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Title: Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material

Photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. We present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V 2O 3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a 1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A 1g coherent phonon. Furthermore, this configuration is in stark contrast with the thermally accessible ones - the A 1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [2] ;  [2] ;  [2] ;  [5] ;  [2] ;  [2] ;  [6] ;  [7] ;  [8] ;  [9] ;  [9] ;  [9] ;  [10] ;  [10] ;  [3] ;  [2]
  1. Univ. of Paris-Sud, Orsay (France). Lab. of Solid State Physics; ETH Zurich (Switzerland). Inst. for Quantum Electronics
  2. Univ. of Paris-Sud, Orsay (France). Lab. of Solid State Physics
  3. International School for Advanced Studies SISSA, Trieste (Italy)
  4. Superior National School of Advanced Techniques, Palaiseau (France). Ecole Polytechnique
  5. Ecole Polytechnique, Palaiseau (France). CEA Center
  6. Synchrotron SOLEIL, Gif-sur-Yvette (France); Univ. of Paris-Sud, Orsay (France)
  7. Univ. of Paris-Sud, Orsay (France). Lab. of Solid State Physics; Synchrotron SOLEIL, Gif-sur-Yvette (France)
  8. Synchrotron SOLEIL, Gif-sur-Yvette (France); Sorbonne Univ., Paris (France)
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1344178
Alternate Identifier(s):
OSTI ID: 1379678

Lantz, G., Mansart, B., Grieger, D., Boschetto, D., Nilforoushan, N., Papalazarou, E., Moisan, N., Perfetti, L., Jacques, V. L. R., Le Bolloc'h, D., Laulhé, C., Ravy, S., Rueff, J-P, Glover, T. E., Hertlein, M. P., Hussain, Z., Song, S., Chollet, M., Fabrizio, M., and Marsi, M.. Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material. United States: N. p., Web. doi:10.1038/ncomms13917.
Lantz, G., Mansart, B., Grieger, D., Boschetto, D., Nilforoushan, N., Papalazarou, E., Moisan, N., Perfetti, L., Jacques, V. L. R., Le Bolloc'h, D., Laulhé, C., Ravy, S., Rueff, J-P, Glover, T. E., Hertlein, M. P., Hussain, Z., Song, S., Chollet, M., Fabrizio, M., & Marsi, M.. Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material. United States. doi:10.1038/ncomms13917.
Lantz, G., Mansart, B., Grieger, D., Boschetto, D., Nilforoushan, N., Papalazarou, E., Moisan, N., Perfetti, L., Jacques, V. L. R., Le Bolloc'h, D., Laulhé, C., Ravy, S., Rueff, J-P, Glover, T. E., Hertlein, M. P., Hussain, Z., Song, S., Chollet, M., Fabrizio, M., and Marsi, M.. 2017. "Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material". United States. doi:10.1038/ncomms13917. https://www.osti.gov/servlets/purl/1344178.
@article{osti_1344178,
title = {Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material},
author = {Lantz, G. and Mansart, B. and Grieger, D. and Boschetto, D. and Nilforoushan, N. and Papalazarou, E. and Moisan, N. and Perfetti, L. and Jacques, V. L. R. and Le Bolloc'h, D. and Laulhé, C. and Ravy, S. and Rueff, J-P and Glover, T. E. and Hertlein, M. P. and Hussain, Z. and Song, S. and Chollet, M. and Fabrizio, M. and Marsi, M.},
abstractNote = {Photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. We present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V2O3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A1g coherent phonon. Furthermore, this configuration is in stark contrast with the thermally accessible ones - the A1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.},
doi = {10.1038/ncomms13917},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {1}
}

Works referenced in this record:

Metal-insulator transitions
journal, October 1998
  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039