Synthesis of a Neutral Mixed-Valence Diferrocenyl Carborane for Molecular Quantum-Dot Cellular Automata Applications
The preparation of 7‐Fc+‐8‐Fc‐7,8‐nido‐[C2B9H10]− (Fc+FcC2B9−) demonstrates the successful incorporation of a carborane cage as an internal counteranion bridging between ferrocene and ferrocenium units. This neutral mixed‐valence FeII/FeIII complex overcomes the proximal electronic bias imposed by e...
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Veröffentlicht in: | Angewandte Chemie International Edition 2015-12, Vol.54 (51), p.15448-15451 |
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creator | Christie, John A. Forrest, Ryan P. Corcelli, Steven A. Wasio, Natalie A. Quardokus, Rebecca C. Brown, Ryan Kandel, S. Alex Lu, Yuhui Lent, Craig S. Henderson, Kenneth W. |
description | The preparation of 7‐Fc+‐8‐Fc‐7,8‐nido‐[C2B9H10]− (Fc+FcC2B9−) demonstrates the successful incorporation of a carborane cage as an internal counteranion bridging between ferrocene and ferrocenium units. This neutral mixed‐valence FeII/FeIII complex overcomes the proximal electronic bias imposed by external counterions, a practical limitation in the use of molecular switches. A combination of UV/Vis‐NIR spectroscopic and TD‐DFT computational studies indicate that electron transfer within Fc+FcC2B9− is achieved through a bridge‐mediated mechanism. This electronic framework therefore provides the possibility of an all‐neutral null state, a key requirement for the implementation of quantum‐dot cellular automata (QCA) molecular computing. The adhesion, ordering, and characterization of Fc+FcC2B9− on Au(111) has been observed by scanning tunneling microscopy.
Zwitterionic molecular switches: A neutral mixed‐valence compound has been synthesized and characterized. Spectroscopic data, in conjunction with TD‐DFT calculations, indicate a bridge‐mediated charge transfer that allows for an all‐neutral null state vital to QCA molecular switch applications. |
doi_str_mv | 10.1002/anie.201507688 |
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Zwitterionic molecular switches: A neutral mixed‐valence compound has been synthesized and characterized. Spectroscopic data, in conjunction with TD‐DFT calculations, indicate a bridge‐mediated charge transfer that allows for an all‐neutral null state vital to QCA molecular switch applications.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.201507688</identifier><identifier>PMID: 26516063</identifier><identifier>CODEN: ACIEAY</identifier><language>eng</language><publisher>Weinheim: WILEY-VCH Verlag</publisher><subject>Automata theory ; Carborane ; carboranes ; Cellular automata ; Computer applications ; Electron transfer ; mixed-valence compounds ; Molecular machines ; QCA ; Scanning tunneling microscopy ; STM ; Switches ; zwitterions</subject><ispartof>Angewandte Chemie International Edition, 2015-12, Vol.54 (51), p.15448-15451</ispartof><rights>2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.</rights><rights>2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>Copyright Wiley Subscription Services, Inc. Dec 2015</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c6128-a2298daf18f9e3f1b818c505f9f2b990a1a7299d1954cb284898f6e6daa03b323</citedby><cites>FETCH-LOGICAL-c6128-a2298daf18f9e3f1b818c505f9f2b990a1a7299d1954cb284898f6e6daa03b323</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.201507688$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.201507688$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,776,780,1411,27901,27902,45550,45551</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/26516063$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Christie, John A.</creatorcontrib><creatorcontrib>Forrest, Ryan P.</creatorcontrib><creatorcontrib>Corcelli, Steven A.</creatorcontrib><creatorcontrib>Wasio, Natalie A.</creatorcontrib><creatorcontrib>Quardokus, Rebecca C.</creatorcontrib><creatorcontrib>Brown, Ryan</creatorcontrib><creatorcontrib>Kandel, S. Alex</creatorcontrib><creatorcontrib>Lu, Yuhui</creatorcontrib><creatorcontrib>Lent, Craig S.</creatorcontrib><creatorcontrib>Henderson, Kenneth W.</creatorcontrib><title>Synthesis of a Neutral Mixed-Valence Diferrocenyl Carborane for Molecular Quantum-Dot Cellular Automata Applications</title><title>Angewandte Chemie International Edition</title><addtitle>Angew. Chem. Int. Ed</addtitle><description>The preparation of 7‐Fc+‐8‐Fc‐7,8‐nido‐[C2B9H10]− (Fc+FcC2B9−) demonstrates the successful incorporation of a carborane cage as an internal counteranion bridging between ferrocene and ferrocenium units. This neutral mixed‐valence FeII/FeIII complex overcomes the proximal electronic bias imposed by external counterions, a practical limitation in the use of molecular switches. A combination of UV/Vis‐NIR spectroscopic and TD‐DFT computational studies indicate that electron transfer within Fc+FcC2B9− is achieved through a bridge‐mediated mechanism. This electronic framework therefore provides the possibility of an all‐neutral null state, a key requirement for the implementation of quantum‐dot cellular automata (QCA) molecular computing. The adhesion, ordering, and characterization of Fc+FcC2B9− on Au(111) has been observed by scanning tunneling microscopy.
Zwitterionic molecular switches: A neutral mixed‐valence compound has been synthesized and characterized. Spectroscopic data, in conjunction with TD‐DFT calculations, indicate a bridge‐mediated charge transfer that allows for an all‐neutral null state vital to QCA molecular switch applications.</description><subject>Automata theory</subject><subject>Carborane</subject><subject>carboranes</subject><subject>Cellular automata</subject><subject>Computer applications</subject><subject>Electron transfer</subject><subject>mixed-valence compounds</subject><subject>Molecular machines</subject><subject>QCA</subject><subject>Scanning tunneling microscopy</subject><subject>STM</subject><subject>Switches</subject><subject>zwitterions</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2015</creationdate><recordtype>article</recordtype><recordid>eNqFkc1v1DAQxSMEoqVw5YgsceGSxWPHX8fVblsqdRchvo6Wk9jCxYm3diK6_z0uW1aIA5xmNPq9p6d5VfUS8AIwJm_N6O2CYGBYcCkfVafACNRUCPq47A2ltZAMTqpnOd8UXkrMn1YnhDPgmNPTavq4H6dvNvuMokMGbe08JRPQxt_Zvv5igh07i9be2ZRiZ8d9QCuT2pjMaJGLCW1isN0cTEIfZjNO81Cv44RWNoRfx-U8xcFMBi13u-A7M_k45ufVE2dCti8e5ln1-eL80-pdff3-8mq1vK47DkTWhhAle-NAOmWpg1aC7BhmTjnSKoUNGEGU6kGxpmuJbKSSjlveG4NpSwk9q94cfHcp3s42T3rwuSvRSvg4Zw2CYykbwE1BX_-F3sQ5jSWdJowToIKWf_2DAsEEYIIbWajFgepSzDlZp3fJDybtNWB935q-b00fWyuCVw-2czvY_oj_rqkA6gD88MHu_2Onl9ur8z_N64PW58neHbUmfddcUMH01-2llnIj1-oCNKc_AUeisd0</recordid><startdate>20151214</startdate><enddate>20151214</enddate><creator>Christie, John A.</creator><creator>Forrest, Ryan P.</creator><creator>Corcelli, Steven A.</creator><creator>Wasio, Natalie A.</creator><creator>Quardokus, Rebecca C.</creator><creator>Brown, Ryan</creator><creator>Kandel, S. Alex</creator><creator>Lu, Yuhui</creator><creator>Lent, Craig S.</creator><creator>Henderson, Kenneth W.</creator><general>WILEY-VCH Verlag</general><general>WILEY‐VCH Verlag</general><general>Wiley Subscription Services, Inc</general><scope>BSCLL</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope></search><sort><creationdate>20151214</creationdate><title>Synthesis of a Neutral Mixed-Valence Diferrocenyl Carborane for Molecular Quantum-Dot Cellular Automata Applications</title><author>Christie, John A. ; Forrest, Ryan P. ; Corcelli, Steven A. ; Wasio, Natalie A. ; Quardokus, Rebecca C. ; Brown, Ryan ; Kandel, S. Alex ; Lu, Yuhui ; Lent, Craig S. ; Henderson, Kenneth W.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c6128-a2298daf18f9e3f1b818c505f9f2b990a1a7299d1954cb284898f6e6daa03b323</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2015</creationdate><topic>Automata theory</topic><topic>Carborane</topic><topic>carboranes</topic><topic>Cellular automata</topic><topic>Computer applications</topic><topic>Electron transfer</topic><topic>mixed-valence compounds</topic><topic>Molecular machines</topic><topic>QCA</topic><topic>Scanning tunneling microscopy</topic><topic>STM</topic><topic>Switches</topic><topic>zwitterions</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Christie, John A.</creatorcontrib><creatorcontrib>Forrest, Ryan P.</creatorcontrib><creatorcontrib>Corcelli, Steven A.</creatorcontrib><creatorcontrib>Wasio, Natalie A.</creatorcontrib><creatorcontrib>Quardokus, Rebecca C.</creatorcontrib><creatorcontrib>Brown, Ryan</creatorcontrib><creatorcontrib>Kandel, S. Alex</creatorcontrib><creatorcontrib>Lu, Yuhui</creatorcontrib><creatorcontrib>Lent, Craig S.</creatorcontrib><creatorcontrib>Henderson, Kenneth W.</creatorcontrib><collection>Istex</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Christie, John A.</au><au>Forrest, Ryan P.</au><au>Corcelli, Steven A.</au><au>Wasio, Natalie A.</au><au>Quardokus, Rebecca C.</au><au>Brown, Ryan</au><au>Kandel, S. Alex</au><au>Lu, Yuhui</au><au>Lent, Craig S.</au><au>Henderson, Kenneth W.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Synthesis of a Neutral Mixed-Valence Diferrocenyl Carborane for Molecular Quantum-Dot Cellular Automata Applications</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew. Chem. Int. Ed</addtitle><date>2015-12-14</date><risdate>2015</risdate><volume>54</volume><issue>51</issue><spage>15448</spage><epage>15451</epage><pages>15448-15451</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><coden>ACIEAY</coden><abstract>The preparation of 7‐Fc+‐8‐Fc‐7,8‐nido‐[C2B9H10]− (Fc+FcC2B9−) demonstrates the successful incorporation of a carborane cage as an internal counteranion bridging between ferrocene and ferrocenium units. This neutral mixed‐valence FeII/FeIII complex overcomes the proximal electronic bias imposed by external counterions, a practical limitation in the use of molecular switches. A combination of UV/Vis‐NIR spectroscopic and TD‐DFT computational studies indicate that electron transfer within Fc+FcC2B9− is achieved through a bridge‐mediated mechanism. This electronic framework therefore provides the possibility of an all‐neutral null state, a key requirement for the implementation of quantum‐dot cellular automata (QCA) molecular computing. The adhesion, ordering, and characterization of Fc+FcC2B9− on Au(111) has been observed by scanning tunneling microscopy.
Zwitterionic molecular switches: A neutral mixed‐valence compound has been synthesized and characterized. Spectroscopic data, in conjunction with TD‐DFT calculations, indicate a bridge‐mediated charge transfer that allows for an all‐neutral null state vital to QCA molecular switch applications.</abstract><cop>Weinheim</cop><pub>WILEY-VCH Verlag</pub><pmid>26516063</pmid><doi>10.1002/anie.201507688</doi><tpages>4</tpages><edition>International ed. in English</edition></addata></record> |
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subjects | Automata theory Carborane carboranes Cellular automata Computer applications Electron transfer mixed-valence compounds Molecular machines QCA Scanning tunneling microscopy STM Switches zwitterions |
title | Synthesis of a Neutral Mixed-Valence Diferrocenyl Carborane for Molecular Quantum-Dot Cellular Automata Applications |
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