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Ultrafast Pathways of the Photoinduced Insulator–Metal Transition in a Low‐Dimensional Organic Conductor
Author(s) -
Smit Bart,
Hüwe Florian,
Payne Nancy,
Olaoye Olufemi,
Bauer Irene,
Pflaum Jens,
Schwoerer Markus,
Schwoerer Heinrich
Publication year - 2019
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201900652
Subject(s) - materials science , ultrafast electron diffraction , peierls transition , phase transition , chemical physics , photoinduced electron transfer , electron , responsivity , electron transfer , condensed matter physics , ultrashort pulse , molecular physics , optoelectronics , laser , optics , photochemistry , chemistry , physics , quantum mechanics , photodetector
Among functional organic materials, low‐dimensional molecular crystals represent an intriguing class of solids due to their tunable electronic, magnetic, and structural ground states. This work investigates Cu(Me,Br‐dicyanoquinonediimine) 2 single crystals, a charge transfer radical ion salt which exhibits a Peierls insulator‐to‐metal transition at low temperatures. The ultrafast electron diffraction experiments observe collective atomic motions at the photoinduced phase transition with a temporal resolution of 1 ps. These measurements reveal the photoinduced lifting of the insulating phase to happen within 2 ps in the entire crystal volume with an external quantum efficiency of conduction band electrons per absorbed photon of larger than 20. This huge cooperativity of the system, directly monitored during the phase transition, is accompanied by specific intramolecular motions. However, only an additional internal volume expansion, corresponding to a pressure relief, allows the metallic state for long times to be optically locked. The identification of the microscopic molecular pathways that optically drive the structural Peierls transition in Cu(DCNQI) 2 highlights the tailored response to external stimuli available in these complex functional materials, a feature enabling high‐speed optical sensing and switching with outstanding signal responsivity.