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Bonding, Luminescence, Metallophilicity in Linear Au3 and Au2Ag Chains Stabilized by Rigid Diphosphanyl NHC Ligands

The heterofunctional and rigid ligand N,N′-diphosphanyl-imidazol-2-ylidene (PC NHC P; P = P­(t-Bu)2), through its phosphorus and two N-heterocyclic carbene (NHC) donors, stabilizes trinuclear chain complexes, with either Au3 or AgAu2 cores, and dinuclear Au2 complexes. The two oppositely situated PC...

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Published in:Inorganic chemistry 2016-09, Vol.55 (17), p.8527-8542
Main Authors: Ai, Pengfei, Mauro, Matteo, Gourlaouen, Christophe, Carrara, Serena, De Cola, Luisa, Tobon, Yeny, Giovanella, Umberto, Botta, Chiara, Danopoulos, Andreas A, Braunstein, Pierre
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container_title Inorganic chemistry
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creator Ai, Pengfei
Mauro, Matteo
Gourlaouen, Christophe
Carrara, Serena
De Cola, Luisa
Tobon, Yeny
Giovanella, Umberto
Botta, Chiara
Danopoulos, Andreas A
Braunstein, Pierre
description The heterofunctional and rigid ligand N,N′-diphosphanyl-imidazol-2-ylidene (PC NHC P; P = P­(t-Bu)2), through its phosphorus and two N-heterocyclic carbene (NHC) donors, stabilizes trinuclear chain complexes, with either Au3 or AgAu2 cores, and dinuclear Au2 complexes. The two oppositely situated PC NHC P (L) ligands that “sandwich” the metal chain can support linear and rigid structures, as found in the known tricationic Au­(I) complex [Au3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 (OTf = CF3SO3; [Au3 L 2]­(OTf)3; Chem. Commun. 2014, 50, 103–105) now also obtained by transmetalation from [Ag3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Ag3 L 2]­(OTf)3), or in the mixed-metal tricationic [Au2Ag­(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Au2AgL 2]­(OTf)3). The latter was obtained stepwise by the addition of AgOTf to the digold­(I) complex [Au2(μ2-PC NHC P,κP,κC NHC)2]­(OTf)2 ([Au2 L 2 ]­(OTf)2). The latter contains two dangling P donors and displays fluxional behavior in solution, and the Au···Au separation of 2.8320(6) Å in the solid state is consistent with metallophilic interactions. In the solvento complex [Au3Cl2(tht)­(μ3-PC NHC P,κP,κC NHC,κP)]­(OTf)·MeCN ([Au3Cl2(tht)L]­(OTf)·MeCN), which contains only one L and one tht ligand (tht = tetrahydrothiophene), the metal chain is bent (148.94(2)°), and the longer Au···Au separation (2.9710(4) Å) is in line with relaxation of the rigidity due to a more “open” structure. Similar features were observed in [Au3Cl2(SMe2)L]­(OTf)·2MeCN. A detailed study of the emission properties of [Au3 L 2]­(OTf)3, [Au3Cl2(tht)L]­(OTf)·MeCN, [Au2 L 2]­(OTf)2, and [Au2AgL 2]­(OTf)3 was performed by means of steady state and time-resolved photophysical techniques. The complex [Au3 L 2]­(OTf)3 displays a bright (photoluminescence quantum yield = 80%) and narrow emission band centered at 446 nm with a relatively small Stokes’ shift and long-lived excited-state lifetime on the microsecond timescale, both in solution and in the solid state. In line with the very narrow emission profile centered in the violet-blue region, fabrication of organic light-emitting devices (OLEDs) comprising the [Au3 L 2]­(OTf)3 complex demonstrated its usefulness as a deep-blue emitter in solution-processed OLEDs. Electrochemical and Raman spectroscopic studies were also performed on [Au3 L 2]­(OTf)3. Experimental results were rationalized by means of Wave-Function Theory (WFT) and Density Functional Theory (DFT). MP2 calculations gave a satisfactory description of the stru
doi_str_mv 10.1021/acs.inorgchem.6b01095
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The two oppositely situated PC NHC P (L) ligands that “sandwich” the metal chain can support linear and rigid structures, as found in the known tricationic Au­(I) complex [Au3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 (OTf = CF3SO3; [Au3 L 2]­(OTf)3; Chem. Commun. 2014, 50, 103–105) now also obtained by transmetalation from [Ag3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Ag3 L 2]­(OTf)3), or in the mixed-metal tricationic [Au2Ag­(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Au2AgL 2]­(OTf)3). The latter was obtained stepwise by the addition of AgOTf to the digold­(I) complex [Au2(μ2-PC NHC P,κP,κC NHC)2]­(OTf)2 ([Au2 L 2 ]­(OTf)2). The latter contains two dangling P donors and displays fluxional behavior in solution, and the Au···Au separation of 2.8320(6) Å in the solid state is consistent with metallophilic interactions. In the solvento complex [Au3Cl2(tht)­(μ3-PC NHC P,κP,κC NHC,κP)]­(OTf)·MeCN ([Au3Cl2(tht)L]­(OTf)·MeCN), which contains only one L and one tht ligand (tht = tetrahydrothiophene), the metal chain is bent (148.94(2)°), and the longer Au···Au separation (2.9710(4) Å) is in line with relaxation of the rigidity due to a more “open” structure. Similar features were observed in [Au3Cl2(SMe2)L]­(OTf)·2MeCN. A detailed study of the emission properties of [Au3 L 2]­(OTf)3, [Au3Cl2(tht)L]­(OTf)·MeCN, [Au2 L 2]­(OTf)2, and [Au2AgL 2]­(OTf)3 was performed by means of steady state and time-resolved photophysical techniques. The complex [Au3 L 2]­(OTf)3 displays a bright (photoluminescence quantum yield = 80%) and narrow emission band centered at 446 nm with a relatively small Stokes’ shift and long-lived excited-state lifetime on the microsecond timescale, both in solution and in the solid state. In line with the very narrow emission profile centered in the violet-blue region, fabrication of organic light-emitting devices (OLEDs) comprising the [Au3 L 2]­(OTf)3 complex demonstrated its usefulness as a deep-blue emitter in solution-processed OLEDs. Electrochemical and Raman spectroscopic studies were also performed on [Au3 L 2]­(OTf)3. Experimental results were rationalized by means of Wave-Function Theory (WFT) and Density Functional Theory (DFT). MP2 calculations gave a satisfactory description of the structures of the cationic complexes [Au 3 L 2]3+ and [Au2 L 2]2+ and pointed to Au···Au interactions having an electrostatic component owing to the dissimilar charge distribution in the chain caused by the heterofunctional ligand. The nature of the emitting states and their geometric distortions relative to the ground states in [Au3 L 2]3+ and [Au2 L 2]2+ was studied by DFT, revealing contraction of the Au···Au distances and coordination geometry changes by association of the dangling P donor, respectively.</description><identifier>ISSN: 0020-1669</identifier><identifier>EISSN: 1520-510X</identifier><identifier>DOI: 10.1021/acs.inorgchem.6b01095</identifier><identifier>PMID: 27494635</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Chemical Sciences ; or physical chemistry ; Theoretical and</subject><ispartof>Inorganic chemistry, 2016-09, Vol.55 (17), p.8527-8542</ispartof><rights>Copyright © 2016 American Chemical Society</rights><rights>Distributed under a Creative Commons Attribution 4.0 International License</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-2409-2849</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,780,784,885,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/27494635$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://hal.science/hal-01389172$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Ai, Pengfei</creatorcontrib><creatorcontrib>Mauro, Matteo</creatorcontrib><creatorcontrib>Gourlaouen, Christophe</creatorcontrib><creatorcontrib>Carrara, Serena</creatorcontrib><creatorcontrib>De Cola, Luisa</creatorcontrib><creatorcontrib>Tobon, Yeny</creatorcontrib><creatorcontrib>Giovanella, Umberto</creatorcontrib><creatorcontrib>Botta, Chiara</creatorcontrib><creatorcontrib>Danopoulos, Andreas A</creatorcontrib><creatorcontrib>Braunstein, Pierre</creatorcontrib><title>Bonding, Luminescence, Metallophilicity in Linear Au3 and Au2Ag Chains Stabilized by Rigid Diphosphanyl NHC Ligands</title><title>Inorganic chemistry</title><addtitle>Inorg. Chem</addtitle><description>The heterofunctional and rigid ligand N,N′-diphosphanyl-imidazol-2-ylidene (PC NHC P; P = P­(t-Bu)2), through its phosphorus and two N-heterocyclic carbene (NHC) donors, stabilizes trinuclear chain complexes, with either Au3 or AgAu2 cores, and dinuclear Au2 complexes. The two oppositely situated PC NHC P (L) ligands that “sandwich” the metal chain can support linear and rigid structures, as found in the known tricationic Au­(I) complex [Au3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 (OTf = CF3SO3; [Au3 L 2]­(OTf)3; Chem. Commun. 2014, 50, 103–105) now also obtained by transmetalation from [Ag3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Ag3 L 2]­(OTf)3), or in the mixed-metal tricationic [Au2Ag­(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Au2AgL 2]­(OTf)3). The latter was obtained stepwise by the addition of AgOTf to the digold­(I) complex [Au2(μ2-PC NHC P,κP,κC NHC)2]­(OTf)2 ([Au2 L 2 ]­(OTf)2). The latter contains two dangling P donors and displays fluxional behavior in solution, and the Au···Au separation of 2.8320(6) Å in the solid state is consistent with metallophilic interactions. In the solvento complex [Au3Cl2(tht)­(μ3-PC NHC P,κP,κC NHC,κP)]­(OTf)·MeCN ([Au3Cl2(tht)L]­(OTf)·MeCN), which contains only one L and one tht ligand (tht = tetrahydrothiophene), the metal chain is bent (148.94(2)°), and the longer Au···Au separation (2.9710(4) Å) is in line with relaxation of the rigidity due to a more “open” structure. Similar features were observed in [Au3Cl2(SMe2)L]­(OTf)·2MeCN. A detailed study of the emission properties of [Au3 L 2]­(OTf)3, [Au3Cl2(tht)L]­(OTf)·MeCN, [Au2 L 2]­(OTf)2, and [Au2AgL 2]­(OTf)3 was performed by means of steady state and time-resolved photophysical techniques. The complex [Au3 L 2]­(OTf)3 displays a bright (photoluminescence quantum yield = 80%) and narrow emission band centered at 446 nm with a relatively small Stokes’ shift and long-lived excited-state lifetime on the microsecond timescale, both in solution and in the solid state. In line with the very narrow emission profile centered in the violet-blue region, fabrication of organic light-emitting devices (OLEDs) comprising the [Au3 L 2]­(OTf)3 complex demonstrated its usefulness as a deep-blue emitter in solution-processed OLEDs. Electrochemical and Raman spectroscopic studies were also performed on [Au3 L 2]­(OTf)3. Experimental results were rationalized by means of Wave-Function Theory (WFT) and Density Functional Theory (DFT). MP2 calculations gave a satisfactory description of the structures of the cationic complexes [Au 3 L 2]3+ and [Au2 L 2]2+ and pointed to Au···Au interactions having an electrostatic component owing to the dissimilar charge distribution in the chain caused by the heterofunctional ligand. The nature of the emitting states and their geometric distortions relative to the ground states in [Au3 L 2]3+ and [Au2 L 2]2+ was studied by DFT, revealing contraction of the Au···Au distances and coordination geometry changes by association of the dangling P donor, respectively.</description><subject>Chemical Sciences</subject><subject>or physical chemistry</subject><subject>Theoretical and</subject><issn>0020-1669</issn><issn>1520-510X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNo9kd1u1DAQhS1ERbeFRwD5EqTuMmMntnO5bAuLlILEj8Sd5SRO4ipx0jiptDw9Xu3SqxnNfHOkOYeQtwgbBIYfTRk2zg9TU7a234gCELL0BVlhymCdIvx5SVYAsUchsktyFcIDAGQ8Ea_IJZNJlgierkj4NPjK-eaG5kvvvA2l9aW9ofd2Nl03jK3rXOnmA3We5nFvJrpdODW-ipVtG7prjfOB_pxNEdG_tqLFgf5wjavorRvbIYyt8YeOftvvokATD8NrclGbLtg353pNfn---7Xbr_PvX77utvnaMKHmdV2YJOOyTEBVtQGFdS2FSm1WYMJBKMYtmgoUM5ktJRc2KayULElRFRK44Nfkw0m3NZ0eJ9eb6aAH4_R-m-vjDJCrDCV7wsi-P7HjNDwuNsy6d9GLrjPeDkvQqFCmqZJMRfTdGV2K3lbPyv9NjQCegJiRfhiWyccvNYI-BqePw-fg9Dk4_g_DA4sk</recordid><startdate>20160906</startdate><enddate>20160906</enddate><creator>Ai, Pengfei</creator><creator>Mauro, Matteo</creator><creator>Gourlaouen, Christophe</creator><creator>Carrara, Serena</creator><creator>De Cola, Luisa</creator><creator>Tobon, Yeny</creator><creator>Giovanella, Umberto</creator><creator>Botta, Chiara</creator><creator>Danopoulos, Andreas A</creator><creator>Braunstein, Pierre</creator><general>American Chemical Society</general><scope>NPM</scope><scope>7X8</scope><scope>1XC</scope><orcidid>https://orcid.org/0000-0002-2409-2849</orcidid></search><sort><creationdate>20160906</creationdate><title>Bonding, Luminescence, Metallophilicity in Linear Au3 and Au2Ag Chains Stabilized by Rigid Diphosphanyl NHC Ligands</title><author>Ai, Pengfei ; Mauro, Matteo ; Gourlaouen, Christophe ; Carrara, Serena ; De Cola, Luisa ; Tobon, Yeny ; Giovanella, Umberto ; Botta, Chiara ; Danopoulos, Andreas A ; Braunstein, Pierre</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a268t-fba4937c408dfa081ff7685e9b14306823e1ad082a9ec736e4be7724518b70363</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Chemical Sciences</topic><topic>or physical chemistry</topic><topic>Theoretical and</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ai, Pengfei</creatorcontrib><creatorcontrib>Mauro, Matteo</creatorcontrib><creatorcontrib>Gourlaouen, Christophe</creatorcontrib><creatorcontrib>Carrara, Serena</creatorcontrib><creatorcontrib>De Cola, Luisa</creatorcontrib><creatorcontrib>Tobon, Yeny</creatorcontrib><creatorcontrib>Giovanella, Umberto</creatorcontrib><creatorcontrib>Botta, Chiara</creatorcontrib><creatorcontrib>Danopoulos, Andreas A</creatorcontrib><creatorcontrib>Braunstein, Pierre</creatorcontrib><collection>PubMed</collection><collection>MEDLINE - Academic</collection><collection>Hyper Article en Ligne (HAL)</collection><jtitle>Inorganic chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ai, Pengfei</au><au>Mauro, Matteo</au><au>Gourlaouen, Christophe</au><au>Carrara, Serena</au><au>De Cola, Luisa</au><au>Tobon, Yeny</au><au>Giovanella, Umberto</au><au>Botta, Chiara</au><au>Danopoulos, Andreas A</au><au>Braunstein, Pierre</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Bonding, Luminescence, Metallophilicity in Linear Au3 and Au2Ag Chains Stabilized by Rigid Diphosphanyl NHC Ligands</atitle><jtitle>Inorganic chemistry</jtitle><addtitle>Inorg. Chem</addtitle><date>2016-09-06</date><risdate>2016</risdate><volume>55</volume><issue>17</issue><spage>8527</spage><epage>8542</epage><pages>8527-8542</pages><issn>0020-1669</issn><eissn>1520-510X</eissn><abstract>The heterofunctional and rigid ligand N,N′-diphosphanyl-imidazol-2-ylidene (PC NHC P; P = P­(t-Bu)2), through its phosphorus and two N-heterocyclic carbene (NHC) donors, stabilizes trinuclear chain complexes, with either Au3 or AgAu2 cores, and dinuclear Au2 complexes. The two oppositely situated PC NHC P (L) ligands that “sandwich” the metal chain can support linear and rigid structures, as found in the known tricationic Au­(I) complex [Au3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 (OTf = CF3SO3; [Au3 L 2]­(OTf)3; Chem. Commun. 2014, 50, 103–105) now also obtained by transmetalation from [Ag3(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Ag3 L 2]­(OTf)3), or in the mixed-metal tricationic [Au2Ag­(μ3-PC NHC P,κP,κC NHC,κP)2]­(OTf)3 ([Au2AgL 2]­(OTf)3). The latter was obtained stepwise by the addition of AgOTf to the digold­(I) complex [Au2(μ2-PC NHC P,κP,κC NHC)2]­(OTf)2 ([Au2 L 2 ]­(OTf)2). The latter contains two dangling P donors and displays fluxional behavior in solution, and the Au···Au separation of 2.8320(6) Å in the solid state is consistent with metallophilic interactions. In the solvento complex [Au3Cl2(tht)­(μ3-PC NHC P,κP,κC NHC,κP)]­(OTf)·MeCN ([Au3Cl2(tht)L]­(OTf)·MeCN), which contains only one L and one tht ligand (tht = tetrahydrothiophene), the metal chain is bent (148.94(2)°), and the longer Au···Au separation (2.9710(4) Å) is in line with relaxation of the rigidity due to a more “open” structure. Similar features were observed in [Au3Cl2(SMe2)L]­(OTf)·2MeCN. A detailed study of the emission properties of [Au3 L 2]­(OTf)3, [Au3Cl2(tht)L]­(OTf)·MeCN, [Au2 L 2]­(OTf)2, and [Au2AgL 2]­(OTf)3 was performed by means of steady state and time-resolved photophysical techniques. The complex [Au3 L 2]­(OTf)3 displays a bright (photoluminescence quantum yield = 80%) and narrow emission band centered at 446 nm with a relatively small Stokes’ shift and long-lived excited-state lifetime on the microsecond timescale, both in solution and in the solid state. In line with the very narrow emission profile centered in the violet-blue region, fabrication of organic light-emitting devices (OLEDs) comprising the [Au3 L 2]­(OTf)3 complex demonstrated its usefulness as a deep-blue emitter in solution-processed OLEDs. Electrochemical and Raman spectroscopic studies were also performed on [Au3 L 2]­(OTf)3. Experimental results were rationalized by means of Wave-Function Theory (WFT) and Density Functional Theory (DFT). MP2 calculations gave a satisfactory description of the structures of the cationic complexes [Au 3 L 2]3+ and [Au2 L 2]2+ and pointed to Au···Au interactions having an electrostatic component owing to the dissimilar charge distribution in the chain caused by the heterofunctional ligand. The nature of the emitting states and their geometric distortions relative to the ground states in [Au3 L 2]3+ and [Au2 L 2]2+ was studied by DFT, revealing contraction of the Au···Au distances and coordination geometry changes by association of the dangling P donor, respectively.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>27494635</pmid><doi>10.1021/acs.inorgchem.6b01095</doi><tpages>16</tpages><orcidid>https://orcid.org/0000-0002-2409-2849</orcidid></addata></record>
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title Bonding, Luminescence, Metallophilicity in Linear Au3 and Au2Ag Chains Stabilized by Rigid Diphosphanyl NHC Ligands
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