Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers
Abstract
Vertical stacking is widely viewed as a promising approach for designing advanced functionalities using two-dimensional (2D) materials. Combining crystallographically commensurate materials in these 2D stacks has been shown to result in rich new electronic structure, magnetotransport, and optical properties. In this context, vertical stacks of crystallographically incommensurate 2D materials with well-defined crystallographic order are a counterintuitive concept and, hence, fundamentally intriguing. We show that crystallographically dissimilar and incommensurate atomically thin MoS2 and Bi2Se3 layers can form rotationally aligned stacks with long-range crystallographic order. Our first-principles theoretical modeling predicts heterocrystal electronic band structures, which are quite distinct from those of the parent crystals, characterized with an indirect bandgap. Experiments reveal striking optical changes when Bi2Se3 is stacked layer by layer on monolayer MoS2, including 100% photoluminescence (PL) suppression, tunable transmittance edge (1.1→0.75 eV), suppressed Raman, and wide-band evolution of spectral transmittance. Disrupting the interface using a focused laser results in a marked the reversal of PL, Raman, and transmittance, demonstrating for the first time that in situ manipulation of interfaces can enable “reconfigurable” 2D materials. We demonstrate submicrometer resolution, “laser-drawing” and “bit-writing,” and novel laser-induced broadband light emission in these heterocrystal sheets.
- Authors:
-
- Northeastern Univ., Boston, MA (United States)
- Northeastern Univ., Boston, MA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Northeastern Univ., Boston, MA (United States); Univ. of Electronic Science and Technology of China, Sichuan (People's Republic of China)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for the Computational Design of Functional Layered Materials (CCDM); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1469909
- Grant/Contract Number:
- SC0012575; FG02-07ER46352; AC02-05CH11231
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 7; Related Information: CCDM partners with Temple University (lead); Brookhaven National Laboratory; Drexel University; Duke University; North Carolina State University; Northeastern University; Princeton University; Rice University; University of Pennsylvania; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; catalysis (heterogeneous); solar (photovoltaic); energy storage (including batteries and capacitors); hydrogen and fuel cells; defects; mechanical behavior; materials and chemistry by design; synthesis (novel materials)
Citation Formats
Vargas, Anthony, Liu, Fangze, Lane, Christopher, Rubin, Daniel, Bilgin, Ismail, Hennighausen, Zachariah, DeCapua, Matthew, Bansil, Arun, and Kar, Swastik. Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers. United States: N. p., 2017.
Web. doi:10.1126/sciadv.1601741.
Vargas, Anthony, Liu, Fangze, Lane, Christopher, Rubin, Daniel, Bilgin, Ismail, Hennighausen, Zachariah, DeCapua, Matthew, Bansil, Arun, & Kar, Swastik. Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers. United States. https://doi.org/10.1126/sciadv.1601741
Vargas, Anthony, Liu, Fangze, Lane, Christopher, Rubin, Daniel, Bilgin, Ismail, Hennighausen, Zachariah, DeCapua, Matthew, Bansil, Arun, and Kar, Swastik. 2017.
"Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers". United States. https://doi.org/10.1126/sciadv.1601741. https://www.osti.gov/servlets/purl/1469909.
@article{osti_1469909,
title = {Tunable and laser-reconfigurable 2D heterocrystals obtained by epitaxial stacking of crystallographically incommensurate Bi2Se3 and MoS2 atomic layers},
author = {Vargas, Anthony and Liu, Fangze and Lane, Christopher and Rubin, Daniel and Bilgin, Ismail and Hennighausen, Zachariah and DeCapua, Matthew and Bansil, Arun and Kar, Swastik},
abstractNote = {Vertical stacking is widely viewed as a promising approach for designing advanced functionalities using two-dimensional (2D) materials. Combining crystallographically commensurate materials in these 2D stacks has been shown to result in rich new electronic structure, magnetotransport, and optical properties. In this context, vertical stacks of crystallographically incommensurate 2D materials with well-defined crystallographic order are a counterintuitive concept and, hence, fundamentally intriguing. We show that crystallographically dissimilar and incommensurate atomically thin MoS2 and Bi2Se3 layers can form rotationally aligned stacks with long-range crystallographic order. Our first-principles theoretical modeling predicts heterocrystal electronic band structures, which are quite distinct from those of the parent crystals, characterized with an indirect bandgap. Experiments reveal striking optical changes when Bi2Se3 is stacked layer by layer on monolayer MoS2, including 100% photoluminescence (PL) suppression, tunable transmittance edge (1.1→0.75 eV), suppressed Raman, and wide-band evolution of spectral transmittance. Disrupting the interface using a focused laser results in a marked the reversal of PL, Raman, and transmittance, demonstrating for the first time that in situ manipulation of interfaces can enable “reconfigurable” 2D materials. We demonstrate submicrometer resolution, “laser-drawing” and “bit-writing,” and novel laser-induced broadband light emission in these heterocrystal sheets.},
doi = {10.1126/sciadv.1601741},
url = {https://www.osti.gov/biblio/1469909},
journal = {Science Advances},
issn = {2375-2548},
number = 7,
volume = 3,
place = {United States},
year = {Fri Jul 14 00:00:00 EDT 2017},
month = {Fri Jul 14 00:00:00 EDT 2017}
}
Web of Science
Figures / Tables:
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