Real-time probing electron dynamics of an atom in a strong infrared laser field

We present theoretical studies on real-time probing the electron density evolution of an atom in a strong infrared (IR) laser field with few-cycle near-infrared (NIR) and attosecond extreme-ultraviolet (XUV) pulses. Our results indicate that the electron density near the tunneling barrier is reflected in the additional tunneling ionization yield with a delayed NIR pulse and the electron density near the nucleus can be probed by the single photoionization yield with a delayed XUV pulse. It turns out the NIR-probing scheme can be used to study the polarization of the system in an external IR field and the XUV-probing can be additionally applied to explore excitation dynamics during and after the IR field interaction

Direct evidences for inner-shell electron-excitation by laser induced electron recollision

Extreme ultraviolet (XUV) attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe sub-femtosecond dynamics in the microcosms of atoms, molecules and solids[1]. However, with the current technology, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray \hbar\omega>300 eV attosecond bursts and the lower absorption cross-sections in this spectral range. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources.Such an excitation process occurs in a sub-femtosecond timescale, and may provide the necessary "pump" step in a pump-probe experiment[2]. Here we used a few cycle infrared \lambda_{0}~1800nm source[3] and observed direct evidences for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with sub-femtosecond time resolution.Comment: 6 pages, 4 figure

Tunable sub-20 fs pulses from a 500 kHz OPCPA with 15 W average power based on an all-ytterbium laser

An optical parametric chirped pulse amplifier fully based on Yb lasers at 500 kHz is described. Passive optical-synchronization is achieved between a fiber laser-pumped white-light and a 515 nm pump produced with a 200 W picosecond Yb:YAG InnoSlab amplifier. An output power up to 19.7 W with long-term stability of 0.3% is demonstrated for wavelength tunable pulses between 680 nm and 900 nm and spectral stability of 0.2%; 16.5 W can be achieved with a bandwidth supporting 5.4 fs pulses. We demonstrate compression of 30 microjoule pulses to sub-20 fs duration with a prism compressor, suitable for high harmonic generation.Comment: 4 pages, 4 figure

Laser-induced inner-shell excitations through direct electron re-collision versus indirect collision

The dynamics and the decay processes of inner-shell excited atoms are of great interest in physics, chemistry, biology, and technology. The highly excited state decays very quickly through different channels, both radiative and non-radiative. It is therefore a long-standing goal to study such dynamics directly in the time domain. Using few-cycle infrared laser pulses, we investigated the excitation and ionization of inner-shell electrons through laser-induced electron re-collision with the original parent ions and measured the dependence of the emitted x-ray spectra on the intensity and ellipticity of the driving laser. These directly re-colliding electrons can be used as the initiating pump step in pump/probe experiments for studying core-hole dynamics at their natural temporal scale. In our experiment we found that the dependence of the x-ray emission spectrum on the laser intensity and polarization state varies distinctly for the two kinds of atomic systems. Relying on our data and numerical simulations, we explain this behavior by the presence of different excitation mechanisms that are contributing in different ratios to the respective overall x-ray emission yields. Direct re-collision excitation competes with indirect collisions with neighboring atoms by electrons having "drifted away" from the original parent ion. (C) 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreemen

Dynamics of the photoinduced insulator-to-metal transition in a nickelate film

The control of materials properties with light is a promising approach towards the realization of faster and smaller electronic devices. With phases that can be controlled via strain, pressure, chemical composition or dimensionality, nickelates are good candidates for the development of a new generation of high performance and low consumption devices. Here we analyze the photoinduced dynamics in a single crystalline NdNiO$_3$ film upon excitation across the electronic gap. Using time-resolved reflectivity and resonant x-ray diffraction, we show that the pump pulse induces an insulator-to-metal transition, accompanied by the melting of the charge order. Finally we compare our results to similar studies in manganites and show that the same model can be used to describe the dynamics in nickelates, hinting towards a unified description of these photoinduced phase transitions.Comment: 17 pages, 6 figure

Excited-state band structure mapping

[EN] Angle-resolved photoelectron spectroscopy is an extremely powerful probe of materials to access the occupied electronic structure with energy and momentum resolution. However, it remains blind to those dynamic states above the Fermi level that determine technologically relevant transport properties. In this work we extend band structure mapping into the unoccupied states and across the entire Brillouin zone by using a state-of-the-art high repetition rate, extreme ultraviolet femtosecond light source to probe optically excited samples. The wideranging applicability and power of this approach are demonstrated by measurements on the two-dimensional semiconductor WSe2, where the energy-momentum dispersion of valence and conduction bands are observed in a single experiment. This provides a direct momentum-resolved view, not only on the complete out-of-equilibrium band gap but also on its renormalization induced by electronic screening. Our work establishes a benchmark for measuring the band structure of materials, with direct access to the energy-momentum dispersion of the excited-state spectral function.A This work was funded by the Max-Planck-Gesellschaft, by the German Research Foundation (DFG) , within the Emmy Noether Program (Grant No. RE 3977/1) , and Grants No. FOR1700 (Project E5) , No. SPP2244 (Project No. 443366970) , and from the European Research Council, Grant ERC-2015-CoG-682843. M.P. acknowledges financial support from the Swiss National Science Foundation (SNSF) through Grant No. CRSK-2_196756. C.W.N. and C.M. ac-knowledge financial support by Swiss National Science Foundation (SNSF) Grant No. P00P2_170597. A.R. and H.H. acknowledge financial support from the European Research Council (Grant No. ERC-2015-AdG-694097) and the Cluster of Excellence "CUI: Advanced Imaging of Matter" of the Deutsche Forschungsgemeinschaft (Grant EXC 2056, Project No. 390715994)

Dynamics of the photoinduced insulator-to-metal transition in a nickelate film

Material properties can be controlled via strain, pressure, chemical composition, or dimensionality. Nickelates are particularly susceptible due to their strong variations of the electronic and magnetic properties on such external stimuli. Here, we analyze the photoinduced dynamics in a single crystalline NdNiO3 film upon excitation across the electronic gap. Using time-resolved reflectivity and resonant x-ray diffraction, we show that the pump pulse induces an insulator-to-metal transition, accompanied by the melting of the charge order. Finally, we compare our results with similar studies in manganites and show that the same model can be used to describe the dynamics in nickelates, hinting towards a unified description of these photoinduced electronic ordering phase transitions. © 2018 Author(s)

Compact and robust supercontinuum generation and post-compression using multiple thin plates

We report on compact and robust supercontinuum generation and post-compression using transmission of light through multiple thin solid plates at the SwissFEL X-ray free-electron laser facility. A single stage consisting of three thin plates followed by a chirped mirror compressor achieves compression of initially 30-fs pulses with 800-nm center wavelength to sub-10-fs duration. We also demonstrate a two-stage implementation to compress the pulses further to sub-5-fs duration. With the two-stage setup, the generated supercontinuum includes wavelengths ranging from 500 to 1100 nm. The multiplate setup is compact, robust, and stable, which makes it ideal for applications at free-electron laser facilities such as pump-probe experiments and laser-arrival timing tools.ISSN:2095-4719ISSN:2052-328

Generation of millijoule-level sub-5 fs violet laser pulses

We demonstrate the generation, spectral broadening and post-compression of second harmonic pulses using a thin beta barium borate (BBO) crystal on a fused-silica substrate as the nonlinear interaction medium. By combining second harmonic generation in the BBO crystal with self-phase modulation in the fused-silica substrate, we efficiently generate millijoule-level broadband violet pulses from a single optical component. The second harmonic spectrum covers a range from long wave ultraviolet (down to 310 nm) to visible (up to 550 nm) with a bandwidth of 65 nm. Subsequently, we compress the second harmonic beam to a duration of 4.8 fs with a pulse energy of 0.64 mJ (5 fs with a pulse energy of 1.05 mJ) using chirped mirrors. The all-solid free-space apparatus is compact, robust and pulse energy scalable, making it highly advantageous for generating intense second harmonic pulses from near-infrared femtosecond lasers in the sub-5 fs regime.ISSN:2095-4719ISSN:2052-328