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Ultrafast dissolution and creation of bonds in IrTe2 induced by photodoping

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Ideta,  S.-I.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Ultrafast Imaging;
Quantum-Phase Electronics Center, Department of Applied Physics, University of Tokyo;

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Zhang,  Dongfang
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Ultrafast Imaging;

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Dijkstra,  A.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Ultrafast Imaging;
School of Chemistry and School of Physics and Astronomy, University of Leeds;

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Keskin,  S.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Ultrafast Imaging;

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Miller,  R. J. D.
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Ultrafast Imaging;
Departments of Chemistry and Physics, 80 St. George Street, University of Toronto;

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Citation

Ideta, S.-I., Zhang, D., Dijkstra, A., Artyukhin, S., Keskin, S., Cingolani, R., et al. (2018). Ultrafast dissolution and creation of bonds in IrTe2 induced by photodoping. Science Advances, 4(7): eaar3867. doi:10.1126/sciadv.aar3867.


Cite as: http://hdl.handle.net/21.11116/0000-0002-1152-E
Abstract
The observation and control of interweaving spin, charge, orbital, and structural degrees of freedom in materials on ultrafast time scales reveal exotic quantum phenomena and enable new active forms of nanotechnology. Bonding is the prime example of the relation between electronic and nuclear degrees of freedom. We report direct evidence illustrating that photoexcitation can be used for ultrafast control of the breaking and recovery of bonds in solids on unprecedented time scales, near the limit for nuclear motions. We describe experimental and theoretical studies of IrTe2 using femtosecond electron diffraction and density functional theory to investigate bonding instability. Ir-Ir dimerization shows an unexpected fast dissociation and recovery due to the filling of the antibonding dxy orbital. Bond length changes of 20% in IrTe2 are achieved by effectively addressing the bonds directly through this relaxation process. These results could pave the way to ultrafast switching between metastable structures by photoinduced manipulation of the relative degree of bonding in this manner.