Deconstructing the Hubbard Hamiltonian by Ultrafast Quantum Modulation Spectroscopy in Solid-state Mott Insulators

S. Kaiser, S. R. Clark, D. Nicoletti, G. Cotugno, R. I. Tobey, N. Dean, S. Lupi, H. Okamoto, T. Hasegawa, D. Jaksch, A. Cavalleri

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Most available theories for correlated electron transport are based on the Hubbard Hamiltonian. In this effective theory, renormalized hopping and interaction parameters only implicitly incorporate the coupling of correlated charge carriers to microscopic degrees of freedom. Unfortunately, no spectroscopy can individually probe such renormalizations, limiting the applicability of Hubbard models. We show here that the role of each individual degree of freedom can be made explicit by using a new experimental technique, which we term 'quantum modulation spectroscopy' and we demonstrate here in the one-dimensional Mott insulator ET-F2TCNQ. We explore the role on the charge hopping of two localized molecular modes, which we drive with a mid infrared optical pulse. Sidebands appear in the modulated optical spectrum, and their linshape is fitted with a model based on the dynamic Hubbard Hamiltonian. A striking asymmetry between the renormalization of doublons and holons is revealed. The concept of quantum modulation spectroscopy can be used to systematically deconstruct Hubbard Hamiltonians in many materials, exposing the role of any mode, electronic or magnetic, that can be driven to large amplitude with a light field.
Original languageEnglish
Article number3823
Number of pages6
JournalScientific Reports
Early online date22 Jan 2014
Publication statusPublished - 22 Jan 2014


  • cond-mat.str-el


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