Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation.
We report on orbital-dependent quasiparticle dynamics in EuFe2As2, a parent compound of Febased superconductors, and a novel way to experimentally identify this behavior using time-and angle-resolved photoelectron spectroscopy across the spin density wave transition. We observe two different relaxation time scales for photo-excited dxz/dyz and dxy electrons. While the itinerant dxz/dyz electrons relax faster through the electron-electron scattering channel, dxy electrons form a quasi-equilibrium state with the lattice due to their localized character, and the state decays slowly. Our findings suggest that electron correlation in Fe-pnictides is an important property, which should be taken into careful account when describing the electronic properties of both parent and carrier-doped compounds, and therefore establish a strong connection with cuprates.
We present a method for measuring a complete frequency map of laser-dressed states with femtosecond lifetimes. It is based on collecting decay products as a function of the frequency of the excitation pulse and its delay with respect to the linearly chirped laser pulse, centered at the resonant transition frequency. The method has been tested on the case of laser-coupled 2s2p 1 P o and 2p 2 1 S e autoionizing resonances in He and is applicable to other quantum systems with short-lived states. When the laser coupling effects are known, the excitation pulse properties can be extracted from the map.
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