Understanding Antiferromagnetic Coupling in Lead-Free Halide Double Perovskite Semiconductors,The Journal of Physical Chemistry C

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Understanding Antiferromagnetic Coupling in Lead-Free Halide Double Perovskite Semiconductors
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2024-03-14 , DOI: 10.1021/acs.jpcc.3c08129
Kunpot Mopoung ₁ , Weihua Ning ₂ , Muyi Zhang ₁ , Fuxiang Ji ₁ , Kingshuk Mukhuti ₃ , Hans Engelkamp ₃ , Peter C M Christianen ₃ , Utkarsh Singh ₁ , Johan Klarbring ₁ , Sergei I Simak _{1,

4} , Igor A Abrikosov ₁ , Feng Gao ₁ , Irina A Buyanova ₁ , Weimin M Chen ₁ , Yuttapoom Puttisong ₁

Affiliation

Solution-processable semiconductors with antiferromagnetic (AFM) order are attractive for future spintronics and information storage technology. Halide perovskites containing magnetic ions have emerged as multifunctional materials, demonstrating a cross-link between structural, optical, electrical, and magnetic properties. However, stable optoelectronic halide perovskites that are antiferromagnetic remain sparse, and the critical design rules to optimize magnetic coupling still must be developed. Here, we combine the complementary magnetometry and electron-spin-resonance experiments, together with first-principles calculations to study the antiferromagnetic coupling in stable Cs₂(Ag:Na)FeCl₆ bulk semiconductor alloys grown by the hydrothermal method. We show the importance of nonmagnetic monovalence ions at the B^I site (Na/Ag) in facilitating the superexchange interaction via orbital hybridization, offering the tunability of the Curie–Weiss parameters between −27 and −210 K, with a potential to promote magnetic frustration via alloying the nonmagnetic B^I site (Ag:Na ratio). Combining our experimental evidence with first-principles calculations, we draw a cohesive picture of the material design for B-site-ordered antiferromagnetic halide double perovskites.

中文翻译：

了解无铅卤化物双钙钛矿半导体中的反铁磁耦合

具有反铁磁（AFM）顺序的可溶液加工半导体对于未来的自旋电子学和信息存储技术具有吸引力。含有磁性离子的卤化物钙钛矿已成为多功能材料，展示了结构、光学、电学和磁性特性之间的交联。然而，反铁磁的稳定光电卤化物钙钛矿仍然很少，并且仍然必须开发优化磁耦合的关键设计规则。在这里，我们结合互补磁力测量和电子自旋共振实验以及第一性原理计算来研究通过水热法生长的稳定Cs ₂ (Ag:Na)FeCl ₆块状半导体合金中的反铁磁耦合。我们展示了 B ^I位点 (Na/Ag) 上的非磁性单价离子在通过轨道杂化促进超交换相互作用方面的重要性，提供了 -27 至 -210 K 之间的居里-魏斯参数的可调性，并有可能促进磁性通过合金化非磁性 B ^I位点（Ag:Na 比例）来实现挫败感。将我们的实验证据与第一性原理计算相结合，我们绘制了 B 位有序反铁磁卤化物双钙钛矿材料设计的连贯图景。

更新日期：2024-03-14

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