Fu Shichen, Kang Kyungnam, Shayan Kamran, Yoshimura Anthony, Dadras Siamak, Wang Xiaotian, Zhang Lihua, Chen Siwei, Liu Na, Jindal Apoorv, Li Xiangzhi, Pasupathy Abhay N, Vamivakas A Nick, Meunier Vincent, Strauf Stefan, Yang Eui-Hyeok
Department of Mechanical Engineering, Stevens Institute of Technology, Hoboken, NJ, 07030, USA.
Department of Physics, Stevens Institute of Technology, Hoboken, NJ, 07030, USA.
Nat Commun. 2020 Apr 27;11(1):2034. doi: 10.1038/s41467-020-15877-7.
Two-dimensional semiconductors, including transition metal dichalcogenides, are of interest in electronics and photonics but remain nonmagnetic in their intrinsic form. Previous efforts to form two-dimensional dilute magnetic semiconductors utilized extrinsic doping techniques or bulk crystal growth, detrimentally affecting uniformity, scalability, or Curie temperature. Here, we demonstrate an in situ substitutional doping of Fe atoms into MoS monolayers in the chemical vapor deposition growth. The iron atoms substitute molybdenum sites in MoS crystals, as confirmed by transmission electron microscopy and Raman signatures. We uncover an Fe-related spectral transition of Fe:MoS monolayers that appears at 2.28 eV above the pristine bandgap and displays pronounced ferromagnetic hysteresis. The microscopic origin is further corroborated by density functional theory calculations of dipole-allowed transitions in Fe:MoS. Using spatially integrating magnetization measurements and spatially resolving nitrogen-vacancy center magnetometry, we show that Fe:MoS monolayers remain magnetized even at ambient conditions, manifesting ferromagnetism at room temperature.
二维半导体，包括过渡金属二硫属化物，在电子学和光子学领域备受关注，但其本征形式仍为非磁性。此前形成二维稀磁半导体的努力采用了非本征掺杂技术或体相晶体生长方法，这对均匀性、可扩展性或居里温度产生了不利影响。在此，我们展示了在化学气相沉积生长过程中，将铁原子原位替代掺杂到二硫化钼单层中。通过透射电子显微镜和拉曼特征证实，铁原子替代了二硫化钼晶体中的钼位点。我们发现了铁掺杂二硫化钼单层与铁相关的光谱跃迁，其出现在原始带隙上方2.28电子伏特处，并显示出明显的铁磁滞回线。密度泛函理论对铁掺杂二硫化钼中偶极允许跃迁的计算进一步证实了其微观起源。通过空间积分磁化测量和空间分辨氮空位中心磁力测量，我们表明铁掺杂二硫化钼单层即使在环境条件下仍保持磁化，在室温下表现出铁磁性。
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