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Femtosecond study of A1g phonons in the strong 3D topological insulators: From pump-probe to coherent control

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 Added by Jianbo Hu
 Publication date 2018
  fields Physics
and research's language is English




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Fully symmetric A1g phonons are expected to play a dominant role in electron scattering in strong topological insulators (TIs), thus limiting the ballistic transport of future electronic devices. Here, we report on femtosecond time-resolved observation of a pair of A1g coherent phonons and their optical control in two strong 3D TIs, Bi2Te3 and Bi2Se3, by using a second pump pulse in ultrafast spectroscopy measurements. Along with well-defined phonon properties such as frequency and lifetime, an obvious phonon chirp has been observed, implying a strong coupling between photo-carriers and lattices. The coherent phonon manipulation, on the other hand, allows us to change the phonon amplitude selectively but does not affect either the frequency or coherence lifetime of the chosen mode.



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441 - G. Arregui , O. Ortiz , M. Esmann 2018
Inspired by concepts developed for fermionic systems in the framework of condensed matter physics, topology and topological states are recently being explored also in bosonic systems. The possibility of engineering systems with unidirectional wave propagation and protected against disorder is at the heart of this growing interest. Topogical acoustic effects have been observed in a variety of systems, most of them based on kHz-MHz sound waves, with typical wavelength of the order of the centimeter. Recently, some of these concepts have been successfully transferred to acoustic phonons in nanoscaled multilayered systems. The reported demonstration of confined topological phononic modes was based on Raman scattering spectroscopy, yet the resolution did not suffice to determine lifetimes and to identify other acoustic modes in the system. Here, we use time-resolved pump-probe measurements using an asynchronous optical sampling (ASOPS) technique to overcome these resolution limitations. By means of one-dimensional GaAs/AlAs distributed Bragg reflectors (DBRs) as building blocks, we engineer high frequency ($sim$ 200 GHz) topological acoustic interface states. We are able to clearly distinguish confined topological states from stationary band edge modes. The detection scheme reflects the symmetry of the modes directly through the selection rules, evidencing the topological nature of the measured confined state. These experiments enable a new tool in the study of the more complex topology-driven phonon dynamics such as phonon nonlinearities and optomechanical systems with simultaneous confinement of light and sound.
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.
Time-resolved spectroscopies using intense THz pulses appear as a promising tool to address collective electronic excitations in condensed matter. In particular recent experiments showed the possibility to selectively excite collective modes emerging across a phase transition, as it is the case for superconducting and charge-density-wave (CDW) systems. One possible signature of these excitations is the emergence of coherent oscillations of the differential probe field in pump-probe protocols. While the analogy with the case of phonon modes suggests that the basic underlying mechanism should be a sum-frequency stimulated Raman process, a general theoretical scheme able to describe the experiments and to define the relevant optical quantity is still lacking. Here we provide this scheme by showing that coherent oscillations as a function of the pump-probe time delay can be linked to the convolution in the frequency domain between the squared pump field and a Raman-like non-linear optical kernel. This approach is applied and discussed in few paradigmatic examples: ordinary phonons in an insulator, and collective charge and Higgs fluctuations across a superconducting and a CDW transition. Our results not only account very well for the existing experimental data in a wide variety of systems, but they also offer an useful perspective to design future experiments in emerging materials.
479 - J. Braun , R. Rausch , M. Potthoff 2014
A theoretical frame for pump-probe photoemission is presented. The approach is based on a general formulation using the Keldysh formalism for the lesser Greens function to describe the real-time evolution of the electronic degrees of freedom in the initial state after a strong pump pulse that drives the system out of equilibrium. The final state is represented by a time-reversed low-energy electron diffraction state. Our one-step description is related to Pendrys original formulation of the photoemission process as close as possible. The formalism allows for a quantitative calculation of time-dependent photocurrent for simple metals where a picture of effectively independent electrons is assumed as reliable. The theory is worked out for valence- and core-electron excitations. It comprises the study of different relativistic effects as a function of the pump-probe delay.
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