Ultrafast Transition from State-Blocking Dynamics to Electron Localization in Transition Metal ß-Tungsten.

We describe an ultrafast transition of the electronic response of optically excited transition metal ß-tungsten with few-femtosecond time resolution. The response moves from a regime where state filling of the excited carrier population around the Fermi level dominates towards localization of carriers onto the outer d orbitals. This is in contrast to previous measurements using ultrafast element-specific core-level spectroscopy enabled by attosecond transient absorption spectroscopy on transition metals such as titanium and around the transition metal atom in transition metal dichalchogenides MoTe_{2} and MoSe_{2}. This surprisingly different dynamical response for ß-tungsten can be explained by considering the electron-electron dynamics on a few-femtosecond timescale and the slower electron-phonon thermalization dynamics.

Ultrafast electron localization and screening in a transition metal dichalcogenide.

The coupling of light to electrical charge carriers in semiconductors is the foundation of many technological applications. Attosecond transient absorption spectroscopy measures simultaneously how excited electrons and the vacancies they leave behind dynamically react to the applied optical fields. In compound semiconductors, these dynamics can be probed via any of their atomic constituents with core-level transitions into valence and conduction band. Typically, the atomic species forming the compound contribute comparably to the relevant electronic properties of the material. One therefore expects to observe similar dynamics, irrespective of the choice of atomic species via which it is probed. Here, we show in the two-dimensional transition metal dichalcogenide semiconductor MoSe2, that through a selenium-based core-level transition we observe charge carriers acting independently from each other, while when probed through molybdenum, the collective, many-body motion of the carriers dominates. Such unexpectedly contrasting behavior can be explained by a strong localization of electrons around molybdenum atoms following absorption of light, which modifies the local fields acting on the carriers. We show that similar behavior in elemental titanium metal [M. Volkov et al., Nat. Phys. 15, 1145-1149 (2019)] carries over to transition metal-containing compounds and is expected to play an essential role for a wide range of such materials. Knowledge of independent particle and collective response is essential for fully understanding these materials.

Phase stabilization of an attosecond beamline combining two IR colors.

We present a phase-stabilized attosecond pump-probe beamline involving two separate infrared wavelengths for high-harmonic generation (HHG) and pump or probe. The output of a Ti:sapphire laser is partly used to generate attosecond pulses via HHG and partly to pump an optical parametric amplifier (OPA) that converts the primary Ti:sapphire radiation to a longer wavelength. The attosecond pulse and down-converted infrared are recombined after a more than 20-m-long Mach-Zehnder interferometer that spans across two laboratories and separate optical tables. We demonstrate a technique for active stabilization of the relative phase of the pump and probe to within 450 as rms, without the need for an auxiliary continuous wave (cw) laser. The long-term stability of our system is demonstrated with an attosecond photoelectron streaking experiment. While the technique has been shown for one specific OPA output wavelength (1560 nm), it should also be applicable to other OPA output wavelengths. Our setup design permits tuning of the OPA wavelength independently from the attosecond pulse generation. This approach yields new possibilities for studying the wavelength-dependence of field-driven attosecond electron dynamics in various systems.