LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity

doi:10.1039/C9TA11150F

Title: LiSi ₃ As ₆ and Li ₂ SiAs ₂ with flexible SiAs ₂ polyanions: synthesis, structure, bonding, and ionic conductivity

Abstract

Two novel ternary phases, LiSi₃As₆ and Li₂SiAs₂, have been synthesized and characterized. Both phases have an identical Si : As ratio of 1 : 2 providing insight on how layers of the parent phase SiAs₂ accommodate excess electrons from Li cations to form Si–As anionic frameworks. LiSi₃As₆ exhibits a variety of bonding schemes involving Si–Si and As–As bonds, as well as corner-sharing SiAs₄ tetrahedra, while Li₂SiAs₂ is isostructural to the previously reported Li₂SiP₂, with adamantane-like Si₄As₁₀ units connected into 3D framework. LiSi₃As₆ and Li₂SiAs₂ are predicted to be indirect semiconductors which was experimentally confirmed by optical properties characterization. Li₂SiAs₂ exhibits low thermal conductivity of 1.20 W m^–1 K^–1 at 300 K in combination with a room temperature ionic conductivity of 7 × 10^–6 S cm^–1, an order of magnitude greater than that of the phosphide and nitride analogues, indicating its potential as a solid-state Li-ion conductor.

Authors:

^[1]; Lee, Kathleen ^[2]; Marple, Maxwell A. T. ^[3];

^[1]; Sen, Sabyasachi ^[3];

^[1]

Department of Chemistry, Iowa State University, Ames, USA, Ames Laboratory
Department of Chemistry, University of California, Davis, Davis, USA
Department of Materials Science and Engineering, University of California, Davis, Davis, USA

Publication Date:: 2020-01-09

Research Org.:: Ames Lab., Ames, IA (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:: 1594197

Alternate Identifier(s):: OSTI ID: 1601276

Report Number(s):: IS-J-10161
Journal ID: ISSN 2050-7488; JMCAET

Grant/Contract Number:: AC02-07CH11358

Resource Type:: Published Article

Journal Name:: Journal of Materials Chemistry. A

Additional Journal Information:: Journal Name: Journal of Materials Chemistry. A Journal Volume: 8 Journal Issue: 6; Journal ID: ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United Kingdom

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Mark, Justin, Lee, Kathleen, Marple, Maxwell A. T., Lee, Shannon, Sen, Sabyasachi, and Kovnir, Kirill. LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity.  United Kingdom: N. p., 2020. 
        Web.  doi:10.1039/C9TA11150F.

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                    Mark, Justin, Lee, Kathleen, Marple, Maxwell A. T., Lee, Shannon, Sen, Sabyasachi, & Kovnir, Kirill. LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity.  United Kingdom.  doi:10.1039/C9TA11150F.

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                    Mark, Justin, Lee, Kathleen, Marple, Maxwell A. T., Lee, Shannon, Sen, Sabyasachi, and Kovnir, Kirill. Thu .  
        "LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity".  United Kingdom.  doi:10.1039/C9TA11150F.

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@article{osti_1594197,

  title        = {LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity},

  author       = {Mark, Justin and Lee, Kathleen and Marple, Maxwell A. T. and Lee, Shannon and Sen, Sabyasachi and Kovnir, Kirill},

  abstractNote = {Two novel ternary phases, LiSi3As6 and Li2SiAs2, have been synthesized and characterized. Both phases have an identical Si : As ratio of 1 : 2 providing insight on how layers of the parent phase SiAs2 accommodate excess electrons from Li cations to form Si–As anionic frameworks. LiSi3As6 exhibits a variety of bonding schemes involving Si–Si and As–As bonds, as well as corner-sharing SiAs4 tetrahedra, while Li2SiAs2 is isostructural to the previously reported Li2SiP2, with adamantane-like Si4As10 units connected into 3D framework. LiSi3As6 and Li2SiAs2 are predicted to be indirect semiconductors which was experimentally confirmed by optical properties characterization. Li2SiAs2 exhibits low thermal conductivity of 1.20 W m–1 K–1 at 300 K in combination with a room temperature ionic conductivity of 7 × 10–6 S cm–1, an order of magnitude greater than that of the phosphide and nitride analogues, indicating its potential as a solid-state Li-ion conductor.},

  doi          = {10.1039/C9TA11150F},

  journal      = {Journal of Materials Chemistry. A},

  number       = 6,

  volume       = 8,

  place        = {United Kingdom},

  year         = {2020},

  month        = {1}

}

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margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Hönle, W.; Buresch, J.; Peters, K.</span> </li> <li> Zeitschrift für Kristallographie - New Crystal Structures, Vol. 217, Issue JG</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1524/ncrs.2002.217.jg.485" class="text-muted" target="_blank" rel="noopener noreferrer">10.1524/ncrs.2002.217.jg.485<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/10.1021/jacs.9b05301" target="_blank" rel="noopener noreferrer" class="name">Fast Ionic Conductivity in the Most Lithium-Rich Phosphidosilicate Li 14 SiP 6<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="2019-08-07">August 2019</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;"> Strangmüller, Stefan; Eickhoff, Henrik; Müller, David</span> </li> <li> Journal of the American Chemical Society, Vol. 141, Issue 36</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/jacs.9b05301" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/jacs.9b05301<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/10.1021/jacs.9b04653" target="_blank" rel="noopener noreferrer" class="name">Ba 2 Si 3 P 6 : 1D Nonlinear Optical Material with Thermal Barrier Chains<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="2019-07-05">July 2019</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;"> Mark, Justin; Wang, Jian; Wu, Kui</span> </li> <li> Journal of the American Chemical Society, Vol. 141, Issue 30</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/jacs.9b04653" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/jacs.9b04653<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/C2EE23355J" target="_blank" rel="noopener noreferrer" class="name">Phase stability, electrochemical stability and ionic conductivity of the Li <sub>10±1</sub> MP <sub>2</sub> X <sub>12</sub> (M = Ge, Si, Sn, Al or P, and X = O, S or Se) family of superionic conductors<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="2013-01-01">January 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;"> Ong, Shyue Ping; Mo, Yifei; Richards, William Davidson</span> </li> <li> Energy Environ. Sci., Vol. 6, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/C2EE23355J" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/C2EE23355J<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.jpowsour.2014.07.159" target="_blank" rel="noopener noreferrer" class="name">Synthesis, structure and lithium ionic conductivity of solid solutions of Li10(Ge1−M )P2S12 (M = Si, Sn)<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="2014-12-01">December 2014</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;"> Kato, Yuki; Saito, Ryoko; Sakano, Mitsuru</span> </li> <li> Journal of Power Sources, Vol. 271</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/j.jpowsour.2014.07.159" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/j.jpowsour.2014.07.159<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/10.3891/acta.chem.scand.19-1232" target="_blank" rel="noopener noreferrer" class="name">The Crystal Structure of SiAs.<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="1965-01-01">January 1965</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;"> Wadsten, Tommy; Burmester, S.; Cederberg, G.</span> </li> <li> Acta Chemica Scandinavica, Vol. 19</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.3891/acta.chem.scand.19-1232" class="text-muted" target="_blank" rel="noopener noreferrer">10.3891/acta.chem.scand.19-1232<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/anie.199718081" target="_blank" rel="noopener noreferrer" class="name">ELF: The Electron Localization Function<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="1997-09-17">September 1997</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;"> Savin, Andreas; Nesper, Reinhard; Wengert, Steffen</span> </li> <li> Angewandte Chemie International Edition in English, Vol. 36, Issue 17</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1002/anie.199718081" class="text-muted" target="_blank" rel="noopener noreferrer">10.1002/anie.199718081<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 osti-curated" 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="1" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/21212193-crystal-electronic-structures-photoluminescence-properties-rare-earth-doped-lisi-sub-sub" itemprop="url">Crystal, electronic structures and photoluminescence properties of rare-earth doped LiSi{sub 2}N{sub 3}</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">Li, Y Q</span> ; <span class="author">College of Materials Science and Engineering, Nanjing University of Technology, New Model Road 5, Nanjing, Jiangsu 210009</span> ; <span class="author">Hirosaki, N</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Journal of Solid State Chemistry</span> </span> </div> <div class="abstract">The crystal and electronic structures, and luminescence properties of Eu{sup 2+}, Ce{sup 3+} and Tb{sup 3+} activated LiSi{sub 2}N{sub 3} are reported. LiSi{sub 2}N{sub 3} is an insulator with an indirect band gap of about 5.0 eV (experimental value {approx}6.4 eV) and the Li 2s, 2p states are positioned on the top of the valence band close to the Fermi level and the bottom of the conduction band. The solubility of Eu{sup 2+} is significantly higher than Ce{sup 3+} and Tb{sup 3+} in LiSi{sub 2}N{sub 3} which may be strongly related to the valence difference between Li{sup +} and rare-earth<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> ions. LiSi{sub 2}N{sub 3}:Eu{sup 2+} shows yellow emission at about 580 nm due to the 4f{sup 6}5d{sup 1}{yields}4f{sup 7} transition of Eu{sup 2+}. Double substitution is found to be the effective ways to improve the luminescence efficiency of LiSi{sub 2}N{sub 3}:Eu{sup 2+}, especially for the partial replacement of (LiSi){sup 5+} with (CaAl){sup 5+}, which gives red emission at 620 nm, showing highly promising applications in white LEDs. LiSi{sub 2}N{sub 3}:Ce{sup 3+} emits blue light at about 450 nm arising from the 5d{sup 1}{yields}4f{sup 1}5d{sup 0} transition of Ce{sup 3+} upon excitation at 320 nm. LiSi{sub 2}N{sub 3}:Tb{sup 3+} gives strong green line emission with a maximum peak at about 542 nm attributed to the {sup 5}D{sub 4}{yields}{sup 7}F{sub J} (J=3-6) transition of Tb{sup 3+}, which is caused by highly efficient energy transfer from the LiSi{sub 2}N{sub 3} host to the Tb{sup 3+} ions. - Graphical abstract: Local crystal structure and luminescence spectra of Li{sub 1-2x-y}Ca{sub y}Eu{sub x}Si{sub 2-y}Al{sub y}N{sub 3}. The emission band of Eu{sup 2+} shifts from yellow to red spectral region by the double substitution Ca{sup 2+}{yields}Li{sup +} and Al{sup 3+}{yields}Si{sup 4+} simultaneously in Li{sub 1-2x}Eu{sub x}Si{sub 2}N{sub 3} due to the significant changes in the local environment of the Li{sub Ca,Eu} ions.</span><a href='#' onclick='$(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">DOI: <a class="misc doi-link " href="https://doi.org/10.1016/j.jssc.2008.10.031" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="21212193" data-product-type="Journal Article" data-product-subtype="" >10.1016/j.jssc.2008.10.031</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/5572160-zintl-phase-layered-network-structure-ksi-sub-sub" itemprop="url">Zintl phase with a layered network structure, KSi/sub 3/As/sub 3/</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">Hurng, W M</span> ; <span class="author">Corbett, J D</span> ; <span class="author">Wang, S L</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Inorg. Chem.; (United States)</span> </span> </div> <div class="abstract">The title compound is obtained in high yield from a two-step reaction of K with Si in sealed tantalum and then of that product with As in silica at 800-900/sup 0/C. Ion exchange with NaI at 500 /sup 0/C gives the sodium derivative. The structure of the purple KSi/sub 3/A/sub 3/ crystals has been established by x-ray diffraction means at room temperature (orthorhombic, space group Pbam, Z = 4, a = 10.010 (4) A, b = 19.139 (8) A, c = 3.664 (1) A, R = 0.044 for 674 reflections, 2theta < 55/sup 0/). The infinity /sup 2/(Si/sub 3/As/sub 3/)/sup<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> -/ anion layers may be generated by Si-Si bonding between puckered Si/sub 3/As/sub 3/(As) rings to form chains followed by side-by-side condensation of these to sheets. The structure may be derived from the layered structure of SiAs in a concerted way through reductive ring opening and Si-Si bond formation. Comparisons are also made with more reduced Si-As anion chains and clusters and with the closely related Li/sub 3/NaSi/sub 6/. K/sub 2/SiAs/sub 2/ has also been synthesized and shown to be isostructural with K/sub 2/SiP/sub 2/. 20 references, 4 figures, 4 tables.</span><a href='#' onclick='$(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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/ic00262a012" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="5572160" data-product-type="Journal Article" data-product-subtype="AC" >10.1021/ic00262a012</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="/biblio/7071770-synthesis-structure-zintl-phase-sub-sias-sub" itemprop="url">Synthesis and structure of the zintl phase K sub 2 SiAs sub 2</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">Hurng, W M</span> ; <span class="author">Peterson, E S</span> ; <span class="author">Corbett, J D</span> <span class="text-muted pubdata"> - Inorganic Chemistry; (USA)</span> </span> </div> <div class="abstract">The remarkable instability of K{sub 2}SiAs{sub 2}, often explosive at room temperature, is reported herein. It is also noted that K{sub 2}Si (As, P){sub 2} and the binary phase Si(Se, S) are not only isosteric but also isostructural except for the potassium cations. Diminished yields from synthesis reactions run for a longer time at 450{degree}C or at higher temperatures have strongly suggested that K{sub 2}SiAs{sub 2} is only a kinetic intermediate on the way to KSi{sub 3}As{sub 3} and binary phases. 19 refs., 3 figs., 2 tabs.</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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/ic00321a029" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="7071770" data-product-type="Journal Article" data-product-subtype="AC" >10.1021/ic00321a029</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/1480115-family-li-na-ag-si-ge-structural-magnetic-properties" itemprop="url">A <sub>2</sub>MnXO<sub>4</sub> Family (A = Li, Na, Ag; X = Si, Ge): Structural and Magnetic Properties</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">Nalbandyan, Vladimir B.</span> ; <span class="author">Zvereva, Elena A.</span> ; <span class="author">Shukaev, Igor L.</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Inorganic Chemistry</span> </span> </div> <div class="abstract">Four new manganese germanates and silicates, A<sub>2</sub>MnGeO<sub>4</sub> (A = Li, Na) and A<sub>2</sub>MnSiO<sub>4</sub> (A = Na, Ag), were prepared, and their crystal structures were determined using the X-ray Rietveld method. All of them contain all components in tetrahedral coordination. Li<sub>2</sub>MnGeO<sub>4</sub> is orthorhombic (Pmn2<sub>1</sub>) layered, isostructural with Li<sub>2</sub>CdGeO<sub>4</sub>, and the three other compounds are monoclinic (Pn) cristobalite-related frameworks. As in other stuffed cristobalites of various symmetry (Pn A<sub>2</sub>MXO<sub>4</sub>, Pna2<sub>1</sub> and Pbca AMO<sub>2</sub>), average bond angles on bridging oxygens (here, Mn–O–X) increase with increasing A/X and/or A/M radius ratios, indicating the trend to the ideal cubic (Fd<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> $$ \overline{3}\ $$m) structure typified by CsAlO<sub>2</sub>. The sublattices of the magnetic Mn<sup>2+</sup> ions in both structure types under study (Pmn2<sub>1</sub> and Pn) are essentially the same; namely, they are pseudocubic eutaxy with 12 nearest neighbors. The magnetic properties of the four new phases plus Li<sub>2</sub>MnSiO4 were characterized by carrying out magnetic susceptibility, specific heat, magnetization, and electron spin resonance measurements and also by performing energy-mapping analysis to evaluate their spin exchange constants. Ag<sub>2</sub>MnSiO<sub>4</sub> remains paramagnetic down to 2 K, but A<sub>2</sub>MnXO<sub>4</sub> (A = Li, Na; X = Si, Ge) undergo a three-dimensional antiferromagnetic ordering. All five phases exhibit short-range AFM ordering correlations, hence showing them to be low-dimensional magnets and a magnetic field induced spin-reorientation transition at T < TN for all AFM phases. We constructed the magnetic phase diagrams for A<sub>2</sub>MnXO<sub>4</sub> (A = Li, Na; X = Si, Ge) on the basis of the thermodynamic data in magnetic fields up to 9 T. The magnetic properties of all five phases experimentally determined are well explained by their spin exchange constants evaluated by performing energy-mapping analysis.</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 4<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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/acs.inorgchem.7b02130" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1480115" data-product-type="Journal Article" data-product-subtype="AM" >10.1021/acs.inorgchem.7b02130</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1480115" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1480115" 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="5" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/22584113-syntheses-structural-characterization-non-centrosymmetric-na-sub-sub-sub-ga-si-ge-sn-zn-cd-sulfides" itemprop="url">Syntheses and structural characterization of non-centrosymmetric Na{sub 2}M{sub 2}M'S{sub 6} (M, M′=Ga, In, Si, Ge, Sn, Zn, Cd) sulfides</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">Yohannan, Jinu P.</span> ; <span class="author">Vidyasagar, Kanamaluru</span> <span class="text-muted pubdata"> - Journal of Solid State Chemistry</span> </span> </div> <div class="abstract">Seven new non-centrosymmetric Na{sub 2}M{sub 2}M’S{sub 6} sulfides, namely, Na{sub 2}Sn{sub 2}ZnS{sub 6}(1){sub ,} Na{sub 2}Ga{sub 2}GeS{sub 6}(2), Na{sub 2}Ga{sub 2}SnS{sub 6}(3-α), Na{sub 2}Ga{sub 2}SnS{sub 6}(3-β){sub ,} Na{sub 2}Ge{sub 2}ZnS{sub 6}(4){sub ,} Na{sub 2}Ge{sub 2}CdS{sub 6}(5){sub ,} Na{sub 2}In{sub 2}SiS{sub 6}(6) and Na{sub 2}In{sub 2}GeS{sub 6}(7), were synthesized by high temperature solid state reactions and structurally characterized by single crystal X-ray diffraction. They crystallize in non-centrosymmetric Fdd2 and Cc space groups and their three-dimensional [M{sub 2}M′S{sub 6}]{sup 2-}framework structures consist of MS{sub 4} and M′S{sub 4} tetrahedra corner-connected to one another in either orderly or disordered fashion. Sodium ions reside<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> in the tunnels of the anionic framework. Compounds 1, 2 and 3-α have the structure of known Li{sub 2}Ga{sub 2}GeS{sub 6}, whereas compounds 6 and 7 are isostructural with known Li{sub 2}In{sub 2}GeS{sub 6} compound. Isostructural compounds 4 and 5 represent a new structural variant. Compounds 3-α and its new monoclinic structural variant 3-β have disordered structural framework. All of them are wide band gap semiconductors. Na{sub 2}Ga{sub 2}GeS{sub 6}(2), Na{sub 2}Ga{sub 2}SnS{sub 6}(3), Na{sub 2}Ge{sub 2}ZnS{sub 6}(4) and Na{sub 2}In{sub 2}GeS{sub 6}(7) compounds are found to be second-harmonic generation (SHG) active. Compounds 1, 2 and 3-α melt congruently. - Graphical abstract: Na{sub 2}Ga{sub 2}GeS{sub 6}, Na{sub 2}Ga{sub 2}SnS{sub 6}, Na{sub 2}Ge{sub 2}ZnS{sub 6}, Na{sub 2}In{sub 2}GeS{sub 6}, Na{sub 2}Sn{sub 2}ZnS{sub 6}, Na{sub 2}Ge{sub 2}CdS{sub 6} and Na{sub 2}In{sub 2}SiS{sub 6} have non-centrosymmetric structures and the first four compounds are SHG active. Display Omitted - Highlights: • Seven new Na{sub 2}M{sub 2}M′S{sub 6} compounds with non-centrosymmetric structures were synthesized. • They are wide band gap semiconductors. • Na{sub 2}Ga{sub 2}GeS{sub 6}, Na{sub 2}Ga{sub 2}SnS{sub 6}, Na{sub 2}Ge{sub 2}ZnS{sub 6} and Na{sub 2}In{sub 2}GeS{sub 6} are SHG active.</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">DOI: <a class="misc doi-link " href="https://doi.org/10.1016/J.JSSC.2016.03.026" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="22584113" data-product-type="Journal Article" data-product-subtype="AC" >10.1016/J.JSSC.2016.03.026</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> </ul> </aside> </div> </section> <section id="biblio-related-works" class="tab-content tab-content-sec" data-tab="related"> <div class="padding"> <p class="lead text-muted" style="font-size: 18px; margin-top:0px;"><span style="text-transform:capitalize;">Other research</span> related to this record:</p> <aside> <div class="list"> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.25505/fiz.icsd.cc23lnjx" target="_blank" rel="noopener noreferrer" class="name">CSD 1954349: Experimental Crystal Structure Determination<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">dataset</span>, <span class="date" data-date="2020-01-01">January 2020</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;"> Justin, Mark,; Kathleen, Lee,; T., Marple, Maxwell A.</span> </li> <li> FIZ Karlsruhe - Leibniz Institute for Information Infrastructure</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.25505/fiz.icsd.cc23lnjx" class="text-muted" target="_blank" rel="noopener noreferrer">10.25505/fiz.icsd.cc23lnjx<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> <li class="text-right"> <em class="text-muted"> This dataset is a supplement to the current record</em> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.25505/fiz.icsd.cc23lnky" target="_blank" rel="noopener noreferrer" class="name">CSD 1954350: Experimental Crystal Structure Determination<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; 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Title: LiSi 3 As 6 and Li 2 SiAs 2 with flexible SiAs 2 polyanions: synthesis, structure, bonding, and ionic conductivity

Abstract

Citation Formats

SiS2-isostrukturelle Anionen [SiP22−], [GeAs22−] und [SnAs22−] in Alkaliverbindungen journal, September 1991

The Crystal Structures of SiP2, SiAs2, and GeP. journal, January 1967

Electrochemical characterization of Li10SnP2S12: An electrolyte or a negative electrode for solid state Li-ion batteries? journal, November 2016

Enhancing Li Ion Conductivity of Garnet-Type Li 5 La 3 Nb 2 O 12 by Y- and Li-Codoping: Synthesis, Structure, Chemical Stability, and Transport Properties journal, September 2012

Origin of Fast Ion Conduction in Li 10 GeP 2 S 12 , a Superionic Conductor journal, December 2016

Supertetrahedral Networks and Lithium-Ion Mobility in Li 2 SiP 2 and LiSi 2 P 3 journal, September 2016

Title: LiSi ₃ As ₆ and Li ₂ SiAs ₂ with flexible SiAs ₂ polyanions: synthesis, structure, bonding, and ionic conductivity

SiS2-isostrukturelle Anionen [SiP22−], [GeAs22−] und [SnAs22−] in Alkaliverbindungen
journal, September 1991

The Crystal Structures of SiP2, SiAs2, and GeP.
journal, January 1967

Electrochemical characterization of Li10SnP2S12: An electrolyte or a negative electrode for solid state Li-ion batteries?
journal, November 2016

Enhancing Li Ion Conductivity of Garnet-Type Li 5 La 3 Nb 2 O 12 by Y- and Li-Codoping: Synthesis, Structure, Chemical Stability, and Transport Properties
journal, September 2012

Origin of Fast Ion Conduction in Li ₁₀ GeP ₂ S ₁₂ , a Superionic Conductor
journal, December 2016

Supertetrahedral Networks and Lithium-Ion Mobility in Li ₂ SiP ₂ and LiSi ₂ P ₃
journal, September 2016