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DOI | 10.1088/1748-9326/aa568e |
A low-spin Fe(III) complex with 100-ps ligand-to-metal charge transfer photoluminescence | |
Chabera, Pavel1; Liu, Yizhu2; Prakash, Om2; Thyrhaug, Erling1; El Nahhas, Amal1; Honarfar, Alireza1; Essen, Sofia2; Fredin, Lisa A.3; Harlang, Tobias C. B.1,4; Kjaer, Kasper S.1,4; Handrup, Karsten5; Ericson, Fredric3; Tatsuno, Hideyuki1; Morgan, Kelsey6; Schnadt, Joachim5; Haggstrom, Lennart7; Ericsson, Tore7; Sobkowiak, Adam7; Lidin, Sven2; Huang, Ping8; Styring, Stenbjorn8; Uhlig, Jens1; Bendix, Jesper9; Lomoth, Reiner8; Sundstrom, Villy1; Persson, Petter3; Warnmark, Kenneth2 | |
2017-03-30 | |
发表期刊 | NATURE
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ISSN | 0028-0836 |
EISSN | 1476-4687 |
出版年 | 2017 |
卷号 | 543期号:7647页码:695-+ |
文章类型 | Article |
语种 | 英语 |
国家 | Sweden; Denmark; USA |
英文摘要 | Transition-metal complexes are used as photosensitizers(1), in light-emitting diodes, for biosensing and in photocatalysis(2). A key feature in these applications is excitation from the ground state to a charge-transfer state(3,4); the long charge-transfer-state lifetimes typical for complexes of ruthenium(5) and other precious metals are often essential to ensure high performance. There is much interest in replacing these scarce elements with Earth-abundant metals, with iron(6) and copper(7) being particularly attractive owing to their low cost and non-toxicity. But despite the exploration of innovative molecular designs(6,8-10), it remains a formidable scientific challenge(11) to access Earth-abundant transition-metal complexes with long-lived charge-transfer excited states. No known iron complexes are considered(12) photoluminescent at room temperature, and their rapid excited-state deactivation precludes their use as photosensitizers(13-15). Here we present the iron complex [Fe(btz)(3)](3+) (where btz is 3,3'-dimethyl-1,1'-bis(p-tolyl)-4,4'-bis(1,2,3-triazol-5-ylidene)), and show that the superior sigma-donor and pi-acceptor electron properties of the ligand stabilize the excited state sufficiently to realize a long charge-transfer lifetime of 100 picoseconds (ps) and room-temperature photoluminescence. This species is a low-spin Fe(III) d(5) complex, and emission occurs from a long-lived doublet ligand-to-metal charge-transfer ((LMCT)-L-2) state that is rarely seen for transition-metal complexes(4,16,17). The absence of intersystem crossing, which often gives rise to large excited-state energy losses in transition-metal complexes, enables the observation of spin-allowed emission directly to the ground state and could be exploited as an increased driving force in photochemical reactions on surfaces. These findings suggest that appropriate design strategies can deliver new iron-based materials for use as light emitters and photosensitizers. |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000397619700051 |
WOS关键词 | EXCITED-STATES ; IRON(II) ; LIFETIME ; LIGHT ; PHOTOSENSITIZER ; ABSORPTION ; DYNAMICS ; SET ; ROW |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/37559 |
专题 | 气候变化 |
作者单位 | 1.Lund Univ, Dept Chem, Div Phys Chem, Box 124, SE-22100 Lund, Sweden; 2.Lund Univ, Dept Chem, CAS, Box 124, SE-22100 Lund, Sweden; 3.Lund Univ, Dept Chem, Div Theoret Chem, Box 124, SE-22100 Lund, Sweden; 4.Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark; 5.Lund Univ, Dept Phys, Div Synchrotron Radiat Res, Box 118, SE-22100 Lund, Sweden; 6.NIST, Boulder, CO 80305 USA; 7.Uppsala Univ, Dept Chem, Angstrom Lab, Box 538, SE-75121 Uppsala, Sweden; 8.Uppsala Univ, Dept Chem, Angstrom Lab, Box 523, SE-75120 Uppsala, Sweden; 9.Univ Copenhagen, Dept Chem, Univ Pk 5, DK-2100 Copenhagen, Denmark |
推荐引用方式 GB/T 7714 | Chabera, Pavel,Liu, Yizhu,Prakash, Om,et al. A low-spin Fe(III) complex with 100-ps ligand-to-metal charge transfer photoluminescence[J]. NATURE,2017,543(7647):695-+. |
APA | Chabera, Pavel.,Liu, Yizhu.,Prakash, Om.,Thyrhaug, Erling.,El Nahhas, Amal.,...&Warnmark, Kenneth.(2017).A low-spin Fe(III) complex with 100-ps ligand-to-metal charge transfer photoluminescence.NATURE,543(7647),695-+. |
MLA | Chabera, Pavel,et al."A low-spin Fe(III) complex with 100-ps ligand-to-metal charge transfer photoluminescence".NATURE 543.7647(2017):695-+. |
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