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  Mode-Selective Control of the Crystal Lattice

Först, M., Mankowsky, R., & Cavalleri, A. (2015). Mode-Selective Control of the Crystal Lattice. Accounts of Chemical Research, 48(2), 380-387. doi:10.1021/ar500391x.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0025-0BAD-C Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002A-FB5B-B
Genre: Journal Article

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https://dx.doi.org/10.1021/ar500391x (Publisher version)
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 Creators:
Först, Michael1, 2, Author              
Mankowsky, Roman1, 2, Author              
Cavalleri, Andrea1, 2, 3, Author              
Affiliations:
1Quantum Condensed Matter Dynamics, Condensed Matter Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938293              
2Department of Physics, Clarendon Laboratory, University of Oxford, ou_persistent22              
3Center for Free Electron Laser Science, Hamburg 22761, Germany, ou_persistent22              

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Free keywords: Optical, Electron, and Mass Spectroscopy and Other Related Properties
 Abstract: Driving phase changes by selective optical excitation of specific vibrational modes in molecular and condensed phase systems has long been a grand goal for laser science. However, phase control has to date primarily been achieved by using coherent light fields generated by femtosecond pulsed lasers at near-infrared or visible wavelengths. This field is now being advanced by progress in generating intense femtosecond pulses in the mid-infrared, which can be tuned into resonance with infrared-active crystal lattice modes of a solid. Selective vibrational excitation is particularly interesting in complex oxides with strong electronic correlations, where even subtle modulations of the crystallographic structure can lead to colossal changes of the electronic and magnetic properties. In this Account, we summarize recent efforts to control the collective phase state in solids through mode-selective lattice excitation. The key aspect of the underlying physics is the nonlinear coupling of the resonantly driven phonon to other (Raman-active) modes due to lattice anharmonicities, theoretically discussed as ionic Raman scattering in the 1970s. Such nonlinear phononic excitation leads to rectification of a directly excited infrared-active mode and to a net displacement of the crystal along the coordinate of all anharmonically coupled modes. We present the theoretical basis and the experimental demonstration of this phenomenon, using femtosecond optical spectroscopy and ultrafast X-ray diffraction at a free electron laser. The observed nonlinear lattice dynamics is shown to drive electronic and magnetic phase transitions in many complex oxides, including insulator–metal transitions, charge/orbital order melting and magnetic switching in manganites. Furthermore, we show that the selective vibrational excitation can drive high-TC cuprates into a transient structure with enhanced superconductivity. The combination of nonlinear phononics with ultrafast crystallography at X-ray free electron lasers may provide new design rules for the development of materials that exhibit these exotic behaviors also at equilibrium.

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Language(s): eng - English
 Dates: 2014-10-242015-01-162015-02-17
 Publication Status: Published in print
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/ar500391x
 Degree: -

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Title: Accounts of Chemical Research
  Other : Acc. Chem. Res.
Source Genre: Journal
 Creator(s):
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Publ. Info: Easton, Pa. : American Chemical Society
Pages: - Volume / Issue: 48 (2) Sequence Number: - Start / End Page: 380 - 387 Identifier: ISSN: 0001-4842
CoNE: /journals/resource/954925373792