Intercalating Anions between Terminated Anion Layers: Unusual Ionic S–Se Bonds and Hole-Doping Induced Superconductivity in S0.24(NH3)0.26Fe2Se2
- Ruijin SunRuijin SunInstitute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaMore by Ruijin Sun
- Shifeng Jin*Shifeng Jin*[email protected]Institute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaMore by Shifeng Jin
- Lin GuLin GuInstitute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaMore by Lin Gu
- Qinghua ZhangQinghua ZhangInstitute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaMore by Qinghua Zhang
- Qingzhen HuangQingzhen HuangNIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United StatesMore by Qingzhen Huang
- Tianping Ying
- YiRan PengYiRan PengDepartment of Physics and Center for Advanced Quantum Studies, Beijing Normal University, Beijing 100875, ChinaMore by YiRan Peng
- Jun DengJun DengInstitute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaMore by Jun Deng
- Zhiping YinZhiping YinDepartment of Physics and Center for Advanced Quantum Studies, Beijing Normal University, Beijing 100875, ChinaMore by Zhiping Yin
- Xiaolong Chen*Xiaolong Chen*[email protected]Institute of Physics, Chinese Academy of Science, Beijing 100190, ChinaSchool of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, ChinaCollaborative Innovation Center of Quantum Matter, Beijing 100190, ChinaSongshan Lake Materials Laboratory, Dongguan 523808, ChinaMore by Xiaolong Chen
Abstract
The pairing of ions of opposite charge is a central principle of chemistry. Even though the ability to intercalate anions is desirable for many applications, it remains a key challenge for numerous host materials with their outmost layers beingn anions. In this work, we introduce a hydrothermal ion-exchange synthesis to intercalate oxidative S and Se anions between the Se layers of FeSe, which leads to single crystals of novel compounds (Se/S)x(NH3)yFe2Se2. In particular, the unusual anion–anion bonding between the intercalated S (or Se) and Se layers exhibits strong ionic characteristics. The charge transfer through the Se layer to S (or Se) intercalants is further confirmed by the elevated oxidation state of Fe ions and the dominant hole carriers in the intercalated compounds. By intercalating S, for the first time superconductivity emerged in hole-doped iron chalcogenides. The generality of this chemical approach was further demonstrated with layered FeS and NiSe. Our findings thus open an avenue to exploring diverse aspects of anionic intercalation in similar materials.
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