Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3: Large Rashba Splitting in Topological Insulator Heterostructure

Shu Hsuan Su, Pei Yu Chuang, Sheng Wen Chen, Hsin Yu Chen, Yi Tung, Wei Chuan Chen, Chia Hsin Wang, Yaw Wen Yang, Jung Chun Andrew Huang, Tay Rong Chang, Hsin Lin, Horng Tay Jeng, Cheng Maw Cheng, Ku Ding Tsuei, Hai Lin Su, Yu Cheng Wu

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Ultrathin bilayers (BLs) of bismuth have been predicated to be a two-dimensional (2D) topological insulator. Here we report on a new route to manufacture the high-quality Bi bilayers from a 3D topological insulator, a top-down approach to prepare large-area and well-ordered Bi(111) BL with deliberate hydrogen etching on epitaxial Bi2Se3 films. With scanning tunneling microscopy (STM) and X-ray photoelectron spectra (XPS) in situ, we confirm that the removal of Se from the top of a quintuple layer (QL) is the key factor, leading to a uniform formation of Bi(111) BL in the van der Waals gap between the first and second QL of Bi2Se3. The angle resolved photoemission spectroscopy (ARPES) in situ and complementary density functional theory (DFT) calculations show a giant Rashba splitting with a coupling constant of 4.5 eV Å in the Bi(111) BL on Bi2Se3. Moreover, the thickness of Bi BLs can be tuned by the amount of hydrogen exposure. Our ARPES and DFT study indicated that the Bi hole-like bands increase with increasing the Bi BL thickness. The selective hydrogen etching is a promising route to produce a uniform ultrathin 2D topological insulator (TI) that is useful for fundamental investigations and applications in spintronics and valleytronics.

Original languageEnglish
Pages (from-to)8992-9000
Number of pages9
JournalChemistry of Materials
Volume29
Issue number21
DOIs
Publication statusPublished - 2017 Nov 14

Fingerprint

Heterojunctions
Hydrogen
Etching
Photoelectron spectroscopy
Density functional theory
Magnetoelectronics
Bismuth
Epitaxial films
Scanning tunneling microscopy
Photoelectrons
X rays

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Su, Shu Hsuan ; Chuang, Pei Yu ; Chen, Sheng Wen ; Chen, Hsin Yu ; Tung, Yi ; Chen, Wei Chuan ; Wang, Chia Hsin ; Yang, Yaw Wen ; Huang, Jung Chun Andrew ; Chang, Tay Rong ; Lin, Hsin ; Jeng, Horng Tay ; Cheng, Cheng Maw ; Tsuei, Ku Ding ; Su, Hai Lin ; Wu, Yu Cheng. / Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3 : Large Rashba Splitting in Topological Insulator Heterostructure. In: Chemistry of Materials. 2017 ; Vol. 29, No. 21. pp. 8992-9000.
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title = "Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3: Large Rashba Splitting in Topological Insulator Heterostructure",
abstract = "Ultrathin bilayers (BLs) of bismuth have been predicated to be a two-dimensional (2D) topological insulator. Here we report on a new route to manufacture the high-quality Bi bilayers from a 3D topological insulator, a top-down approach to prepare large-area and well-ordered Bi(111) BL with deliberate hydrogen etching on epitaxial Bi2Se3 films. With scanning tunneling microscopy (STM) and X-ray photoelectron spectra (XPS) in situ, we confirm that the removal of Se from the top of a quintuple layer (QL) is the key factor, leading to a uniform formation of Bi(111) BL in the van der Waals gap between the first and second QL of Bi2Se3. The angle resolved photoemission spectroscopy (ARPES) in situ and complementary density functional theory (DFT) calculations show a giant Rashba splitting with a coupling constant of 4.5 eV {\AA} in the Bi(111) BL on Bi2Se3. Moreover, the thickness of Bi BLs can be tuned by the amount of hydrogen exposure. Our ARPES and DFT study indicated that the Bi hole-like bands increase with increasing the Bi BL thickness. The selective hydrogen etching is a promising route to produce a uniform ultrathin 2D topological insulator (TI) that is useful for fundamental investigations and applications in spintronics and valleytronics.",
author = "Su, {Shu Hsuan} and Chuang, {Pei Yu} and Chen, {Sheng Wen} and Chen, {Hsin Yu} and Yi Tung and Chen, {Wei Chuan} and Wang, {Chia Hsin} and Yang, {Yaw Wen} and Huang, {Jung Chun Andrew} and Chang, {Tay Rong} and Hsin Lin and Jeng, {Horng Tay} and Cheng, {Cheng Maw} and Tsuei, {Ku Ding} and Su, {Hai Lin} and Wu, {Yu Cheng}",
year = "2017",
month = "11",
day = "14",
doi = "10.1021/acs.chemmater.7b01908",
language = "English",
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Su, SH, Chuang, PY, Chen, SW, Chen, HY, Tung, Y, Chen, WC, Wang, CH, Yang, YW, Huang, JCA, Chang, TR, Lin, H, Jeng, HT, Cheng, CM, Tsuei, KD, Su, HL & Wu, YC 2017, 'Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3: Large Rashba Splitting in Topological Insulator Heterostructure', Chemistry of Materials, vol. 29, no. 21, pp. 8992-9000. https://doi.org/10.1021/acs.chemmater.7b01908

Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3 : Large Rashba Splitting in Topological Insulator Heterostructure. / Su, Shu Hsuan; Chuang, Pei Yu; Chen, Sheng Wen; Chen, Hsin Yu; Tung, Yi; Chen, Wei Chuan; Wang, Chia Hsin; Yang, Yaw Wen; Huang, Jung Chun Andrew; Chang, Tay Rong; Lin, Hsin; Jeng, Horng Tay; Cheng, Cheng Maw; Tsuei, Ku Ding; Su, Hai Lin; Wu, Yu Cheng.

In: Chemistry of Materials, Vol. 29, No. 21, 14.11.2017, p. 8992-9000.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Selective Hydrogen Etching Leads to 2D Bi(111) Bilayers on Bi2Se3

T2 - Large Rashba Splitting in Topological Insulator Heterostructure

AU - Su, Shu Hsuan

AU - Chuang, Pei Yu

AU - Chen, Sheng Wen

AU - Chen, Hsin Yu

AU - Tung, Yi

AU - Chen, Wei Chuan

AU - Wang, Chia Hsin

AU - Yang, Yaw Wen

AU - Huang, Jung Chun Andrew

AU - Chang, Tay Rong

AU - Lin, Hsin

AU - Jeng, Horng Tay

AU - Cheng, Cheng Maw

AU - Tsuei, Ku Ding

AU - Su, Hai Lin

AU - Wu, Yu Cheng

PY - 2017/11/14

Y1 - 2017/11/14

N2 - Ultrathin bilayers (BLs) of bismuth have been predicated to be a two-dimensional (2D) topological insulator. Here we report on a new route to manufacture the high-quality Bi bilayers from a 3D topological insulator, a top-down approach to prepare large-area and well-ordered Bi(111) BL with deliberate hydrogen etching on epitaxial Bi2Se3 films. With scanning tunneling microscopy (STM) and X-ray photoelectron spectra (XPS) in situ, we confirm that the removal of Se from the top of a quintuple layer (QL) is the key factor, leading to a uniform formation of Bi(111) BL in the van der Waals gap between the first and second QL of Bi2Se3. The angle resolved photoemission spectroscopy (ARPES) in situ and complementary density functional theory (DFT) calculations show a giant Rashba splitting with a coupling constant of 4.5 eV Å in the Bi(111) BL on Bi2Se3. Moreover, the thickness of Bi BLs can be tuned by the amount of hydrogen exposure. Our ARPES and DFT study indicated that the Bi hole-like bands increase with increasing the Bi BL thickness. The selective hydrogen etching is a promising route to produce a uniform ultrathin 2D topological insulator (TI) that is useful for fundamental investigations and applications in spintronics and valleytronics.

AB - Ultrathin bilayers (BLs) of bismuth have been predicated to be a two-dimensional (2D) topological insulator. Here we report on a new route to manufacture the high-quality Bi bilayers from a 3D topological insulator, a top-down approach to prepare large-area and well-ordered Bi(111) BL with deliberate hydrogen etching on epitaxial Bi2Se3 films. With scanning tunneling microscopy (STM) and X-ray photoelectron spectra (XPS) in situ, we confirm that the removal of Se from the top of a quintuple layer (QL) is the key factor, leading to a uniform formation of Bi(111) BL in the van der Waals gap between the first and second QL of Bi2Se3. The angle resolved photoemission spectroscopy (ARPES) in situ and complementary density functional theory (DFT) calculations show a giant Rashba splitting with a coupling constant of 4.5 eV Å in the Bi(111) BL on Bi2Se3. Moreover, the thickness of Bi BLs can be tuned by the amount of hydrogen exposure. Our ARPES and DFT study indicated that the Bi hole-like bands increase with increasing the Bi BL thickness. The selective hydrogen etching is a promising route to produce a uniform ultrathin 2D topological insulator (TI) that is useful for fundamental investigations and applications in spintronics and valleytronics.

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