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We recently published a study concerning femtosecond pump–probe absorption edge spectroscopy of cubic GaN (fundamental bandgap: 3.23 eV), resulting in the transient dielectric function. In the present study, we continue our investigations of those pump–probe measurements by determining the time-dependent transition energy at the Fermi-vector between the conduction and valence bands. The generation of electron–hole pairs by the 266 nm pump-beam (4.66 eV) shifts the absorption edge by ≈ 500 meV within 1 ps due to many-body effects like band-filling and bandgap renormalization. Modeling this ultra-fast change is achieved by converting the transition energies into free-carrier concentrations, assuming the electron contributions to be dominant. We consider the relaxation, recombination, and diffusion of those free-carriers as well as either an additional gain-recombination or temperature effects. This allows for describing the transition energies on short time scales. Both models yield similar values for the characteristic relaxation time (≈ 0.21 ps), recombination time (≈ 25 ps), and diffusion coefficient (≈ 1 cm 2 /s). [ABSTRACT FROM AUTHOR]

An ultra-fast change of the absorption onset for zincblende gallium-nitride (zb-GaN) (fundamental bandgap: 3.23 eV) is observed by investigating the imaginary part of the dielectric function using time-dependent femtosecond pump–probe spectroscopic ellipsometry between 2.9 and 3.7 eV. The 266 nm (4.66 eV) pump pulses induce a large electron–hole pair concentration up to 4 × 10 20 cm − 3 , which shift the transition energy between conduction and valence bands due to many-body effects up to ≈ 500 meV. Here, the absorption onset increases due to band filling while the bandgap renormalization at the same time decreases the bandgap. Additionally, the absorption of the pump-beam creates a free-carrier profile within the 605 nm zb-GaN layer with high free-carrier concentrations at the surface, and low concentrations at the interface to the substrate. This leads to varying optical properties from the sample surface (high transition energy) to substrate (low transition energy), which are taken into account by grading analysis for an accurate description of the experimental data. For this, a model describing the time- and position-dependent free-carrier concentration is formulated by considering the relaxation, recombination, and diffusion of those carriers. We provide a quantitative analysis of optical experimental data (ellipsometric angles Ψ and Δ) as well as a plot for the time-dependent change of the imaginary part of the dielectric function. [ABSTRACT FROM AUTHOR]

Herein, the complex pseudodielectric function of Ge and Si from femtosecond pump–probe spectroscopic ellipsometry with 267, 400, and 800 nm pump–pulse wavelengths is analyzed by fitting analytical lineshapes to the second derivatives of the pseudodielectric function with respect to energy. This yields the critical point parameters (threshold energy, lifetime broadening, amplitude, and excitonic phase angle) of E1 and E1+Δ1 in Ge and E1 in Si as functions of delay time. Coherent longitudinal acoustic phonon oscillations with a period of about 11 ps are observed in the transient critical point parameters of Ge. From the amplitude of these oscillations, the laser‐induced strain is found to be on the order of 0.03% for Ge measured with the 800 nm pump pulse, which is in reasonable agreement with the strain calculated from theory. [ABSTRACT FROM AUTHOR]

We present a setup for time-resolved spectroscopic ellipsometry in a pump–probe scheme using femtosecond laser pulses. As a probe, the system deploys supercontinuum white light pulses that are delayed with respect to single-wavelength pump pulses. A polarizer–sample–compensator–analyzer configuration allows ellipsometric measurements by scanning the compensator azimuthal angle. The transient ellipsometric parameters are obtained from a series of reflectance-difference spectra that are measured for various pump–probe delays and polarization (compensator) settings. The setup is capable of performing time-resolved spectroscopic ellipsometry from the near-infrared through the visible to the near-ultraviolet spectral range at 1.3 eV–3.6 eV. The temporal resolution is on the order of 100 fs within a delay range of more than 5 ns. We analyze and discuss critical aspects such as fluctuations of the probe pulses and imperfections of the polarization optics and present strategies deployed for circumventing related issues. [ABSTRACT FROM AUTHOR]