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Title: 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:
 [1]; ORCiD logo [2];  [1];  [1];  [1];  [1];  [1];  [1];  [3]
  1. Northeastern Univ., Boston, MA (United States)
  2. Northeastern Univ., Boston, MA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. 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}
}

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Cited by: 36 works
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Figures / Tables:

Fig. 1 Fig. 1: Structure of MoS2-Bi2Se3 heterocrystals. (A and B) Optical images of heterocrystals of 1QL-thick (A) and 2QL-thick (B) Bi2Se3 grown on 1TL MoS2 on quartz and SiO2/Si substrates, respectively. The contrast in (A) has been intentionally enhanced to obtain better visibility (see fig. S2 for the original image). (C)more » Low-magnification TEM image of a 1TL MoS2 sample (grown on a Si3N4 TEM membrane) partially covered with few-QL-thick Bi2Se3 grains. The SAED pattern of the sample was taken from the region outlined by the dashed circle, shown in (D). (D) Despite the presence of multiple nucleation sites, the Bi2Se3 unit cells grow in perfect rotational alignment with respect to the underlying MoS2 single crystal, resulting in the distinct, well-aligned superposed diffraction patterns of Bi2Se3 (green hexagon) and MoS2 (red hexagon). The lateral dimensions of this new crystal can be obtained from the pattern-separation distances along the (100) direction as shown (see fig. S11 for a larger image). (E) AFM step height analysis along a Bi2Se3 step edge in a heterocrystal. The step heights were found to be about 0.9 to 1.1 nm (see also section S1). (F and G) Geometry-optimized proposed structure of the 1TL-1QL heterocrystal. The unit cell of the heterocrystal structure has been demarcated using the red outline in the side view (F) and top view (G) of the crystal. (H) The top and side views of the parent unit cells are shown for comparison.« less

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Works referenced in this record:

Novel hetero-layered materials with tunable direct band gaps by sandwiching different metal disulfides and diselenides
journal, March 2013


Graphene, related two-dimensional crystals, and hybrid systems for energy conversion and storage
journal, January 2015


Generalized Gradient Approximation Made Simple
journal, October 1996


Quintuple-layer epitaxy of thin films of topological insulator Bi2Se3
journal, August 2009


Epitaxial growth of single-domain graphene on hexagonal boron nitride
journal, July 2013


Thermochemically evolved nanoplatelets of bismuth selenide with enhanced thermoelectric figure of merit
journal, November 2014


Synthesis of Strongly Fluorescent Molybdenum Disulfide Nanosheets for Cell-Targeted Labeling
journal, October 2014


Giant enhancement of light emission from nanoscale Bi 2 Se 3
journal, June 2015


Observation of tunable band gap and anisotropic Dirac semimetal state in black phosphorus
journal, August 2015


Emerging Photoluminescence in Monolayer MoS2
journal, April 2010


Colloquium : Topological band theory
journal, June 2016


Strain and curvature induced evolution of electronic band structures in twisted graphene bilayer
journal, July 2013


Valley-polarized exciton dynamics in a 2D semiconductor heterostructure
journal, February 2016


The ABC of 2D materials
journal, July 2015


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Vertical 2D/3D Semiconductor Heterostructures Based on Epitaxial Molybdenum Disulfide and Gallium Nitride
journal, February 2016


Van der Waals Epitaxy of Two-Dimensional MoS 2 –Graphene Heterostructures in Ultrahigh Vacuum
journal, May 2015


Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States
journal, November 2013


Tuning Dirac states by strain in the topological insulator Bi2Se3
journal, March 2014


Growth of High-Mobility Bi 2 Te 2 Se Nanoplatelets on hBN Sheets by van der Waals Epitaxy
journal, September 2012


Direct Growth of MoS 2 /h-BN Heterostructures via a Sulfide-Resistant Alloy
journal, January 2016


Controlled charge trapping by molybdenum disulphide and graphene in ultrathin heterostructured memory devices
journal, March 2013


Growth of large area few-layer or monolayer MoS2 from controllable MoO3 nanowire nuclei
journal, January 2014


Atomically thin p–n junctions with van der Waals heterointerfaces
journal, August 2014


Growing Vertical in the Flatland
journal, December 2015


Strongly Constrained and Appropriately Normed Semilocal Density Functional
journal, July 2015


Chemical Vapor Deposition Growth of Graphene and Related Materials
journal, December 2015


van der Waals Epitaxy of MoS2 Layers Using Graphene As Growth Templates
journal, May 2012


Vertical 2D Heterostructures
journal, July 2015


Two-dimensional heterostructures: fabrication, characterization, and application
journal, January 2014


Gate-induced superconductivity in atomically thin MoS2 crystals
journal, January 2016


Anomalous Lattice Vibrations of Single- and Few-Layer MoS 2
journal, March 2010


Coexisting massive and massless Dirac fermions in symmetry-broken bilayer graphene
journal, July 2013


Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films
journal, May 2013


Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices
journal, May 2013


Cloning of Dirac fermions in graphene superlattices
journal, May 2013


Van der Waals heterostructures
journal, July 2013


Vertical and in-plane heterostructures from WS2/MoS2 monolayers
journal, September 2014


Photoluminescence quenching in gold - MoS2 hybrid nanoflakes
journal, July 2014


Direct Growth of Single- and Few-Layer MoS 2 on h-BN with Preferred Relative Rotation Angles
journal, September 2015


Ab initio molecular dynamics for open-shell transition metals
journal, November 1993


Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform
journal, April 2015


Direct and Scalable Deposition of Atomically Thin Low-Noise MoS 2 Membranes on Apertures
journal, June 2015


Protecting the properties of monolayer MoS2 on silicon based substrates with an atomically thin buffer
journal, February 2016


Engineering Light Outcoupling in 2D Materials
journal, January 2015


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014


Moire bands in twisted double-layer graphene
journal, July 2011


All Chemical Vapor Deposition Growth of MoS 2 :h-BN Vertical van der Waals Heterostructures
journal, April 2015


Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2
journal, July 2015


Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure
journal, May 2013


Optical switches based on nanowires synthesized by molten salt solvent method
journal, November 2009


Precisely aligned graphene grown on hexagonal boron nitride by catalyst free chemical vapor deposition
journal, September 2013


Role of the Seeding Promoter in MoS 2 Growth by Chemical Vapor Deposition
journal, January 2014


Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006


An atlas of two-dimensional materials
journal, January 2014


A subthermionic tunnel field-effect transistor with an atomically thin channel
journal, September 2015


Rotationally Commensurate Growth of MoS 2 on Epitaxial Graphene
journal, November 2015


The Changing Colors of a Quantum-Confined Topological Insulator
journal, January 2014


Highly efficient gate-tunable photocurrent generation in vertical heterostructures of layered materials
journal, October 2013


Observation of Van Hove singularities in twisted graphene layers
journal, November 2009


Colloidal synthesis of MoS 2 quantum dots: size-dependent tunable photoluminescence and bioimaging
journal, January 2015


Optical properties and electronic structure of amorphous Ge and Si
journal, January 1968


Leaning on a ledge
journal, November 2020


Resonant internal Quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2
text, January 2015


Anomalous Lattice Vibrations of Single and Few-Layer MoS2
text, January 2010


Moire bands in twisted double-layer graphene
text, January 2010


Cloning of Dirac fermions in graphene superlattices
text, January 2012


Strongly Constrained and Appropriately Normed Semilocal Density Functional
preprint, January 2015


Works referencing / citing this record:

Second-Harmonic Spectroscopy for Defects Engineering Monitoring in Transition Metal Dichalcogenides
journal, January 2018


Recent Advances in van der Waals Heterojunctions Based on Semiconducting Transition Metal Dichalcogenides
journal, August 2018


Recent Progress of Janus 2D Transition Metal Chalcogenides: From Theory to Experiments
journal, September 2018


Evidence of a purely electronic two-dimensional lattice at the interface of TMD/Bi 2 Se 3 heterostructures
journal, January 2019


A roadmap for electronic grade 2D materials
journal, January 2019


Widely tunable Bi 2 Se 3 /transition metal dichalcogenide 2D heterostructures for write-read-erase-reuse applications
journal, August 2019


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.