguingly correlated with the dependence of melt structure on temperature.In the case of the Al_(2)O_(3)and Y_(3)A_(l5)O_(12)(YAG),the observed large structural changes from superheating to under-cooling melt(i.e.,higher temperature susceptibility)correspond to a low GFA.Conversely,the 74Al_(2)O_(3)-26Y_(2)O_(3)(AY26)melt,with the smallest temperature susceptibility,exhibits the highest GFA.Simulation models illustrate that the temperature susceptibility of melt is associated with its atomic arrangement,especially the stability of cation-cation pairs.A balanced network(in AY26 melt),where the unsteady OAl3 tri-clusters are minimized and steady apex-to-apex connections between adjacent network units are abundant,contributes to stabilizing cationic interactions.This,in turn,fosters the formation of large-sized Al-O-Al rings,which topologically facilitates the subsequent glass-forming transition.Our findings provide new structural insight into the GFA of AY-bearing melts and may expand to other unconventional glass-forming systems to accelerate glassy materials design.展开更多
基金supported by the National Natural Science Foundation of China-Key Program(No.52234010)National Natural Science Foundation of China(No.51971138)+2 种基金National Natural Science Foundation of China-Distinguished Young Scholars(No.52325407)National Key Basic Research Program of China(No.2020YFA0406101)the fund of the State Key Laboratory of Solidification Processing in NWPU(No.SKLSP202102).
文摘Despite its significance in both fundamental science and industrial applications,the glass-forming tran-sition in the Al_(2)O_(3)-Y_(2)O_(3)(AY)refractory system is not yet fully understood due to the elusive structure evolution upon cooling.Here,atomic-scale structural changes in AY-bearing melts with different compo-sitions and temperatures are tracked by employing in situ high-energy synchrotron X-ray diffraction and empirical potential structure refinement simulation.We find that the glass-forming abilities(GFA)of AY-bearing melts are intriguingly correlated with the dependence of melt structure on temperature.In the case of the Al_(2)O_(3)and Y_(3)A_(l5)O_(12)(YAG),the observed large structural changes from superheating to under-cooling melt(i.e.,higher temperature susceptibility)correspond to a low GFA.Conversely,the 74Al_(2)O_(3)-26Y_(2)O_(3)(AY26)melt,with the smallest temperature susceptibility,exhibits the highest GFA.Simulation models illustrate that the temperature susceptibility of melt is associated with its atomic arrangement,especially the stability of cation-cation pairs.A balanced network(in AY26 melt),where the unsteady OAl3 tri-clusters are minimized and steady apex-to-apex connections between adjacent network units are abundant,contributes to stabilizing cationic interactions.This,in turn,fosters the formation of large-sized Al-O-Al rings,which topologically facilitates the subsequent glass-forming transition.Our findings provide new structural insight into the GFA of AY-bearing melts and may expand to other unconventional glass-forming systems to accelerate glassy materials design.
