文摘
Cubic La(Fe,Si)13-based compounds have been recently developed as promising negative thermal expansion(NTE) materials, but the narrow NTE operation-temperature window(鈭?10 K) restricts their actual applications. In this work, we demonstrate that the NTE operation-temperature window of LaFe13鈥?i>xSix can be significantly broadened by adjusting Fe鈥揊e magnetic exchange coupling as x ranges from 2.8 to 3.1. In particular, the NTE operation-temperature window of LaFe10.1Si2.9 is extended to 220 K. More attractively, the coefficients of thermal expansion of LaFe10.0Si3.0 and LaFe9.9Si3.1 are homogeneous in the NTE operation-temperature range of about 200 K, which is much valuable for the stability of fabricating devices. The further experimental characterizations combined with first-principles studies reveal that the tetragonal phase is gradually introduced into the cubic phase as the Si content increases, hence modifies the Fe鈥揊e interatomic distance. The reduction of the overall Fe鈥揊e magnetic exchange interactions contributes to the broadness of NTE operation-temperature window for LaFe13鈥?i>xSix.