He Xinyi, Chen Jinshuai, Katase Takayoshi, Minohara Makoto, Ide Keisuke, Hiramatsu Hidenori, Kumigashira Hiroshi, Hosono Hideo, Kamiya Toshio
Laboratory for Materials and Structures, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan.
Research Institute for Advanced Electronics and Photonics, National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki 305-8568, Japan.
ACS Appl Mater Interfaces. 2022 Apr 27;14(16):18682-18689. doi: 10.1021/acsami.2c01464. Epub 2022 Apr 14.
Metastable cubic (SnPb)Se with ≥ 0.5 is expected to be a high mobility semiconductor due to its Dirac-like electronic state, but it has an excessively high carrier concentration of ∼10 cm and is not suitable for semiconductor device applications such as thin film transistors and solar cells. Further, thin films of (SnPb)Se require a complicated synthesis process because of the high vapor pressure of Pb. We herein report the direct growth of metastable cubic (SnCa)Se films alloyed with CaSe, which has a wider bandgap and lower vapor pressure than PbSe. The cubic (SnCa)Se epitaxial films with = 0.4-0.8 are stabilized on YSZ (111) single crystalline substrates by pulsed laser deposition. (SnCa)Se has a direct-transition-type bandgap, and the bandgap energy can be varied from 1.4 eV ( = 0.4) to 2.0 eV ( = 0.8) by changing . These films with = 0.4-0.6 show p-type conduction with low hole carrier concentrations of ∼10 cm. Hall mobility analysis suggests that the hole transport would be dominated by 180° rotational domain structures, which is specific to (111) oriented epitaxial films. However, it, in turn, clarifies that the in-grain carrier mobility in the (SnCa)Se film is as high as 322 cm/(Vs), which is much higher than those in thermodynamically stable layered SnSe and other Sn-based layered semiconductor films at room temperature. Therefore, the present results prove the potential of high mobility (SnCa)Se films for semiconductor device applications via a simple thin-film deposition process.
锡铅比(Sn/Pb)≥0.5的亚稳立方相(SnPb)Se由于其类狄拉克电子态有望成为高迁移率半导体,但其载流子浓度过高,约为10²¹cm⁻³,不适用于薄膜晶体管和太阳能电池等半导体器件应用。此外,由于铅的高蒸气压,(SnPb)Se薄膜需要复杂的合成工艺。在此,我们报道了与CaSe合金化的亚稳立方相(SnCa)Se薄膜的直接生长,CaSe的带隙比PbSe更宽,蒸气压更低。通过脉冲激光沉积在YSZ(111)单晶衬底上稳定生长了锡铅比(Sn/Pb)=0.4 - 0.8的立方相(SnCa)Se外延薄膜。(SnCa)Se具有直接跃迁型带隙,通过改变锡铅比,带隙能量可在1.4 eV(锡铅比=0.4)至2.0 eV(锡铅比=0.8)之间变化。这些锡铅比(Sn/Pb)=0.4 - 0.6的薄膜表现出p型导电,空穴载流子浓度低,约为10¹⁸cm⁻³。霍尔迁移率分析表明,空穴输运将由180°旋转畴结构主导,这是(111)取向外延薄膜所特有的。然而,这反过来也表明,(SnCa)Se薄膜中的晶粒内载流子迁移率高达322 cm²/(V·s),远高于室温下热力学稳定的层状SnSe和其他Sn基层状半导体薄膜中的迁移率。因此,目前的结果证明了通过简单的薄膜沉积工艺,高迁移率(SnCa)Se薄膜在半导体器件应用中的潜力。