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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. doi: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}
}

Journal Article:
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Figures / Tables:

Fig. 1 Fig. 1: Schematic illustration of 3D heterostructures. Schematic of (REX)1+ x(MX2), where M= transition metal, for example, Nb or Ta, RE= rare-earth metal, for example, La or Sm, and X= S or Se. a The three different projections shown can be observed by STEM imaging. b Perspective views of MX2more » and REX building blocks. c Projection of the heterostructure shown in a along [0 0 1] direction highlighting incommensurability along the a-axis with chalcogen atoms in the REX fragments omitted for clarity.« less

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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; 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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. 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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="sr-only">Previous Page</span><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="sr-only">Next Page</span><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> <input type="submit" id="sort_submit_references" name="submit" aria-label="submit" style="display: none;"/> </form> </div> </div> </div> </section> <section id="biblio-images" class="tab-content tab-content-sec osti-curated" data-tab="biblio"> <div class="row"> <div class="col-sm-9 order-sm-9"> <div class="padding"> <p class="lead text-muted" style="font-size: 18px; margin-top:0px;"><span id="image-type-label">Figures / Tables</span> found in this record:</p> <div class="list clearfix"> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 2" data-order="1" data-imgid="1633764-img429850" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429850.png" data-title="Fig. 1" data-desc="Schematic illustration of 3D heterostructures. Schematic of (REX)1+ x(MX2), where M= transition metal, for example, Nb or Ta, RE= rare-earth metal, for example, La or Sm, and X= S or Se. a The three different projections shown can be observed by STEM imaging. b Perspective views of MX2 and REX building blocks. c Projection of the heterostructure shown in a along [0 0 1] direction highlighting incommensurability along the a-axis with chalcogen atoms in the REX fragments omitted for clarity." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429850" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429850"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 1 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 2)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429850.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 3" data-order="2" data-imgid="1633764-img429852" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429852.png" data-title="Fig. 2" data-desc="Mechanochemical synthesis of the (SmS)(TaS2) heterostructure. a PXRD patterns of (SmS)(TaS2) obtained by ball milling of SmS and TaS2, or Sm, S, and TaS2 in the planetary mill for 30 h, and of the respective materials annealed at 1000 °C for 3 days. PXRD patterns of the starting materials, SmS and TaS2, are presented in Supplementary Information. b, c HAADF-STEM images of respective as-milled samples. The insets display enhanced views of the 3D heteroatomic moieties. Scale bars, 5 nm." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429852" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429852"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 2 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 3)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429852.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 4" data-order="3" data-imgid="1633764-img429856" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429856.png" data-title="Fig. 3" data-desc="Schematic representation of 3D heterostructures synthesis. Mechanochemical synthesis of (REX)n(MX2) heterostructures, where RE= rare earth; M= Ta or Nb; X= S or Se; and n values vary between 1 and 1.2." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429856" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429856"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 3 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 4)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429856.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 4" data-order="4" data-imgid="1633764-img429855" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429855.png" data-title="Fig. 4" data-desc="Microscopy characterization of the (SmS)(TaS2). STEM-EDS and HAADF-STEM images of (SmS)(TaS2) synthesized by ball milling and annealing of SmS and TaS2 mixture. A broad pink line in the EDS elemental mapping indicates a TaS2–TaS2 double layer that is clearly seen in the HAADF-STEM image (interlayer spacing 0.61 nm). Scale bar, 5 nm." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429855" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429855"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 4 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 4)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429855.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 4" data-order="5" data-imgid="1633764-img814608" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0814608.png" data-title="Table 1" data-desc="(REX)n(MX2) heterostructures synthesized in this work." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img814608" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img814608"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Table 1 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 4)</small><span class="d-none type">table</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0814608.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 5" data-order="6" data-imgid="1633764-img429857" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429857.png" data-title="Fig. 5" data-desc="Synthesis of the (LaSe)(NbSe2) heterostructure. a PXRD patterns and b HAADF-STEM images of (LaSe)(NbSe2) obtained by ball milling LaSe and NbSe2 for 12 h; c the HAADF-STEM image of the annealed material. An NbSe2–NbSe2 double layer is recognized in the lower right-hand corner of the image. Insets: enhanced atomic-scale views of 3D heterostructural arrangements. Scale bars, 5 nm." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429857" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429857"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 5 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 5)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429857.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 6" data-order="7" data-imgid="1633764-img429849" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429849.png" data-title="Fig. 6" data-desc="DFT calculations for (REX)n(MX2) heterostructures. a Relative DFT energies ΔE (i.e., the difference of total energies per atom relative to 2H-MX2) of (SmS)n(TaS2), n= 1.19 and of b (LaSe)n(NbSe2), n= 1.14 misfit compounds compared to single-phase cubic-REX [SmS, LaSe] and 2H-MX2 [TaS2, NbSe2] building blocks." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429849" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429849"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 6 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 6)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429849.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 6" data-order="8" data-imgid="1633764-img814609" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0814609.png" data-title="Table 2" data-desc="Total (Etotal) and formation (Eform) energies of (REX)n(MX2) heterostructures with comparison to cubic-REX and 2H-MX2 chalcogenidesa." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img814609" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img814609"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Table 2 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 6)</small><span class="d-none type">table</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0814609.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 7" data-order="9" data-imgid="1633764-img429851" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429851.png" data-title="Fig. 7" data-desc="DOS calculations for (REX)n(MX2) heterostructures. a Partial DOS and charge density of cubic-SmS, b 2H-TaS2, c (SmS)1.19(TaS2), d cubic-LaSe, e 2H-NbSe2, and f (LaSe)1.14(NbSe2). Charge density isosurfaces (0.03 e−/Å3) are plotted to highlight the distribution." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429851" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429851"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 7 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 7)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429851.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </div> <div class="col-sm-3 float-left biblio-image-tile" data-apporder="p. 8" data-order="10" data-imgid="1633764-img429853" data-imgsrc="/biblio/1633764/image/008/144/0081441/2/0429853.png" data-title="Fig. 8" data-desc="Electrical resistivity characterization of heterostructures. a Electrical resistivity versus temperature measured in 0 and 9 T fields for as-milled and c annealed (LaSe)(NbSe2); b as-milled and d annealed (SmS)(TaS2)." data-ostiid="1633764" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;"> <a href="#img" class="biblio-image-tile-a ga-click-event" data-imgid="1633764-img429853" data-lityx data-category="Extracted Images" data-label="biblio: image thumbnail" data-value="1633764-img429853"> <div style=" padding: .5em; border: 1px solid #eee; background-color: #fff; "> <small class="name">Fig. 8 <small class="pull-right" style="margin-right: .5em;color:#999;top: 3px;position: relative;">(p. 8)</small><span class="d-none type">figure</span></small> <div style=" background-image:url('/biblio/1633764/image/008/144/0081441/2/t0429853.png'); background-repeat:no-repeat; background-size:contain; background-position-x: center; width: 100%; height: 175px; margin-top:.5em; "> </div> </div> </a> </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-images" data-filter="type" data-pattern="*"><span class="fa fa-angle-right"></span> All Images</a></li> <li class="small" style="margin-left:.75em; 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padding:1em;"> <em>Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.</em> </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/1797577-incommensurate-transition-metal-dichalcogenides-via-mechanochemical-reshuffling-binary-precursors" itemprop="url">Incommensurate transition-metal dichalcogenides <em>via</em> mechanochemical reshuffling of binary precursors</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">Singh, Prashant</span> ; <span class="author">Malynych, Serhiy Z.</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Nanoscale Advances</span> </span> </div> <div class="abstract">A new family of heterostructured transition-metal dichalcogenides (TMDCs) with incommensurate (“misfit”) spatial arrangements of well-defined layers was prepared from structurally dissimilar single-phase 2H-MoS<sub>2</sub> and 1T-HfS<sub>2</sub> materials. The experimentally observed heterostructuring is energetically favorable over the formation of homogeneous multi-principle element dichalcogenides observed in related dichalcogenide systems of Mo, W, and Ta. The resulting three-dimensional (3D) heterostructures show semiconducting behavior with an indirect band gap around 1 eV, agreeing with values predicted from density functional theory. Results of this joint experimental and theoretical study open new avenues for generating unexplored metal-dichalcogenide heteroassemblies with incommensurate structures and tunable physical properties.</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/d1na00064k" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1797577" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1039/d1na00064k</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1797577" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1797577" 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="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="4" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/22410192-detection-nanoscale-embedded-layers-using-laboratory-specular-ray-diffraction" itemprop="url">Detection of nanoscale embedded layers using laboratory specular X-ray diffraction</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">Beekman, Matt</span> ; <span class="author">Rodriguez, Gabriel</span> ; <span class="author">Atkins, Ryan</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Journal of Applied Physics</span> </span> </div> <div class="abstract">Unusual specular X-ray diffraction patterns have been observed from certain thin film intergrowths of metal monochalcogenide (MX) and transition metal dichalcogenide (TX{sub 2}) structures. These patterns exhibit selective “splitting” or broadening of selected (00l) diffraction peaks, while other (00l) reflections remain relatively unaffected [Atkins et al., Chem. Mater. 24, 4594 (2012)]. Using a simplified optical model in the kinematic approximation, we illustrate that these peculiar and somewhat counterintuitive diffraction features can be understood in terms of additional layers of one of the intergrowth components, MX or TX{sub 2}, interleaved between otherwise “ideal” regions of MX-TX{sub 2} intergrowth. The interpretation is<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> in agreement with scanning transmission electron microscope imaging, which reveals the presence of such stacking “defects” in films prepared from non-ideal precursors. In principle, the effect can be employed as a simple, non-destructive laboratory probe to detect and characterize ultrathin layers of one material, e.g., 2-dimensional crystals, embedded between two slabs of a second material, effectively using the two slabs as a highly sensitive interferometer of their separation distance.</span><a href='#' onclick='$(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/10.1063/1.4920928" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="22410192" data-product-type="Journal Article" data-product-subtype="AC" >https://doi.org/10.1063/1.4920928</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="6" /><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="7" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1779060-quasi-two-dimensional-heterostructures-km1xte-late3-mn-zn-charge-density-waves" itemprop="url">Quasi-Two-Dimensional Heterostructures (K<em>M</em><sub>1 – <em>x</em></sub>Te)(LaTe<sub>3</sub>) (<em>M</em> = 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. Here, we report intergrowth compounds KLaM<sub>1 - x</sub>Te<sub>4</sub> (M = Mn and Zn;<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> $$x \approx$$ 0.35) featuring two chemically distinct alternating layers [LaTe<sub>3</sub>] and [KM<sub>1 - x</sub>Te]. 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. KLaMn<sub>1 – x</sub>Te<sub>4</sub> crystallizes in the orthorhombic superspace group Pmnm(01/2 gamma)s00 with lattice parameters a = 4.4815(3) Å, b = 21.6649(16) Å, and c = 4.5220(3) Å. 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 [LaTe<sub>3</sub>] layers. The Mn analog exhibits a cluster spin glass behavior with spin freezing temperature $$T_f \approx$$ 5 K attributed to disordered Mn vacancies and competing magnetic interactions in the [Mn<sub>1 - x</sub>Te] 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 [KM<sub>1 - x</sub>Te] to [LaTe<sub>3</sub>] layers exists in KLaM<sub>1 – x</sub>Te<sub>4</sub>, leading to an enhanced electronic specific heat coefficient. The resistivities of KLaM<sub>1 - x</sub>Te<sub>4</sub> (M = Mn and Zn) exhibit metallic behavior at high temperatures and an upturn at low temperatures, suggesting partial localization of carriers in the [LaTe<sub>3</sub>] layers with some degree of disorder associated with the M atom vacancies in the [M<sub>1 - x</sub>Te] 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="AM" >https://doi.org/10.1021/acs.chemmater.0c04923</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1779060" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1779060" 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="pure-menu-item"><a target="_blank" class="pure-menu-link" title="Vulnerability Disclosure Program" href="https://doe.responsibledisclosure.com/hc/en-us" rel="noopener noreferrer">Vulnerability Disclosure Program</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="sr-only">Facebook</span><em class="fa fa-facebook" style=""></em></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="sr-only">Twitter</span><em class="fa fa-twitter" style=""></em></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="sr-only">YouTube</span><em class="fa fa-youtube-play" style=""></em></a></li> </ul> </div> </div> </div> </div> </footer> <link href="/pages/css/pages.fonts.221101.1527.css" rel="stylesheet"> <script src="/pages/js/pages.221101.1527.js"></script><noscript></noscript> <script defer src="/pages/js/pages.biblio.221101.1527.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.221101.1527 --> </html>