Photosalient 7 図 Å 2 HOMO 5d z 2 図 2 HOMO dσ dσ* 図 2 HOMO dσ* 図 2 HOMO 7 HOMO 1 図 2 8 Au CN nm 2.0 ns 図 3 Au CN 2 3 図 2 Schematic repr
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- ふじきみ ゆのもと
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1 最近の研究から 金属間相互作用の増強が鍵となる光誘起結晶相転移と Photosalient 効果 Tomohiro SEKI and Hajime ITO: Photoinduced Crystalline Structure Change and Photosalient Effect through Strengthening Metallophilic Interaction We report the first photoinduced single-crystal-to-single-crystal SCSC phase transition of a gold complex 1 that involves strengthening of intermolecular aurophilic interactions. This is also the first solid state photochromism of gold complexes. Upon UV irradiation, blue-emitting crystals 1B of aryl gold I isocyanide complex 1 transform into the weakly yellow-emitting crystals 1Y. X-ray diffraction analyses exhibit that the phase transition proceeds in an SCSC manner. After phase transition from 1B to 1Y, the intermolecular Au Au separation decreases from to Å, resulting in a red-shifted emission. The photoinduced strengthening of the aurophilic interactions in the excited state initiates the change in the crystal structure from 1B to 1Y. Moreover, crystal 1B showed a photosalient effect: the 1B crystals jump upon irradiation with strong UV light owing to the phase transition into 1Y. The photoinduced strengthening of aurophilic interactions in the crystal generate the sudden mechanical movement of the crystal. 1. はじめに 1 1 Nature 図 1 2 図 1 Photochromism of the crystal of diarylethene derivative. 365 nm 金原子間相互作用とその光応答特性
2 Photosalient 7 図 Å 2 HOMO 5d z 2 図 2 HOMO dσ dσ* 図 2 HOMO dσ* 図 2 HOMO 7 HOMO 1 図 2 8 Au CN nm 2.0 ns 図 3 Au CN 2 3 図 2 Schematic representation of aurophilic bonds and their simplified orbital levels. dσ dσ* dσ* HOMO 1 Au CN Au CN I 1 図 4 図 3 Au CN 2 3 Schematic representation of the relaxation pathway upon photoirradiation of Au CN 2 3 complexes 図 Structures of
3 3. 金イソシアニド錯体 1の光誘起結晶相転移 3.1 アリール金イソシアニド錯体 Photosalient 3.2 金イソシアニド錯体 1の紫外光照射に伴う結晶相転移 1 1B 図 5 1B Φ em nm 図 6 λ em,max 448 nm 450 nm 371 nm 400 nm 1B X _ P1 R wr GOF a Å b Å c Å α β γ Z 4 V Å 3 d g cm 3 図 7 1B R 1 wr 2 X 1Y X 1 H NMR 図 6 1B 1Y Excitation and emission spectra of 1B and 1Y. 1B 450 nm 1Y 590 nm 1B 370 nm 1Y 390 nm Inset 1Y. τ av 34.2 μs 590 nm 1B 図 5 1B 1Y A series of photographs of the SCSC phase transition from 1B to 1Y induced by strong photoirradiation 367 nm, approx. 100 mw cm 2 taken under excitation at 365 nm. 図 7 1B The single-crystal structure of 1B. a ORTEP b ORTEP c CPK ORTEP
4 Photosalient Head-to-tail Å 1B 1Y 図 nm 100 mw cm 2 60 s 1B 図 5 1Y 5 mw cm 2 1B 10 1Y Φ em 0.5 λ em, max 580 nm 図 6 1B 132 nm 図 6 23 nm580 nm τ av μs 1B τ av 50 1Y X 1B 1B 1Y X 1B 1Y _ 1Y P1 R wr GOF a Å b Å c Å α β γ Z 2 V Å 3 d g cm 3 図 8 1 H NMR 1Y Head-to-tail 1B B 1Y 2 1Y 図 8 1Y The single-crystal structure of 1Y. a ORTEP b ORTEP c CPK ORTEP Å 1B 0.2 Å 3.3 励起状態における金原子間相互作用の増強を利用した光誘起結晶相転移 1 1B 1Y 1B 1B 1Y 1B 1Y 120 DSC B 1Y nm 200 mw cm 2 1B 1B 1Y 1B 1B 1Y 229
5 1B DFT PBEPBE/ SDD 1B 図 9 HOMO 図 2 1B 1B 1B 3 1T Opt 1B 1T Opt 図 9 Head-to-tail 2.86 Å 1B 3 図 2 HOMO 1T Opt 1Y 図 9 1B 1B 1Y 1B 1Y 3.4 Photosalient 効果 1 Photosalient Salient 図 Salient Thermosalient Photosalient Salient Photosalient 1 Photosalient mw cm nm Photosalient 図 mw cm 2 図 10 Salient Schematic representation of salient effect. 図 9 1B 1T Opt 1Y Comparison of the structures and frontier orbital levels and the corresponding molecular orbitals of 1B, 1T Opt, and 1Y. 図 11 1 Photosalient A series of photographs of the photosalient effect of 1B through the transformation into 1Y induced by strong photoirradiation 367 nm, approx. 400 mw cm 2. d
6 Photosalient 1B 5 図 11a b 1B 1Y 図 11c 21 図 11d 1 1B Photosalient 1B Salient 16 1 Photosalient Photosalient Photosalient1 Salient 1 Photosalient 1B 1Y Salient Naumov Salient 16 Salient Thermosalient X Salient Salient 1 V/Z Δ V/Z Δ V/Z 25 Å 3 1 Naumov Salient _ P1 Δ V/Z 6.8 Å Photosalient Naumov Salient 1 4. おわりに 1 1B Photosalient 1 Photosalient 5 文献 1 a J. Zhang, Q. Zou and H. Tian: Adv. Mater. 25, ; b M. Irie, T. Fukaminato, K. Matsuda and S. Kobatake: Chem. Rev. 114, S. Kobatake, S. Takami, H. Muto, T. Ishikawa and M. Irie: Nature 446, O. S. Bushuyev, A. Tomberg, T. Friscic and C. J. Barrett: J. Am. Chem. Soc. 135, J. W. Chung, S.-J. Yoon, B.-K. An and S. Y. Park: J. Phys. Chem. C 117, S. Iyengar and M. C. Biewer: Cryst. Growth Des. 5, N. K. Nath, L. Pejov, S. M. Nichols, C. Hu, N. Saleh, B. Kahr and P. Naumov: J. Am. Chem. Soc. 136, a A. L. Balch: Gold Bull. 37, ; b P. Pyykko: Angew. Chem., Int. Ed. 43, ; c V. W. Yam and E. C. Cheng: Chem. Soc. Rev. 37, a G. Cui, X. Y. Cao, W. H. Fang, M. Dolg and W. Thiel: Angew. Chem., Int. Ed. 52, ; b H. H. Patterson, S. M. Kanan and M. A. Omary: Coord. Chem. Rev. 208, a M. Iwamura, K. Nozaki, S. Takeuchi and T. Tahara, J. Am. Chem. Soc. 135, ; b K. H. Kim, J. G. Kim, S. Nozawa, T. Sato, K. Y. Oang, T. W. Kim, H. Ki, J. Jo, S. Park and C. Song: Nature 518, a K. Haldrup, T. Harlang, M. Christensen, A. Dohn, T. B. van Driel, K. S. Kjaer, N. Harrit, J. Vibenholt, L. Guerin, M. Wulff and M. M. Nielsen: Inorg. Chem. 50, ; b R. M. van der Veen, C. J. Milne, A. El Nahhas, F. A. Lima, V. T. Pham, J. Best, J. A. Weinstein, C. N. Borca, R. Abela, C. Bressler and M. Chergui: Angew. Chem., Int. Ed. 48, H. Ito, T. Saito, N. Oshima, N. Kitamura, S. Ishizaka, Y. Hinatsu, 231
7 M. Wakeshima, M. Kato, K. Tsuge and M. Sawamura: J. Am. Chem. Soc. 130, a Y. Sagara and T. Kato: Nat. Chem. 1, ; b A. L. Balch: Angew. Chem. Int. Ed. 48, ; c C. Jobbágy and A. Deák, Eur. J. Inorg. Chem. 2014, a K. Kawaguchi, T. Seki, T. Karatsu, A. Kitamura, H. Ito and S. Yagai: Chem. Commun. 49, ; b T. Seki, T. Ozaki, T. Okura, K. Asakura, A. Sakon, H. Uekusa and H. Ito: Chem. Sci. 6, a T. Seki, K. Sakurada and H. Ito: Angew. Chem., Int. Ed. v52, ; b H. Ito, M. Muromoto, S. Kurenuma, S. Ishizaka, N. Kitamura, H. Sato and T. Seki: Nat. Commun. 4, T. Seki, K. Sakurada, M. Muromoto and H. Ito: Chem. Sci. 6, a N. K. Nath, M. K. Panda, S. C. Sahoo and P. Naumov: CrystEngComm 16, ; b S. C. Sahoo, M. K. Panda, N. K. Nath and P. Naumov: J. Am. Chem. Soc. 135, a M. C. Etter and A. R. Siedle: J. Am. Chem. Soc. 105, ; b I. Colombier, S. Spagnoli, A. Corval, P. Baldeck, M. Giraud, A. Léaustic and P. Yu: Mol. Cryst. Liq. Cryst. 431, プロフィール Tomohiro SEKI Faculty of Engineering, Frontier Chemistry Center, Hokkaido University Kita 13 Nishi 8 Kita-ku, Sapporo, Hokkaido , Japan seki@eng.hokudai.ac.jp Hajime ITO Faculty of Engineering, Frontier Chemistry Center, Hokkaido University Kita 13 Nishi 8 Kita-ku, Sapporo, Hokkaido , Japan hajito@eng.hokudai.ac.jp
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