GSTDTAP  > 气候变化
DOI10.1088/1748-9326/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
ISSN0028-0836
EISSN1476-4687
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
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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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