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Title: Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides

Abstract

Three-dimensional heterostructures are usually created either by assembling two-dimensional building blocks into hierarchical architectures or using stepwise chemical processes that sequentially deposit individual monolayers. Both approaches suffer from a number of issues, including lack of suitable precursors, limited reproducibility, and poor scalability of the preparation protocols. Therefore, development of alternative methods that enable preparation of heterostructured materials is desired. We create heterostructures with incommensurate arrangements of well-defined building blocks using a synthetic approach that comprises mechanical disassembly and simultaneous reordering of layered transition-metal dichalcogenides, MX2, and non-layered monochalcogenides, REX, where M = Ta, Nb, RE = Sm, La, and X = S, Se. We show that the discovered solid-state processes are rooted in stochastic mechanochemical transformations directed by electronic interaction between chemically and structurally dissimilar solids toward atomic-scale ordering, and offer an alternative to conventional heterostructuring. Details of composition–structure–properties relationships in the studied materials are also highlighted.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1];  [3]; ORCiD logo [1]; ORCiD logo [3];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [1]; ORCiD logo [5];  [1]
  1. Ames Lab., Ames, IA (United States)
  2. State Univ. of New York (SUNY), Buffalo, NY (United States); Ames Lab., Ames, IA (United States)
  3. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
  4. Iowa State Univ., Ames, IA (United States)
  5. Reed College, Portland, OR (United States); Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1633764
Report Number(s):
IS-J-10,216
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dolotko, Oleksandr, Hlova, Ihor Z., Pathak, Arjun K., Mudryk, Yaroslav, Pecharsky, Vitalij K., Singh, Prashant, Johnson, Duane D., Boote, Brett W., Li, Jingzhe, Smith, Emily A., Carnahan, Scott L., Rossini, Aaron J., Zhou, Lin, Eastman, Ely M., and Balema, Viktor P. Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides. United States: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-16672-0.
Dolotko, Oleksandr, Hlova, Ihor Z., Pathak, Arjun K., Mudryk, Yaroslav, Pecharsky, Vitalij K., Singh, Prashant, Johnson, Duane D., Boote, Brett W., Li, Jingzhe, Smith, Emily A., Carnahan, Scott L., Rossini, Aaron J., Zhou, Lin, Eastman, Ely M., & Balema, Viktor P. Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides. United States. https://doi.org/10.1038/s41467-020-16672-0
Dolotko, Oleksandr, Hlova, Ihor Z., Pathak, Arjun K., Mudryk, Yaroslav, Pecharsky, Vitalij K., Singh, Prashant, Johnson, Duane D., Boote, Brett W., Li, Jingzhe, Smith, Emily A., Carnahan, Scott L., Rossini, Aaron J., Zhou, Lin, Eastman, Ely M., and Balema, Viktor P. Fri . "Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides". United States. https://doi.org/10.1038/s41467-020-16672-0. https://www.osti.gov/servlets/purl/1633764.
@article{osti_1633764,
title = {Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides},
author = {Dolotko, Oleksandr and Hlova, Ihor Z. and Pathak, Arjun K. and Mudryk, Yaroslav and Pecharsky, Vitalij K. and Singh, Prashant and Johnson, Duane D. and Boote, Brett W. and Li, Jingzhe and Smith, Emily A. and Carnahan, Scott L. and Rossini, Aaron J. and Zhou, Lin and Eastman, Ely M. and Balema, Viktor P.},
abstractNote = {Three-dimensional heterostructures are usually created either by assembling two-dimensional building blocks into hierarchical architectures or using stepwise chemical processes that sequentially deposit individual monolayers. Both approaches suffer from a number of issues, including lack of suitable precursors, limited reproducibility, and poor scalability of the preparation protocols. Therefore, development of alternative methods that enable preparation of heterostructured materials is desired. We create heterostructures with incommensurate arrangements of well-defined building blocks using a synthetic approach that comprises mechanical disassembly and simultaneous reordering of layered transition-metal dichalcogenides, MX2, and non-layered monochalcogenides, REX, where M = Ta, Nb, RE = Sm, La, and X = S, Se. We show that the discovered solid-state processes are rooted in stochastic mechanochemical transformations directed by electronic interaction between chemically and structurally dissimilar solids toward atomic-scale ordering, and offer an alternative to conventional heterostructuring. Details of composition–structure–properties relationships in the studied materials are also highlighted.},
doi = {10.1038/s41467-020-16672-0},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {6}
}

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R.; Shanks, H. R.</span> </li> <li> Physical Review B, Vol. 15, Issue 10</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1103/PhysRevB.15.4576" class="text-muted" target="_blank" rel="noopener noreferrer">10.1103/PhysRevB.15.4576<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/j.pnmrs.2008.10.002" target="_blank" rel="noopener noreferrer" class="name">Solid-state selenium-77 NMR<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2009-04-01">April 2009</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Demko, Bryan A.; Wasylishen, Roderick E.</span> </li> <li> Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 54, Issue 3-4</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/j.pnmrs.2008.10.002" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/j.pnmrs.2008.10.002<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1038/nchem.1589" target="_blank" rel="noopener noreferrer" class="name">The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2013-04-01">April 2013</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki</span> </li> <li> Nature Chemistry, Vol. 5, Issue 4, p. 263-275</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1038/nchem.1589" class="text-muted" target="_blank" rel="noopener noreferrer">10.1038/nchem.1589<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1080/00958972.2018.1485019" target="_blank" rel="noopener noreferrer" class="name">Nanotubes from misfit layered compounds<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2018-06-14">June 2018</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Serra, Marco; Tenne, Reshef</span> </li> <li> Journal of Coordination Chemistry, Vol. 71, Issue 11-13</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1080/00958972.2018.1485019" class="text-muted" target="_blank" rel="noopener noreferrer">10.1080/00958972.2018.1485019<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1088/1361-6641/aa7785" target="_blank" rel="noopener noreferrer" class="name">Heterostructures containing dichalcogenides-new materials with predictable nanoarchitectures and novel emergent properties<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2017-08-16">August 2017</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Hamann, Danielle M.; Hadland, Erik C.; Johnson, David C.</span> </li> <li> Semiconductor Science and Technology, Vol. 32, Issue 9</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1088/1361-6641/aa7785" class="text-muted" target="_blank" rel="noopener noreferrer">10.1088/1361-6641/aa7785<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1039/C5TC02983J" target="_blank" rel="noopener noreferrer" class="name">Tubular structures from the LnS–TaS <sub>2</sub> (Ln = La, Ce, Nd, Ho, Er) and LaSe–TaSe <sub>2</sub> misfit layered compounds<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2016-01-01">January 2016</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Radovsky, Gal; Popovitz-Biro, Ronit; Lorenz, Tommy</span> </li> <li> Journal of Materials Chemistry C, Vol. 4, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/C5TC02983J" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/C5TC02983J<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1002/crat.201700126" target="_blank" rel="noopener noreferrer" class="name">Superconducting Tin Selenide/Niobium Diselenide Ferecrystals†<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2017-09-27">September 2017</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Grosse, Corinna; Alemayehu, Matti B.; Mogilatenko, Anna</span> </li> <li> Crystal Research and Technology, Vol. 52, Issue 10</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1002/crat.201700126" class="text-muted" target="_blank" rel="noopener noreferrer">10.1002/crat.201700126<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1039/b203694k" target="_blank" rel="noopener noreferrer" class="name">Solvent-free mechanochemical synthesis of two Pt complexes: cis-(Ph3P)2PtCl2 and cis-(Ph3P)2PtCO3Electronic supplementary information (ESI) available: differential thermal analysis data, X-ray diffraction data. See http://www.rsc.org/suppdata/cc/b2/b203694k/<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2002-06-26">June 2002</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Balema, Viktor P.; Wiench, Jerzy W.; Pruski, Marek</span> </li> <li> Chemical Communications, Issue 15</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/b203694k" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/b203694k<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1088/0953-8984/7/27/023" target="_blank" rel="noopener noreferrer" class="name">Raman scattering from misfit layer compounds (RS) <sub>x</sub> TaS <sub>2</sub> (R identical to La,Ce,Sm or Gd; S identical to sulphur; x approximately=1.2)<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1995-07-03">July 1995</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Kisoda, K.; Hangyo, M.; Nakashima, S.</span> </li> <li> Journal of Physics: Condensed Matter, Vol. 7, Issue 27</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1088/0953-8984/7/27/023" class="text-muted" target="_blank" rel="noopener noreferrer">10.1088/0953-8984/7/27/023<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.4028/www.scientific.net/MSF.378-381.118" target="_blank" rel="noopener noreferrer" class="name">WinPLOTR: A Windows Tool for Powder Diffraction Pattern Analysis<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2001-10-01">October 2001</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Roisnel, T.; Rodríquez-Carvajal, Juan</span> </li> <li> Materials Science Forum, Vol. 378-381</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.4028/www.scientific.net/MSF.378-381.118" class="text-muted" target="_blank" rel="noopener noreferrer">10.4028/www.scientific.net/MSF.378-381.118<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> </div> <div class="pagination-container small"> <a class="pure-button prev page" href="#" rel="prev"><span class="fa fa-angle-left"></span></a><ul class="pagination d-inline-block" style="padding-left:.2em;"></ul><a class="pure-button next page" href="#" rel="next"><span class="fa fa-angle-right"></span></a> </div> </div> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a href="" class="reference-type-filter tab-nav" data-tab="biblio-references" data-filter="type" data-pattern="*"><span class="fa fa-angle-right"></span> All References</a></li> <li class="small" style="margin-left:.75em; 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float:none;">[ × clear filter / sort ]</a> </div> </form> </div> </div> </div> </section> <section id="biblio-related" class="tab-content tab-content-sec " data-tab="biblio"> <div class="row"> <div class="col-sm-9 order-sm-9"> <section id="biblio-similar" class="tab-content tab-content-sec active" data-tab="related"> <div class="padding"> <p class="lead text-muted" style="font-size: 18px; margin-top:0px;">Similar Records in DOE PAGES and OSTI.GOV collections:</p> <aside> <ul class="item-list" itemscope itemtype="http://schema.org/ItemList" style="padding-left:0; list-style-type: none;"> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="0" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1375868-charge-transfer-crystalline-germanium-monolayer-mos-heterostructures-prepared-chemical-vapor-deposition" itemprop="url">Charge transfer in crystalline germanium/monolayer MoS <sub>2</sub> heterostructures prepared by chemical vapor deposition</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Lin, Yung-Chen</span> ; <span class="author">Bilgin, Ismail</span> ; <span class="author">Ahmed, Towfiq</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Nanoscale</span> </span> </div> <div class="abstract">Heterostructuring provides novel opportunities for exploring emergent phenomena and applications by developing designed properties beyond those of homogeneous materials. Advances in nanoscience enable the preparation of heterostructures formed incommensurate materials. Two-dimensional (2D) materials, such as graphene and transition metal dichalcogenides, are of particular interest due to their distinct physical characteristics. There have been recent changes in new research areas related to 2D/2D heterostructures. But, other heterostructures such as 2D/three-dimensional (3D) materials have not been thoroughly studied yet although the growth of 3D materials on 2D materials creating 2D/3D heterostructures with exceptional carrier transport properties has been reported. Here also we<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> report a novel heterostructure composed of Ge and monolayer MoS<sub>2</sub>, prepared by chemical vapor deposition. A single crystalline Ge (110) thin film was grown on monolayer MoS<sub>2</sub>. The electrical characteristics of Ge and MoS<sub>2</sub> in the Ge/MoS<sub>2</sub> heterostructure were remarkably different from those of isolated Ge and MoS<sub>2</sub>. The field-effect conductivity type of the monolayer MoS<sub>2</sub> is converted from n-type to p-type by growth of the Ge thin film on top of it. Undoped Ge on MoS<sub>2</sub> is highly conducting. The observations can be explained by charge transfer in the heterostructure as opposed to chemical doping via the incorporation of impurities, based on our first-principles calculations.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <span class="fa fa-book text-muted" aria-hidden="true"></span> Cited by 6<div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1039/C6NR03621J" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1375868" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1039/C6NR03621J</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1375868" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1375868" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="1" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1779060-quasi-two-dimensional-heterostructures-km1-te-late-sub-mn-zn-charge-density-waves" itemprop="url">Quasi-two-dimensional heterostructures (KM1 (-) Te-x)(LaTe{sub 3}) (M = Mn and Zn) with charge density waves.</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Bao, Jin-Ke</span> ; <span class="author">Malliakas, Christos D.</span> ; <span class="author">Zhang, Chi</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Chemistry of Materials</span> </span> </div> <div class="abstract">Layered heterostructure materials with two different functional building blocks can teach us about emergent physical properties and phenomena arising from interactions between the layers. We report intergrowth compounds KLaM1 - xTe4 (M = Mn and Zn; x approximate to 0.35) featuring two chemically distinct alternating layers [LaTe3] and [KM1 - xTe]. Their crystal structures are incommensurate, determined by single X-ray diffraction for the Mn compound and a transmission electron microscope study for the Zn compound. KLaMn1 (-) Te-x(4) crystallizes in the orthorhombic superspace group Pmnm(01/2 gamma)s00 with lattice parameters a = 4.4815(3) A, b = 21.6649(16) A, and c =<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> 4.5220(3) A. It exhibits charge density wave order at room temperature with a modulation wave vector q = 1/2b* + 0.3478c* originating from electronic instability of Te-square nets in [LaTe3] layers. The Mn analog exhibits a cluster spin glass behavior with spin freezing temperature T-f approximate to 5 K attributed to disordered Mn vacancies and competing magnetic interactions in the [Mn1 - xTe] layers. The Zn analog also has charge density wave order at room temperature with a similar q-vector having the c* component similar to 0.346 confirmed by selected-area electron diffraction. Electron transfer from [KM1 - xTe] to [LaTe3] layers exists in KLaM1 (-) Te-x(4), leading to an enhanced electronic specific heat coefficient. The resistivities of KLaM1 - xTe4 (M = Mn and Zn) exhibit metallic behavior at high temperatures and an upturn at low temperatures, suggesting partial localization of carriers in the [LaTe3] layers with some degree of disorder associated with the M atom vacancies in the [M1 - xTe] layers.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1021/acs.chemmater.0c04923" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1779060" data-product-type="Journal Article" data-product-subtype="AC" >https://doi.org/10.1021/acs.chemmater.0c04923</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="2" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/22311363-computational-prediction-two-dimensional-group-iv-mono-chalcogenides" itemprop="url">Computational prediction of two-dimensional group-IV mono-chalcogenides</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Singh, Arunima K.</span> ; <span class="author">Hennig, Richard G., E-mail: rhennig@cornell.edu</span> <span class="text-muted pubdata"> - Applied Physics Letters</span> </span> </div> <div class="abstract">Density functional calculations determine the structure, stability, and electronic properties of two-dimensional materials in the family of group-IV monochalcogenides, MX (M = Ge, Sn, Pb; X = O, S, Se, Te). Calculations with a van der Waals functional show that the two-dimensional IV-VI compounds are most stable in either a highly distorted NaCl-type structure or a single-layer litharge type tetragonal structure. Their formation energies are comparable to single-layer MoS{sub 2}, indicating the ease of mechanical exfoliation from their layered bulk structures. The phonon spectra confirm their dynamical stability. Using the hybrid HSE06 functional, we find that these materials are semiconductors with bandgaps that are<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> generally larger than for their bulk counterparts due to quantum confinement. The band edge alignments of monolayer group IV-VI materials reveal several type-I and type-II heterostructures, suited for optoelectronics and solar energy conversion.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1063/1.4891230" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="22311363" data-product-type="Journal Article" data-product-subtype="AC" >https://doi.org/10.1063/1.4891230</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="3" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1770863-formation-coherent-heterostructures-single-layer-mos2-au" itemprop="url">Formation of Coherent 1H–1T Heterostructures in Single-Layer MoS<sub>2</sub> on Au(111)</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Wu, Fanglue</span> ; <span class="author">Liu, Zhuotong</span> ; <span class="author">Hawthorne, Nathaniel</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - ACS Nano</span> </span> </div> <div class="abstract">Heterojunctions of semiconductors and metals are the fundamental building blocks of modern electronics. Coherent heterostructures between dissimilar materials can be achieved by composition, doping, or heteroepitaxy of chemically different elements. Here, we report the formation of coherent single-layer 1H–1T MoS<sub>2</sub> heterostructures by mechanical exfoliation on Au(111), which are chemically homogeneous with matched lattices but show electronically distinct semiconducting (1H phase) and metallic (1T phase) character, with the formation of these heterojunctions attributed to a combination of lattice strain and charge transfer. The exfoliation approach employed is free of tape residues usually found in many exfoliation methods and yields single-layer MoS<sub>2</sub><a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> with millimeter (mm) size on the Au surface. Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), scanning tunneling microscopy (STM), and scanning tunneling spectroscopy (STS) have collectively been employed to elucidate the structural and electronic properties of MoS<sub>2</sub> monolayers on Au substrates. Bubbles in the MoS<sub>2</sub> formed by the trapping of ambient adsorbates beneath the single layer during deposition, have also been observed and characterized. Lastly, our work here provides a basis to produce two-dimensional heterostructures which represent potential candidates for future electronic devices.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1021/acsnano.0c06014" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1770863" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acsnano.0c06014</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="4" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1477202-multi-principal-element-transition-metal-dichalcogenides-via-reactive-fusion-heterostructures" itemprop="url">Multi-principal element transition metal dichalcogenides <em>via</em> reactive fusion of 3D-heterostructures</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Hlova, Ihor Z.</span> ; <span class="author">Dolotko, Oleksandr</span> ; <span class="author">Boote, Brett W.</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - ChemComm</span> </span> </div> <div class="abstract">Transition metal dichalcogenides combining multiple principal elements in their structures are synthesized via mechanochemical exfoliation and spontaneous reassembly of binary precursors into 3D-heterostructures that are converted into single-phase layered materials by high-temperature reactive fusion. As a result, physical and chemical events enabling these transformations are summarized in the form of a conceivable reaction mechanism.</div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1039/C8CC06766J" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1477202" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1039/C8CC06766J</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1477202" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1477202" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> </ul> </aside> </div> </section> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a class="tab-nav disabled" data-tab="related" style="color: #636c72 !important; opacity: 1;"><span class="fa fa-angle-right"></span> Similar Records</a></li> </ul> </div> </div> </section> </div></div> </div> </div> </section> <footer class="" style="background-color:#f9f9f9; /* padding-top: 0.5rem; */"> <div class="footer-minor"> <div class="container"> <hr class="footer-separator" /> <div class="text-center" style="margin-top:1.25rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list" id="footer-org-menu"> <li class="pure-menu-item"> <a href="https://energy.gov" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-us-doe-min" alt="U.S. Department of Energy" /> </a> </li> <li class="pure-menu-item"> <a href="https://www.energy.gov/science/office-science" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-office-of-science-min" alt="Office of Science" /> </a> </li> <li class="pure-menu-item"> <a href="/"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-osti-min" alt="Office of Scientific and Technical Information" /> </a> </li> </ul> </div> </div> <div class="text-center small" style="margin-top:0.5em;margin-bottom:2.0rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list"> <li class="pure-menu-item"><a href="/disclaim" class="pure-menu-link"><span class="fa fa-institution"></span> Website Policies <span class="hidden-xs">/ Important Links</span></a></li> <li class="pure-menu-item"><a href="/pages/contact" class="pure-menu-link"><span class="fa fa-comments-o"></span> Contact Us</a></li> <li class="d-block d-md-none"></li> <li class="pure-menu-item"><a href="https://www.facebook.com/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-facebook" style=""></span></a></li> <li class="pure-menu-item"><a href="https://twitter.com/OSTIgov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-twitter" style=""></span></a></li> <li class="pure-menu-item"><a href="https://www.youtube.com/user/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-youtube-play" style=""></span></a></li> </ul> </div> </div> </div> </div> </footer> <link href="/pages/css/pages.fonts.210604.1157.css" rel="stylesheet"> <script src="/pages/js/pages.210604.1157.js"></script><noscript></noscript> <script defer src="/pages/js/pages.biblio.210604.1157.js"></script><noscript></noscript> <script defer src="/pages/js/lity.js"></script><noscript></noscript> <script async type="text/javascript" src="/pages/js/Universal-Federated-Analytics-Min.js?agency=DOE" id="_fed_an_ua_tag"></script><noscript></noscript> </body> <!-- DOE PAGES v.210604.1157 --> </html>