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Strong Electronic Correlation Effects in Coherent Multidimensional Nonlinear Optical Spectroscopy

Karadimitriou, M. E. and Kavousanaki, E. G. and Dani, K. M. and Fromer, N. A. and Perakis, I. E. (2011) Strong Electronic Correlation Effects in Coherent Multidimensional Nonlinear Optical Spectroscopy. Journal of Physical Chemistry B, 115 (18). pp. 5634-5647. ISSN 1520-6106.

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We discuss a many−body theory of the coherent ultrafast nonlinear optical response of systems with a strongly correlated electronic ground state that responds unadiabatically to photoexcitation. We introduce a truncation of quantum kinetic density matrix equations of motion that does not rely on an expansion in terms of the interactions and thus applies to strongly correlated systems. For this we expand in terms of the optical field, separate out contributions to the time−evolved many−body state due to correlated and uncorrelated multiple optical transitions, and use “Hubbard operator” density matrices to describe the exact dynamics of the individual contributions within a subspace of strongly coupled states, including “pure dephasing”. Our purpose is to develop a quantum mechanical tool capable of exploring how, by coherently photoexciting selected modes, one can trigger nonlinear dynamics of strongly coupled degrees of freedom. Such dynamics could lead to photoinduced phase transitions. We apply our theory to the nonlinear response of a two−dimensional electron gas (2DEG) in a magnetic field. We coherently photoexcite the two lowest Landau level (LL) excitations using three time−delayed optical pulses. We identify some striking temporal and spectral features due to dynamical coupling of the two LLs facilitated by inter−Landau−level magnetoplasmon and magnetoroton excitations and compare to three−pulse four−wave−mixing (FWM) experiments. We show that these features depend sensitively on the dynamics of four−particle correlations between an electron−hole pair and a magnetoplasmon/magnetoroton, reminiscent of exciton−exciton correlations in undoped semiconductors. Our results shed light into unexplored coherent dynamics and relaxation of the quantum Hall system (QHS) and can provide new insight into non−equilibrium co−operative phenomena in strongly correlated systems.

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Additional Information:© 2011 American Chemical Society. Published In Issue May 12, 2011; Article ASAP March 11, 2011; Received: December 14, 2010; Accepted: January 21, 2011. This work was supported by the EU ITN program ICARUS.
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Issue or Number:18
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Official Citation:Strong Electronic Correlation Effects in Coherent Multidimensional Nonlinear Optical Spectroscopy M. E. Karadimitriou, E. G. Kavousanaki, K. M. Dani, N. A. Fromer, I. E. Perakis The Journal of Physical Chemistry B 2011 115 (18), 5634-5647
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:23748
Deposited By: Jason Perez
Deposited On:20 May 2011 17:42
Last Modified:03 Oct 2019 02:49

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