Passively CEP stable sub-2-cycle source in the mid-infrared by adiabatic difference frequency generation.

We report on the generation of a passive carrier-envelope phase (CEP) stable 1.7-cycle pulse in the mid-infrared by adiabatic difference frequency generation. With sole material-based compression, we achieve a sub-2-cycle 16-fs pulse at a center wavelength of 2.7 µm and measured a CEP stability of <190 mrad root mean square. The CEP stabilization performance of an adiabatic downconversion process is characterized for the first time, to the best of our knowledge.

Parametric waveform synthesis: a scalable approach to generate sub-cycle optical transients.

The availability of electromagnetic pulses with controllable field waveform and extremely short duration, even below a single optical cycle, is imperative to fully harness strong-field processes and to gain insight into ultrafast light-driven mechanisms occurring in the attosecond time-domain. The recently demonstrated parametric waveform synthesis (PWS) introduces an energy-, power- and spectrum-scalable method to generate non-sinusoidal sub-cycle optical waveforms by coherently combining different phase-stable pulses attained via optical parametric amplifiers. Significant technological developments have been made to overcome the stability issues related to PWS and to obtain an effective and reliable waveform control system. Here we present the main ingredients enabling PWS technology. The design choices concerning the optical, mechanical and electronic setups are justified by analytical/numerical modeling and benchmarked by experimental observations. In its present incarnation, PWS technology enables the generation of field-controllable mJ-level few-femtosecond pulses spanning the visible to infrared range.

Strong-field coherent control of isolated attosecond pulse generation.

Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: improved spectral tunability (allowing selectivity in addressing electronic transitions) and higher photon flux (permitting to measure low cross-section processes). New developments come through parametric waveform synthesis, which provides control over the shape of field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-harmonic generation. Here we demonstrate that the first goal is fulfilled since central energy, spectral bandwidth/shape and temporal duration of isolated attosecond pulses can be controlled by shaping the laser waveform via two key parameters: the relative-phase between two halves of the multi-octave spanning spectrum, and the overall carrier-envelope phase. These results not only promise to expand the experimental possibilities in attosecond science, but also demonstrate coherent strong-field control of free-electron trajectories using tailored optical waveforms.

Secondary-Phase-Assisted Grain Boundary Migration in CuInSe_{2}.

Significant structural evolution occurs during the deposition of CuInSe_{2} solar materials when the Cu content increases. We use in situ heating in a scanning transmission electron microscope to directly observe how grain boundaries migrate during heating, causing nondefected grains to consume highly defected grains. Cu substitutes for In in the near grain boundary regions, turning them into a Cu-Se phase topotactic with the CuInSe_{2} grain interiors. Together with density functional theory and molecular dynamics calculations, we reveal how this Cu-Se phase makes the grain boundaries highly mobile.

CEP dependence of signal and idler upon pump-seed synchronization in optical parametric amplifiers.

We study the effect of pump-seed timing fluctuations on the carrier-envelope phase (CEP) of signal and idler pulses emerging from an OP(CP)A. A simple analytical model is derived in order to provide an intuitive explanation of the origin of CEP fluctuations, while split-step simulations are performed to cover a broad range of different seeding schemes. Finally, we compare the simulation results with real observations of the CEP of idler pulses generated by an OPA. The quantitative model presented provides a key tool for designing the next generation of low-noise CEP-stable OP(CP)A-based sources.

High-dynamic-range arrival time control for flexible, accurate and precise parametric sub-cycle waveform synthesis.

We introduce a simple all-inline variation of a balanced optical cross-correlator (BOC) that allows to measure the arrival time difference (ATD), over the full Nyquist bandwidth, with increased common-mode rejection and long-term stability. An FPGA-based signal processing unit allows for real-time signal normalization and enables locking to any setpoint with an unprecedented accuracy of 0.07 % within an increased ATD range of more than 400 fs, resulting in attosecond resolution locking. The setup precision is verified with an out-of-loop measurement to be less than 80 as residual jitter paving the way for highly demanding applications such as parametric waveform synthesizers.

Traceable Quantitative Raman Microscopy and X-ray Fluorescence Analysis as Nondestructive Methods for the Characterization of Cu(In,Ga)Se2 Absorber Films.

The traceability of measured quantities is an essential condition when linking process control parameters to guaranteed physical properties of a product. Using Raman spectroscopy as an analytical tool for monitoring the production of Cu(In1-xGax)Se2 thin-film solar cells, proper calibration with regard to chemical composition and lateral dimensions is a key prerequisite. This study shows how the multiple requirements of calibration in Raman microscopy might be addressed. The surface elemental composition as well as the integral elemental composition of the samples is traced back by reference-free X-ray fluorescence analysis. Reference Raman spectra are then generated for the relevant Cu(In1-xGax)Se2 related compounds. The lateral dimensions are calibrated with the help of a novel dimensional standard whose regular structures have been traced back to the International System of Units by metrological scanning force microscopy. On this basis, an approach for the quantitative determination of surface coverage values from lateral Raman mappings is developed together with a complete uncertainty budget. Raman and X-ray spectrometry have here been proven as complementary nondestructive methods combining surface sensitivity and in-depth information on elemental and species distribution for the reliable quality control of Cu(In1-xGax)Se2 absorbers and Cu(In1-xGax)3Se5 surface layer formation.

Real-time observation of Cu2ZnSn(S,Se)4 solar cell absorber layer formation from nanoparticle precursors.

The selenization of Cu-Zn-Sn-S nanocrystals is a promising route for the fabrication of low-cost thin film solar cells. However, the reaction pathway of this process is not completely understood. Here, the evolution of phase formation, grain size, and elemental distributions is investigated during the selenization of Cu-Zn-Sn-S nanoparticle precursor thin films by synchrotron-based in situ energy-dispersive X-ray diffraction and fluorescence analysis as well as by ex situ electron microscopy. The precursor films are heated in a closed volume inside a vacuum chamber in the presence of selenium vapor while diffraction and fluorescence signals are recorded. The presented results reveal that during the selenization the cations diffuse to the surface to form large grains on top of the nanoparticle layer and the selenization of the film takes place through two simultaneous reactions: (1) a direct and fast formation of large grained selenides, starting with copper selenide which is subsequently transformed into Cu2ZnSnSe4; and (2) a slower selenization of the remaining nanoparticles. As a consequence of the initial formation of copper selenides at the surface, the subsequent formation of CZTSe starts under Cu-rich conditions despite an overall Cu-poor composition of the film. The implications of this process path for the film quality are discussed. Additionally, the proposed growth model provides an explanation for the previously observed accumulation of carbon from the nanoparticle precursor beneath the large grained layer.