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Band Structure Engineering of Layered WSe<sub>2</sub><i>via</i> One-Step Chemical Functionalization
Park, Jun Hong,Rai, Amritesh,Hwang, Jeongwoon,Zhang, Chenxi,Kwak, Iljo,Wolf, Steven F.,Vishwanath, Suresh,Liu, Xinyu,Dobrowolska, Malgorzata,Furdyna, Jacek,Xing, Huili Grace,Cho, Kyeongjae,Banerjee, S American Chemical Society 2019 ACS NANO Vol.13 No.7
<P>Chemical functionalization is demonstrated to enhance the p-type electrical performance of two-dimensional (2D) layered tungsten diselenide (WSe<SUB>2</SUB>) field-effect transistors (FETs) using a one-step dipping process in an aqueous solution of ammonium sulfide [(NH<SUB>4</SUB>)<SUB>2</SUB>S(aq)]. Molecularly resolved scanning tunneling microscopy and spectroscopy reveal that molecular adsorption on a monolayer WSe<SUB>2</SUB> surface induces a reduction of the electronic band gap from 2.1 to 1.1 eV and a Fermi level shift toward the WSe<SUB>2</SUB> valence band edge (VBE), consistent with an increase in the density of positive charge carriers. The mechanism of electronic transformation of WSe<SUB>2</SUB> by (NH<SUB>4</SUB>)<SUB>2</SUB>S(aq) chemical treatment is elucidated using density functional theory calculations which reveal that molecular “SH” adsorption on the WSe<SUB>2</SUB> surface introduces additional in-gap states near the VBE, thereby, inducing a Fermi level shift toward the VBE along with a reduction in the electronic band gap. As a result of the (NH<SUB>4</SUB>)<SUB>2</SUB>S(aq) chemical treatment, the p-branch ON-currents (<I>I</I><SUB>ON</SUB>) of back-gated few-layer ambipolar WSe<SUB>2</SUB> FETs are enhanced by about 2 orders of magnitude, and a ∼6× increase in the hole field-effect mobility is observed, the latter primarily resulting from the p-doping-induced narrowing of the Schottky barrier width leading to an enhanced hole injection at the WSe<SUB>2</SUB>/contact metal interface. This (NH<SUB>4</SUB>)<SUB>2</SUB>S(aq) chemical functionalization technique can serve as a model method to control the electronic band structure and enhance the performance of devices based on 2D layered transition-metal dichalcogenides.</P> [FIG OMISSION]</BR>