Search

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. Often, 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 $MoSe_2$, that through a selenium-based 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 traced back to 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 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., Comment: 30 pages, 11 figures

Transition metals with their densely confined and strongly coupled valence electrons are key constituents of many materials with unconventional properties, such as high-Tc superconductors, Mott insulators and transition-metal dichalcogenides. Strong electron interaction offers a fast and efficient lever to manipulate their properties with light, creating promising potential for next-generation electronics. However, the underlying dynamics is a fast and intricate interplay of polarization and screening effects, which is poorly understood. It is hidden below the femtosecond timescale of electronic thermalization, which follows the light-induced excitation. Here, we investigate the many-body electron dynamics in transition metals before thermalization sets in. We combine the sensitivity of intra-shell transitions to screening effects with attosecond time resolution to uncover the interplay of photo-absorption and screening. First-principles time-dependent calculations allow us to assign our experimental observations to ultrafast electronic localization on d-orbitals. The latter modifies the whole electronic structure as well as the collective dynamic response of the system on a timescale much faster than the light-field cycle. Our results demonstrate a possibility for steering the electronic properties of solids prior to electron thermalization, suggesting that the ultimate speed of electronic phase transitions is limited only by the duration of the controlling laser pulse. Furthermore, external control of the local electronic density serves as a fine tool for testing state-of-the art models of electron-electron interactions. We anticipate our study to facilitate further investigations of electronic phase transitions, laser-metal interactions and photo-absorption in correlated electron systems on its natural timescale.

Strong-field ionization and rescattering beyond the long-wavelength limit of the dipole approximation is studied with elliptically polarized mid-IR pulses. We have measured the full three-dimensional photoelectron momentum distributions (3D PMDs) with velocity map imaging and tomographic reconstruction. The ellipticity-dependent 3D-PMD measurements revealed an unexpected sharp, thin line-shaped ridge structure in the polarization plane for low momentum photoelectrons. With classical trajectory Monte Carlo (CTMC) simulations and analytical methods we identified the associated ionization dynamics for this sharp ridge to be due to Coulomb focusing of slow recollisions of electrons with a momentum approaching zero. This ridge is another example of the many different ways how the Coulomb field of the parent ion influences the different parts of the momentum space of the ionized electron wave packet. Building on this new understanding of the PMD, we extend our studies on the role played by the magnetic field component of the laser beam when operating beyond the long-wavelength limit of the dipole approximation. In this regime, we find that the PMD exhibits an ellipticity-dependent asymmetry along the beam propagation direction: the peak of the projection of the PMD onto the beam propagation axis is shifted from negative to positive values with increasing ellipticity. This turnover occurs rapidly once the ellipticity exceeds $\sim$0.1. We identify the sharp, thin line-shaped ridge structure in the polarization plane as the origin of the ellipticity-dependent PMD asymmetry in the beam propagation direction. These results yield fundamental insights into strong-field ionization processes, and should increase the precision of the emerging applications relying on this technique, including time-resolved holography and molecular imaging.

Advances in the amplification and manipulation of ultrashort laser pulses has led to revolutions in several areas. Examples include chirped pulse amplification for generating high peak-power lasers, power-scalable amplification techniques, pulse shaping via modulation of spatially-dispersed laser pulses, and efficient frequency-mixing in quasi-phase-matched nonlinear crystals to access new spectral regions. In this work, we introduce and demonstrate a new platform for nonlinear optics which has the potential to combine all of these separate functionalities (pulse amplification, frequency transfer, and pulse shaping) into a single monolithic device. Moreover, our approach simultaneously offers solutions to the performance-limiting issues in the conventionally-used techniques, and supports scaling in power and bandwidth of the laser source. The approach is based on two-dimensional patterning of quasi-phase-matching gratings combined with optical parametric interactions involving spatially dispersed laser pulses. Our proof of principle experiment demonstrates this new paradigm via mid-infrared optical parametric chirped pulse amplification of few-cycle pulses.

We demonstrate a new attosecond pulse reconstruction modality which uses an algorithm that is derived from ptychography. In contrast to other methods, energy and delay sampling are not correlated, and as a result, the number of electron spectra to record is considerably smaller. Together with the robust algorithm, this leads to a more precise and fast convergence of the reconstruction., Comment: 12 pages, 7 figures, the MATLAB code for the method described in this paper is freely available at http://figshare.com/articles/attosecond_Extended_Ptychographyc_Iterative_Engine_ePIE_/1601876

We report the breakdown of the electric dipole approximation in the long-wavelength limit in strong-field ionization with linearly polarized few-cycle mid-infrared laser pulses at intensities on the order of 10$^{13}$ W/cm$^2$. Photoelectron momentum distributions were recorded by velocity map imaging and projected onto the beam propagation axis. We observe an increasing shift of the peak of this projection opposite to the beam propagation direction with increasing laser intensities. From a comparison with semi-classical simulations, we identify the combined action of the magnetic field of the laser pulse and the Coulomb potential as origin of our observations., Comment: 12 pages, 4 figures

We present measurements of single-photon ionization time delays between valence electrons of argon and neon using a coincidence detection technique that allows for the simultaneous measurement of both species under identical conditions. Taking into account the chirp of the ionizing single attosecond pulse (attochirp) ensures that the clock of our measurement technique is started at the same time for both types of electrons, revealing with high accuracy and resolution energy-dependent time delays of a few tens of attoseconds. By comparing our results with theoretical predictions, we confirm that the so-called Wigner delay correctly describes single-photon ionization delays as long as atomic resonances can be neglected. Our data, however, also reveal that such resonances can greatly affect the measured delays beyond the simple Wigner picture.

How quanta of energy and charge are transported on both atomic spatial and ultrafast time scales is at the heart of modern technology. Recent progress in ultrafast spectroscopy has allowed us to directly study the dynamical response of an electronic system to interaction with an electromagnetic field. Here, we present energy-dependent photoemission delays from the noble metal surfaces Ag(111) and Au(111). An interferometric technique based on attosecond pulse trains is applied simultaneously in a gas phase and a solid state target to derive surface-specific photoemission delays. Experimental delays on the order of 100 as are in the same time range as those obtained from simulations. The strong variation of measured delays with excitation energy in Ag(111), which cannot be consistently explained invoking solely electron transport or initial state localization as supposed in previous work, indicates that final state effects play a key role in photoemission from solids.

We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.