Pressure-Dependent Relaxation in the Photoexcited Mott Insulator ETF2TCNQ: Influence of Hopping and Correlations on Quasiparticle Recombination Rates

M. Mitrano, G. Cotugno, S. R. Clark, R. Singla, S. Kaiser, J. Stähler, R. Beyer, M. Dressel, L. Baldassarre, D. Nicoletti, A. Perucchi, T. Hasegawa, H. Okamoto, D. Jaksch, and A. Cavalleri
Phys. Rev. Lett. 112, 117801 – Published 18 March 2014
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Abstract

We measure the ultrafast recombination of photoexcited quasiparticles (holon-doublon pairs) in the one dimensional Mott insulator ETF2TCNQ as a function of external pressure, which is used to tune the electronic structure. At each pressure value, we first fit the static optical properties and extract the electronic bandwidth t and the intersite correlation energy V. We then measure the recombination times as a function of pressure, and we correlate them with the corresponding microscopic parameters. We find that the recombination times scale differently than for metals and semiconductors. A fit to our data based on the time-dependent extended Hubbard Hamiltonian suggests that the competition between local recombination and delocalization of the Mott-Hubbard exciton dictates the efficiency of the recombination.

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  • Received 28 August 2013

DOI:https://doi.org/10.1103/PhysRevLett.112.117801

© 2014 American Physical Society

Authors & Affiliations

M. Mitrano1,*, G. Cotugno1,2, S. R. Clark3,2, R. Singla1, S. Kaiser1,†, J. Stähler4, R. Beyer5, M. Dressel5, L. Baldassarre6, D. Nicoletti1, A. Perucchi7, T. Hasegawa8, H. Okamoto9, D. Jaksch2,3, and A. Cavalleri1,2,‡

  • 1Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany
  • 2Department of Physics, Oxford University, Clarendon Laboratory, Parks Road, OX1 3PU Oxford, United Kingdom
  • 3Centre for Quantum Technologies, National University of Singapore, 3 Science Drive 2, Singapore 117543, Singapore
  • 4Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany
  • 51. Physikalisches Insitut, Universität Stuttgart, Pfaffenwaldring 57, 70550 Stuttgart, Germany
  • 6Center for Life NanoScience@Sapienza, Istituto Italiano di Tecnologia, V.le Regina Elena 291, 00185 Rome, Italy
  • 7INSTM UdR Trieste-ST and Elettra - Sincrotrone Trieste S.C.p.A., S.S. 14 km 163.5 in Area Science Park, 34012 Basovizza, Trieste Italy
  • 8National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8562, Japan
  • 9Department of Advanced Material Science, University of Tokyo, Chiba 277-8561, Japan

  • *Matteo.Mitrano@mpsd.mpg.de
  • Stefan.Kaiser@mpsd.mpg.de
  • Andrea.Cavalleri@mpsd.mpg.de

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Vol. 112, Iss. 11 — 21 March 2014

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