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

作者:Ishikawa Tadahiko; Hayes Stuart A; Keskin Sercan; Corthey Gaston; 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; Miller R J Dwayne
来源:Science, 2015, 350(6267): 1501-1505.
DOI:10.1126/science.aab3480

摘要

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 molecular motions. Even for such a complex system, the key large-amplitude modes 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.

  • 出版日期2015-12-18