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

Research output: Contribution to journalArticle

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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 languageEnglish
Pages (from-to)1501-1505
Number of pages5
JournalScience
Volume350
Issue number6267
DOIs
Publication statusPublished - Dec 18 2015
Externally publishedYes

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coupled modes
molecular orbitals
charge transfer
electronic structure
complex systems
molecular structure
electron diffraction
dimers
expansion
electronics
crystals
electrons

ASJC Scopus subject areas

  • General

Cite this

Ishikawa, T., Hayes, S. A., Keskin, S., Corthey, G., Hada, M., Pichugin, K., ... 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

Direct observation of collective modes coupled to molecular orbital-driven charge transfer. / Ishikawa, Tadahiko; Hayes, Stuart A.; Keskin, Sercan; Corthey, Gastón; Hada, Masaki; Pichugin, Kostyantyn; Marx, Alexander; Hirscht, Julian; Shionuma, Kenta; Onda, Ken; Okimoto, Yoichi; Koshihara, Shin Ya; Yamamoto, Takashi; Cui, Hengbo; Nomura, Mitsushiro; Oshima, Yugo; Abdel-Jawad, Majed; Kato, Reizo; Dwayne Miller, R. J.

In: Science, Vol. 350, No. 6267, 18.12.2015, p. 1501-1505.

Research output: Contribution to journalArticle

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
Ishikawa T, Hayes SA, Keskin S, Corthey G, Hada M, Pichugin K et al. Direct observation of collective modes coupled to molecular orbital-driven charge transfer. Science. 2015 Dec 18;350(6267):1501-1505. https://doi.org/10.1126/science.aab3480
Ishikawa, Tadahiko ; Hayes, Stuart A. ; Keskin, Sercan ; Corthey, Gastón ; Hada, Masaki ; Pichugin, Kostyantyn ; Marx, Alexander ; Hirscht, Julian ; Shionuma, Kenta ; Onda, Ken ; Okimoto, Yoichi ; Koshihara, Shin Ya ; Yamamoto, Takashi ; Cui, Hengbo ; Nomura, Mitsushiro ; Oshima, Yugo ; Abdel-Jawad, Majed ; Kato, Reizo ; Dwayne Miller, R. J. / Direct observation of collective modes coupled to molecular orbital-driven charge transfer. In: Science. 2015 ; Vol. 350, No. 6267. pp. 1501-1505.
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AU - Ishikawa, Tadahiko

AU - Hayes, Stuart A.

AU - Keskin, Sercan

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AU - Hada, Masaki

AU - Pichugin, Kostyantyn

AU - Marx, Alexander

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AU - Yamamoto, Takashi

AU - Cui, Hengbo

AU - Nomura, Mitsushiro

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AU - Abdel-Jawad, Majed

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AU - Dwayne Miller, R. J.

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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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