Quantum spin dynamics

Abstract:

Competition between electron localization and delocalization in Mott insulators underpins the physics of strongly correlated electron systems. Photoexcitation, which redistributes charge, can control this many-body process on the ultrafast 1,2 timescale. So far, time-resolved studies have been carried out in solids in which other degrees of freedom, such as lattice, spin or orbital excitations 3-5 , dominate. However, the underlying quantum dynamics of bareg electronic excitations has remained out of reach. Quantum many-body dynamics are observed only in the controlled environment of optical lattices 6,7 where the dynamics are slower and lattice excitations are absent. By using nearly single-cycle near-infrared pulses, we have measured coherent electronic excitations in the organic salt ET-F 2 TCNQ, a prototypical one-dimensional Mott insulator. After photoexcitation, a new resonance appears, which oscillates at 25THz. Time-dependent simulations of the Mottg Hubbard Hamiltonian reproduce the oscillations, showing that electronic delocalization occurs through quantum interference between bound and ionized holong doublon pairs. © 2011 Macmillan Publishers Limited. All rights reserved.