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Title: Novel Pd 2 Se 3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe 2

Abstract

Two-dimensional (2D) materials are easily fabricated when their bulk form has a layered structure. The monolayer form in layered transition-metal dichalcogenides is typically the same as a single layer of the bulk material. Yet, PdSe 2 presents a puzzle. Its monolayer form has been theoretically shown to be stable, but there have been no reports that monolayer PdSe 2 has been fabricated. Here, combining atomic-scale imaging in a scanning transmission electron microscope and density functional theory, we show that the preferred monolayer form of this material amounts to a melding of two bulk monolayers accompanied by the emission of Se atoms so that the resulting stoichiometry is Pd 2 Se 3 . We further verify the interlayer melding mechanism by creating Se vacancies in situ in the layered PdSe 2 matrix using electron irradiation. The discovery that strong interlayer interactions can be induced by defects and lead to the formation of new 2D materials opens a new venue for the exploration of defect engineering and novel 2D structures.

Authors:
 [1];  [2];  [3];  [3];  [2];  [4]
  1. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
  2. Vanderbilt Univ., Nashville, TN (United States)
  3. Nanyang Technological Univ. (Singapore)
  4. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan); Univ. of Tokyo (Japan)
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1597827
Alternate Identifier(s):
OSTI ID: 1368626
Grant/Contract Number:  
FG02-09ER46554
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 119; Journal Issue: 1; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Lin, Junhao, Zuluaga, Sebastian, Yu, Peng, Liu, Zheng, Pantelides, Sokrates T., and Suenaga, Kazu. Novel Pd2Se3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe2. United States: N. p., 2017. Web. doi:10.1103/PhysRevLett.119.016101.
Lin, Junhao, Zuluaga, Sebastian, Yu, Peng, Liu, Zheng, Pantelides, Sokrates T., & Suenaga, Kazu. Novel Pd2Se3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe2. United States. doi:10.1103/PhysRevLett.119.016101.
Lin, Junhao, Zuluaga, Sebastian, Yu, Peng, Liu, Zheng, Pantelides, Sokrates T., and Suenaga, Kazu. Thu . "Novel Pd2Se3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe2". United States. doi:10.1103/PhysRevLett.119.016101. https://www.osti.gov/servlets/purl/1597827.
@article{osti_1597827,
title = {Novel Pd2Se3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe2},
author = {Lin, Junhao and Zuluaga, Sebastian and Yu, Peng and Liu, Zheng and Pantelides, Sokrates T. and Suenaga, Kazu},
abstractNote = {Two-dimensional (2D) materials are easily fabricated when their bulk form has a layered structure. The monolayer form in layered transition-metal dichalcogenides is typically the same as a single layer of the bulk material. Yet, PdSe2 presents a puzzle. Its monolayer form has been theoretically shown to be stable, but there have been no reports that monolayer PdSe2 has been fabricated. Here, combining atomic-scale imaging in a scanning transmission electron microscope and density functional theory, we show that the preferred monolayer form of this material amounts to a melding of two bulk monolayers accompanied by the emission of Se atoms so that the resulting stoichiometry is Pd2Se3. We further verify the interlayer melding mechanism by creating Se vacancies in situ in the layered PdSe2 matrix using electron irradiation. The discovery that strong interlayer interactions can be induced by defects and lead to the formation of new 2D materials opens a new venue for the exploration of defect engineering and novel 2D structures.},
doi = {10.1103/PhysRevLett.119.016101},
journal = {Physical Review Letters},
number = 1,
volume = 119,
place = {United States},
year = {2017},
month = {7}
}

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Works referenced in this record:

Large-Area Synthesis of Monolayer and Few-Layer MoSe 2 Films on SiO 2 Substrates
journal, April 2014

  • Lu, Xin; Utama, M. Iqbal Bakti; Lin, Junhao
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl5000906

Top–down fabrication of sub-nanometre semiconducting nanoribbons derived from molybdenum disulfide sheets
journal, April 2013

  • Liu, Xiaofei; Xu, Tao; Wu, Xing
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2803

Spin Signature of Nonlocal Correlation Binding in Metal-Organic Frameworks
journal, September 2015


Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Van der Waals heterostructures
journal, July 2013

  • Geim, A. K.; Grigorieva, I. V.
  • Nature, Vol. 499, Issue 7459, p. 419-425
  • DOI: 10.1038/nature12385

Strongly enhanced charge-density-wave order in monolayer NbSe2
journal, July 2015

  • Xi, Xiaoxiang; Zhao, Liang; Wang, Zefang
  • Nature Nanotechnology, Vol. 10, Issue 9, p. 765-769
  • DOI: 10.1038/nnano.2015.143

Not your familiar two dimensional transition metal disulfide: structural and electronic properties of the PdS 2 monolayer
journal, January 2015

  • Wang, Yu; Li, Yafei; Chen, Zhongfang
  • Journal of Materials Chemistry C, Vol. 3, Issue 37
  • DOI: 10.1039/C5TC01345C

Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

  • Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
  • Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
  • DOI: 10.1038/nnano.2012.193

A density functional for sparse matter
journal, January 2009

  • Langreth, D. C.; Lundqvist, B. I.; Chakarova-Käck, S. D.
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 8
  • DOI: 10.1088/0953-8984/21/8/084203

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


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


Experimental and Theoretical Investigation on the Relative Stability of the PdS 2 - and Pyrite-Type Structures of PdSe 2
journal, March 2004

  • Soulard, C.; Rocquefelte, X.; Petit, P. -E.
  • Inorganic Chemistry, Vol. 43, Issue 6
  • DOI: 10.1021/ic0352396

Flexible metallic nanowires with self-adaptive contacts to semiconducting transition-metal dichalcogenide monolayers
journal, April 2014


Remarkable Order of a High-Performance Polymer
journal, May 2013

  • Takacs, Christopher J.; Treat, Neil D.; Krämer, Stephan
  • Nano Letters, Vol. 13, Issue 6
  • DOI: 10.1021/nl4005805

Two-dimensional atomic crystals
journal, July 2005

  • Novoselov, K. S.; Jiang, D.; Schedin, F.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 30, p. 10451-10453
  • DOI: 10.1073/pnas.0502848102

Exploring atomic defects in molybdenum disulphide monolayers
journal, February 2015

  • Hong, Jinhua; Hu, Zhixin; Probert, Matt
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7293

Van der Waals density functional: Self-consistent potential and the nature of the van der Waals bond
journal, September 2007


The crystal structure of PdSe2 and PdS2
journal, April 1957


Oxygen Disorder, a Way to Accommodate Large Epitaxial Strains in Oxides
journal, September 2015

  • Zhang, Yu Yang; Mishra, Rohan; Pennycook, Timothy J.
  • Advanced Materials Interfaces, Vol. 2, Issue 18
  • DOI: 10.1002/admi.201500344

Electronic, transport, and optical properties of bulk and mono-layer PdSe 2
journal, October 2015

  • Sun, Jifeng; Shi, Hongliang; Siegrist, Theo
  • Applied Physics Letters, Vol. 107, Issue 15
  • DOI: 10.1063/1.4933302

An atlas of two-dimensional materials
journal, January 2014

  • Miró, Pere; Audiffred, Martha; Heine, Thomas
  • Chem. Soc. Rev., Vol. 43, Issue 18
  • DOI: 10.1039/C4CS00102H

The electronic properties of graphene
journal, January 2009

  • Castro Neto, A. H.; Guinea, F.; Peres, N. M. R.
  • Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162
  • DOI: 10.1103/RevModPhys.81.109

The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets
journal, April 2013

  • Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki
  • Nature Chemistry, Vol. 5, Issue 4, p. 263-275
  • DOI: 10.1038/nchem.1589

Characterization of collective ground states in single-layer NbSe2
journal, November 2015

  • Ugeda, Miguel M.; Bradley, Aaron J.; Zhang, Yi
  • Nature Physics, Vol. 12, Issue 1
  • DOI: 10.1038/nphys3527

Two Dimensional Materials Beyond MoS 2 : Noble-Transition-Metal Dichalcogenides
journal, February 2014

  • Miró, Pere; Ghorbani-Asl, Mahdi; Heine, Thomas
  • Angewandte Chemie International Edition, Vol. 53, Issue 11
  • DOI: 10.1002/anie.201309280

Defects Engineered Monolayer MoS 2 for Improved Hydrogen Evolution Reaction
journal, January 2016


van der Waals forces in density functional theory: a review of the vdW-DF method
journal, May 2015


van der Waals Bonding in Layered Compounds from Advanced Density-Functional First-Principles Calculations
journal, June 2012


Structural Flexibility and Alloying in Ultrathin Transition-Metal Chalcogenide Nanowires
journal, January 2016


Ultrafast Phase Transition via Catastrophic Phonon Collapse Driven by Plasmonic Hot-Electron Injection
journal, January 2014

  • Appavoo, Kannatassen; Wang, Bin; Brady, Nathaniel F.
  • Nano Letters, Vol. 14, Issue 3
  • DOI: 10.1021/nl4044828

Tunable Band Gap Photoluminescence from Atomically Thin Transition-Metal Dichalcogenide Alloys
journal, April 2013

  • Chen, Yanfeng; Xi, Jinyang; Dumcenco, Dumitru O.
  • ACS Nano, Vol. 7, Issue 5, p. 4610-4616
  • DOI: 10.1021/nn401420h

Vacancy-Induced Formation and Growth of Inversion Domains in Transition-Metal Dichalcogenide Monolayer
journal, April 2015


A Single-Material Logical Junction Based on 2D Crystal PdS 2
journal, December 2015

  • Ghorbani-Asl, Mahdi; Kuc, Agnieszka; Miró, Pere
  • Advanced Materials, Vol. 28, Issue 5
  • DOI: 10.1002/adma.201504274

Extraordinarily Strong Interlayer Interaction in 2D Layered PtS 2
journal, February 2016


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