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Register a new userNonequilibrium Electron Dynamics In Pump-Probe Spectroscopy: Role Of Excited Phonon Populations
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Added by
Omadillo Abdurazakov
Publication date
2018
fields
Physics
and research's language is
English
Authors
O. Abdurazakov
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We study the role of excited phonon populations in the relaxation rates of nonequilibrium electrons using a nonequilibrium Greens function formalism. The transient modifications in the phononic properties are accounted for by self-consistently solving the Dyson equation for the electron and phonon Greens functions. The pump induced changes manifest in both the electronic and phononic spectral functions. We find that the excited phonon populations suppress the decay rates of nonequilibrium electrons due to enhanced phonon absorption. The increased phonon occupation also sets the nonequilibrium decay rates and the equilibrium scattering rates apart. The decay rates are found to be time-dependent, and this is illustrated in the experimentally observed population decay of photoexcited $mathrm{Bi}_{1.5}mathrm{Sb}_{0.5} mathrm{Te}_{1.7}mathrm{Se}_{1.3}$.
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In high-resolution core-valence-valence (CVV) Auger electron spectroscopy from the surface of a solid at thermal equilibrium, the main correlation satellite, visible in the case of strong valence-electron correlations, corresponds to a bound state of the two holes in the final state of the CVV Auger process. We discuss the physical significance of this satellite in nonequilibrium pump-probe Auger spectroscopy by numerical analysis of a single-band Hubbard-type model system including core states and a continuum of high-energy scattering states. It turns out that the spectrum of the photo-doped system, due to the increased double occupancy, shares features with the equilibrium spectrum at higher fillings. The pumping of doublons can be watched when working with overlapping pulses at short $Delta t$. For larger pump-probe delays $Delta t$ and on the typical femtosecond time scale for electronic relaxation processes, spectra are hardly $Delta t$-dependent, reflecting the high stability of bound two-hole states for strong Hubbard-$U$. We argue that taking into account the spatial expansion of single-particle orbitals when these are doubly occupied, as described by the dynamical Hubbard model, produces an oscillation of the barycenter of the satellite as a function of $Delta t$. Pump-probe Auger-electron spectroscopy is thus highly sensitive to dynamical screening of the Coulomb interaction.
A femtosecond laser-irradiated crystallizing technique is tried to convert amorphous Sb2Te3 film into crystalline film. Sensitive coherent phonon spectroscopy (CPS) is used to monitor the crystallization of amorphous Sb2Te3 film at the original irradiation site. The CPS reveals that the vibration strength of two phonon modes that correspond to the characteristic phonon modes of crystalline Sb2Te3, enhances with increasing laser irradiation fluence (LIF), showing the rise of the degree of crystallization with LIF and that femtosecond laser irradiation is a good post-treatment technique. Time-resolved circularly polarized pump-probe spectroscopy is used to investigate electron spin relaxation dynamics of the laser-induced crystallized Sb2Te3 film. Spin relaxation process indeed is observed, confirming the theoretical predictions on the validity of spin-dependent optical transition selection rule and the feasibility of transient spin-grating-based optical detection scheme of spin-plasmon collective modes in Sb2Te3-like topological insulators.
The interplay of Coulomb and electron-phonon interactions with thermal and quantum fluctuations facilitates rich phase diagrams in two-dimensional electron systems. Layered transition metal dichalcogenides hosting charge, excitonic, spin and superconducting order form an epitomic material class in this respect. Theoretical studies of materials like NbS$_2$ have focused on the electron-phonon coupling whereas the Coulomb interaction, particularly strong in the monolayer limit, remained essentially untouched. Here, we analyze the interplay of short- and long-range Coulomb as well as electron-phonon interactions in NbS$_2$ monolayers. The combination of these interactions causes electronic correlations that are fundamentally different to what would be expected from the interaction terms separately. The fully interacting electronic spectral function resembles the non-interacting band structure but with appreciable broadening. An unexpected coexistence of strong charge and spin fluctuations puts NbS$_2$ close to spin and charge order, suggesting monolayer NbS$_2$ as a platform for atomic scale engineering of electronic quantum phases.
We examine the exact equation of motion for the relaxation of populations of strongly correlated electrons after a nonequilibrium excitation by a pulsed field, and prove that the populations do not change when the Greens functions have no average time dependence. We show how the average time dependence enters into the equation of motion to lowest order and describe what governs the relaxation process of the electron populations in the long-time limit. While this result may appear, on the surface, to be required by any steady-state solution, the proof is nontrivial, and provides new critical insight into how nonequilibrium populations relax, which goes beyond the assumption that they thermalize via a simple relaxation rate determined by the imaginary part of the self-energy, or that they can be described by a quasi-equilibrium condition with a Fermi-Dirac distribution and a time-dependent temperature. We also discuss the implications of this result to approximate theories, which may not satisfy the exact relation in the equation of motion.
Two-dimensional electron gases (2DEGs) in SrTiO$_3$ have become model systems for engineering emergent behaviour in complex transition metal oxides. Understanding the collective interactions that enable this, however, has thus far proved elusive. Here we demonstrate that angle-resolved photoemission can directly image the quasiparticle dynamics of the $d$-electron subband ladder of this complex-oxide 2DEG. Combined with realistic tight-binding supercell calculations, we uncover how quantum confinement and inversion symmetry breaking collectively tune the delicate interplay of charge, spin, orbital, and lattice degrees of freedom in this system. We reveal how they lead to pronounced orbital ordering, mediate an orbitally-enhanced Rashba splitting with complex subband-dependent spin-orbital textures and markedly change the character of electron-phonon coupling, co-operatively shaping the low-energy electronic structure of the 2DEG. Our results allow for a unified understanding of spectroscopic and transport measurements across different classes of SrTiO$_3$-based 2DEGs, and yield new microscopic insights on their functional properties.
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