Negative thermal expansion(NTE)is a notable physical property where a material’s volume decreases instead of increasing when heated.The identification of NTE materials is crucial for thermal expansion control enginee...Negative thermal expansion(NTE)is a notable physical property where a material’s volume decreases instead of increasing when heated.The identification of NTE materials is crucial for thermal expansion control engineering.Most NTE materials exhibit NTE only within a narrow temperature range,restricting their applications.Achieving NTE across a broad temperature range remains a significant challenge.This study developed a novel PbTiO_(3)-based system,(1-x)PbTiO_(3–x)BiLuO_(3),incorporating rare-earth elements,using a distinctive high-pressure and high-temperature synthesis technique.We achieved NTE across a broad temperature range by coupling lattice(c/a)with ferroelectric order parameters.The incorporation of BiLuO_(3)resulted in distinctive ferroelectric characteristics,including increased tetragonality,spontaneous polarization,and NTE over a broad temperature range.NTE over an extended temperature range has been achieved in 0.95PbTiO_(3)–0.05BiLuO_(3)(■=−1.7×10^(–5)K^(−1),300–840 K)and 0.90PbTiO_(3)–0.10BiLuO_(3)(■=−1.4×10^(–5)K^(−1),300–860 K),compared to pristine PbTiO_(3)(■=−1.99×10^(–5)K^(−1),300–763 K).The improved tetragonalities and broader NTE temperature range result from the strong hybridization of Pb/Bi–O and Ti/Lu–O atoms,as demonstrated by combined experimental and theoretical analyses,including high-energy synchrotron X-ray diffraction,Raman spectroscopy,and density functional theory calculations.This study introduces a novel example of NTE over a broad temperature range,highlighting its potential as a high-performance thermal expansion compensator.Additionally,it presents an effective method for incorporating rare-earth elements to achieve NTE in PbTiO_(3)-based perovskites across a wide temperature range.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22271309,12425403 and 12261131499)the National Key R&D Program of China(No.2021YFA1400300)+2 种基金financial support from the Science and Technology Development Fund from Macao SAR(No.0062/2023/ITP2)Macao Polytechnic University(No.RP/FCA-03/2023)Synchrotron X-ray powder diffraction experiments were conducted at SPring-8,approved by the Japan Synchrotron Radiation Research Institute(Nos.2024A1506,2024A1695 and 2024B1807)
文摘Negative thermal expansion(NTE)is a notable physical property where a material’s volume decreases instead of increasing when heated.The identification of NTE materials is crucial for thermal expansion control engineering.Most NTE materials exhibit NTE only within a narrow temperature range,restricting their applications.Achieving NTE across a broad temperature range remains a significant challenge.This study developed a novel PbTiO_(3)-based system,(1-x)PbTiO_(3–x)BiLuO_(3),incorporating rare-earth elements,using a distinctive high-pressure and high-temperature synthesis technique.We achieved NTE across a broad temperature range by coupling lattice(c/a)with ferroelectric order parameters.The incorporation of BiLuO_(3)resulted in distinctive ferroelectric characteristics,including increased tetragonality,spontaneous polarization,and NTE over a broad temperature range.NTE over an extended temperature range has been achieved in 0.95PbTiO_(3)–0.05BiLuO_(3)(■=−1.7×10^(–5)K^(−1),300–840 K)and 0.90PbTiO_(3)–0.10BiLuO_(3)(■=−1.4×10^(–5)K^(−1),300–860 K),compared to pristine PbTiO_(3)(■=−1.99×10^(–5)K^(−1),300–763 K).The improved tetragonalities and broader NTE temperature range result from the strong hybridization of Pb/Bi–O and Ti/Lu–O atoms,as demonstrated by combined experimental and theoretical analyses,including high-energy synchrotron X-ray diffraction,Raman spectroscopy,and density functional theory calculations.This study introduces a novel example of NTE over a broad temperature range,highlighting its potential as a high-performance thermal expansion compensator.Additionally,it presents an effective method for incorporating rare-earth elements to achieve NTE in PbTiO_(3)-based perovskites across a wide temperature range.
