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Clathrate BaNi2P4: An Interplay of Heat and Charge Transport Due to Strong Host–Guest Interactions
Chemistry of Materials ( IF 8.6 ) Pub Date : 2020-08-19 , DOI: 10.1021/acs.chemmater.0c02758
Jian Wang 1, 2 , Juli-Anna Dolyniuk 3 , Elizabeth H. Krenkel 2, 4 , Jennifer L. Niedziela 5, 6 , Makariy A. Tanatar 2, 4 , E. I. Timmons 2, 4 , Tyson Lanigan-Atkins 6 , Haidong Zhou 7 , Yongqiang Cheng 8 , Anibal J. Ramirez-Cuesta 8 , Deborah L. Schlagel 2 , Udhara S. Kaluarachchi 4 , Lin-Lin Wang 2 , Sergey L. Bud’ko 2, 4 , Paul C. Canfield 2, 4 , Ruslan Prozorov 2, 4 , Olivier Delaire 5, 6, 9 , Kirill Kovnir 1, 2
Affiliation  

Heat and charge transport properties of the metallic unconventional clathrate BaNi2P4, hosting Ba cations in oversized Ni8P16 cages, are investigated. A novel method of single-crystal growth was developed, yielding 2–3 mm sized crystals of BaNi2P4. We also developed a setup to accurately measure thermal conductivity and electrical resistivity of the synthesized single crystals in a wide temperature range avoiding crystal remounting. BaNi2P4 has a metallic temperature dependence of its electrical resistivity (decreasing with decreasing temperature) and manifests an unconventional T2 power law for 50 K < T < 300 K; below 50 K, the power-law exponent increases gradually such that below 10 K the power law is T5, a predicted but extremely rarely experimentally observed dependence for peculiar electron–phonon interactions. Electronic band structure calculations, consistent with measurements of de Haas–van Alphen oscillations, show large band dispersions with significant contributions of Ba orbitals to states near the Fermi level, which is atypical for clathrates. The thermal properties of BaNi2P4 were probed using a combination of variable-temperature single-crystal X-ray diffraction experiments, heat capacity measurements, first-principles phonon dispersion calculations, and inelastic neutron scattering measurements. BaNi2P4 exhibits significant hybridization of the Ba-guest and Ni–P-framework vibrational modes, which may be enhanced via the detected split of the Ba position, which results in strong Ba-framework interactions.

中文翻译:

包合物BaNi 2 P 4:强烈的宿主-客体相互作用导致热量和电荷传输的相互作用

研究了在超大型Ni 8 P 16笼中承载Ba阳离子的非常规金属笼形BaNi 2 P 4的热和电荷输运性质。开发了一种新的单晶生长方法,可产生2-3 mm大小的BaNi 2 P 4晶体。我们还开发了一种装置,可以在宽温度范围内准确测量合成单晶的导热率和电阻率,而无需重新安装晶体。BaNi 2 P 4具有金属电阻率的温度依赖性(随温度降低而降低),并表现出非常规的T 250 K < T <300 K的幂定律; 低于50 K时,幂律指数逐渐增加,使得低于10 K时,幂律为T 5,这是一种预测的但很少有实验观察到的对特殊电子-声子相互作用的依赖性。电子能带结构的计算与de Haas-van Alphen振荡的测量结果一致,显示出大的色散,其中Ba轨道对费米能级附近的状态有重要贡献,这对于包合物是非典型的。BaNi 2 P 4的热学性质使用可变温度单晶X射线衍射实验,热容测量,第一性原理声子色散计算和非弹性中子散射测量相结合的方法进行探测。BaNi 2 P 4表现出Ba-guest和Ni–P-框架振动模式的显着杂交,这可能通过检测到的Ba位置的分裂而增强,从而导致强烈的Ba-框架相互作用。
更新日期:2020-09-22
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