Direct observation of collective modes coupled to molecular orbital-driven charge transfer

Tadahiko Ishikawa; Stuart A. Hayes; Sercan Keskin; Gastón Corthey; Masaki Hada; Kostyantyn Pichugin; Alexander Marx; Julian Hirscht; Kenta Shionuma; Ken Onda; Yoichi Okimoto; Shin Ya Koshihara; Takashi Yamamoto; Hengbo Cui; Mitsushiro Nomura; Yugo Oshima; Majed Abdel-Jawad; Reizo Kato; R. J. Dwayne Miller

doi:10.1126/science.aab3480

Direct observation of collective modes coupled to molecular orbital-driven charge transfer

Tadahiko Ishikawa, Stuart A. Hayes, Sercan Keskin, Gastón Corthey, Masaki Hada, Kostyantyn Pichugin, Alexander Marx, Julian Hirscht, Kenta Shionuma, Ken Onda, Yoichi Okimoto, Shin Ya Koshihara, Takashi Yamamoto, Hengbo Cui, Mitsushiro Nomura, Yugo Oshima, Majed Abdel-Jawad, Reizo Kato, R. J. Dwayne Miller

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101 Citations (Scopus)

Abstract

Correlated electron systems can undergo ultrafast photoinduced phase transitions involving concerted transformations of electronic and lattice structure. Understanding these phenomena requires identifying the key structural modes that couple to the electronic states.We report the ultrafast photoresponse of the molecular crystal Me₄P[Pt(dmit)₂]₂, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and demonstrate how femtosecond electron diffraction can be applied to directly observe the associated molecularmotions. Even for such a complex system, the key large-amplitudemodes can be identified by eye and involve a dimer expansion and a librational mode.The dynamics are consistent with the time-resolved optical study, revealing how the electronic, molecular, and lattice structures together facilitate ultrafast switching of the state.

Original language	English
Pages (from-to)	1501-1505
Number of pages	5
Journal	Science
Volume	350
Issue number	6267
DOIs	https://doi.org/10.1126/science.aab3480
Publication status	Published - Dec 18 2015
Externally published	Yes

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Ishikawa, T., Hayes, S. A., Keskin, S., Corthey, G., Hada, M., Pichugin, K., Marx, A., Hirscht, J., Shionuma, K., Onda, K., Okimoto, Y., Koshihara, S. Y., Yamamoto, T., Cui, H., Nomura, M., Oshima, Y., Abdel-Jawad, M., Kato, R., & Dwayne Miller, R. J. (2015). Direct observation of collective modes coupled to molecular orbital-driven charge transfer. Science, 350(6267), 1501-1505. https://doi.org/10.1126/science.aab3480

Ishikawa, T, Hayes, SA, Keskin, S, Corthey, G, Hada, M, Pichugin, K, Marx, A, Hirscht, J, Shionuma, K, Onda, K, Okimoto, Y, Koshihara, SY, Yamamoto, T, Cui, H, Nomura, M, Oshima, Y, Abdel-Jawad, M, Kato, R & Dwayne Miller, RJ 2015, 'Direct observation of collective modes coupled to molecular orbital-driven charge transfer', Science, vol. 350, no. 6267, pp. 1501-1505. https://doi.org/10.1126/science.aab3480

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title = "Direct observation of collective modes coupled to molecular orbital-driven charge transfer",

abstract = "Correlated electron systems can undergo ultrafast photoinduced phase transitions involving concerted transformations of electronic and lattice structure. Understanding these phenomena requires identifying the key structural modes that couple to the electronic states.We report the ultrafast photoresponse of the molecular crystal Me4P[Pt(dmit)2]2, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and demonstrate how femtosecond electron diffraction can be applied to directly observe the associated molecularmotions. Even for such a complex system, the key large-amplitudemodes can be identified by eye and involve a dimer expansion and a librational mode.The dynamics are consistent with the time-resolved optical study, revealing how the electronic, molecular, and lattice structures together facilitate ultrafast switching of the state.",

author = "Tadahiko Ishikawa and Hayes, {Stuart A.} and Sercan Keskin and Gast{\'o}n Corthey and Masaki Hada and Kostyantyn Pichugin and Alexander Marx and Julian Hirscht and Kenta Shionuma and Ken Onda and Yoichi Okimoto and Koshihara, {Shin Ya} and Takashi Yamamoto and Hengbo Cui and Mitsushiro Nomura and Yugo Oshima and Majed Abdel-Jawad and Reizo Kato and {Dwayne Miller}, {R. J.}",

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doi = "10.1126/science.aab3480",

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AU - Ishikawa, Tadahiko

AU - Hayes, Stuart A.

AU - Keskin, Sercan

AU - Corthey, Gastón

AU - Hada, Masaki

AU - Pichugin, Kostyantyn

AU - Marx, Alexander

AU - Hirscht, Julian

AU - Shionuma, Kenta

AU - Onda, Ken

AU - Okimoto, Yoichi

AU - Koshihara, Shin Ya

AU - Yamamoto, Takashi

AU - Cui, Hengbo

AU - Nomura, Mitsushiro

AU - Oshima, Yugo

AU - Abdel-Jawad, Majed

AU - Kato, Reizo

AU - Dwayne Miller, R. J.

PY - 2015/12/18

Y1 - 2015/12/18

N2 - Correlated electron systems can undergo ultrafast photoinduced phase transitions involving concerted transformations of electronic and lattice structure. Understanding these phenomena requires identifying the key structural modes that couple to the electronic states.We report the ultrafast photoresponse of the molecular crystal Me4P[Pt(dmit)2]2, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and demonstrate how femtosecond electron diffraction can be applied to directly observe the associated molecularmotions. Even for such a complex system, the key large-amplitudemodes can be identified by eye and involve a dimer expansion and a librational mode.The dynamics are consistent with the time-resolved optical study, revealing how the electronic, molecular, and lattice structures together facilitate ultrafast switching of the state.

AB - Correlated electron systems can undergo ultrafast photoinduced phase transitions involving concerted transformations of electronic and lattice structure. Understanding these phenomena requires identifying the key structural modes that couple to the electronic states.We report the ultrafast photoresponse of the molecular crystal Me4P[Pt(dmit)2]2, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and demonstrate how femtosecond electron diffraction can be applied to directly observe the associated molecularmotions. Even for such a complex system, the key large-amplitudemodes can be identified by eye and involve a dimer expansion and a librational mode.The dynamics are consistent with the time-resolved optical study, revealing how the electronic, molecular, and lattice structures together facilitate ultrafast switching of the state.

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Direct observation of collective modes coupled to molecular orbital-driven charge transfer

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