We demonstrate time-domain sampling of mid-infrared electric field transients and their conjugate counterparts exploiting the dynamical Pockels effect. To this end, the complete polarization change of few-femtosecond probe pulses is studied. An intuitive picture based on a phasor representation is established before gaining quantitative understanding in experiment and theory. In the standard version of electro-optic sampling, the electric field is determined by analyzing the change of ellipticity of the probe polarization. Beyond this, we find that a temporal gradient of the input electric field manifests itself in a rotation of the polarization ellipsoid of the probe. The relative contribution of sum-and difference-frequency mixing processes and their spectral distribution over the near-infrared probe bandwidth are identified as key aspects. If one of these processes dominates, detecting ellipticity changes and polarization rotation as a function of time delay results in two wave forms which are Hilbert transforms of each other. Such conditions may be achieved by angle phase matching in birefringent materials or spectral filtering of the probe after the nonlinear interaction. In this case, a static phase introduced by birefringence or reflection at metallic mirrors results in a specific phase shift of both time traces with respect to the input electric field. Contributions from sum-and difference-frequency generation are found to be equivalent when using electro-optic sensors with isotropic refractive index. Polarization rotations in the lowand high-frequency parts of the probe then tend to cancel out. In this limit, spurious additional phase shifts do not change the phase of the detected transients. This fact leads to a robust recovery of the carrier-envelope phase of the input wave form. Clarifying the role of imperfections of superachromatic phase retarders completes our survey on proper determination of the electric field and its conjugate variable.

Hybrid organic-inorganic heterointerfaces in solar cells suffer from inefficient charge separation yet the origin of performance limitations are widely unknown. In this work, we focus on the role of metal oxide-polymer interface energetics in a charge generation process. For this purpose, we present novel benzothiadiazole based thiophene oligomers that tailor the surface energetics of the inorganic acceptor TiO2 systematically. In a simple bilayer structure with the donor polymer poly(3-hexylthiophene) (P3HT), we are able to improve the charge generation process considerably. By means of an electronic characterization of solar cell devices in combination with ultrafast broadband transient absorption spectroscopy, we demonstrate that this remarkable improvement in performance originates from reduced recombination of localized charge transfer states. In this context, fundamental design rules for interlayers are revealed, which assist the charge separation at organic-inorganic interfaces. Beside acting as a physical spacer in between electrons and holes, interlayers should offer (1) a large energy offset to drive exciton dissociation, (2) a push-pull building block to reduce the Coulomb binding energy of charge transfer states and (3) an energy cascade to limit carrier back diffusion towards the interface.

The nonlinear transformation of fluctuations by frequency broadening is found to produce strong anti-correlations in the spectral output. This effect is investigated by dispersive Fourier transform measurements. We exploit the anti-correlations in order to cancel the intensity noise in a subsequent sum-frequency mixing step. This principle allows for the generation of tunable visible pulses by cascaded nonlinear mixing whilst maintaining the same intensity noise performance as the input pulses. In addition, we demonstrate that the power fluctuations occurring in the process of passive stabilization of the carrier-envelope phase locking via difference frequency generation may be cancelled by an analogous strategy.

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