We present a novel spectroscopic technique for second harmonic generation (SHG) using femtosecond laser pulses at 30 kHz repetition rate, which nevertheless provides high spectral resolution limited only by the spectrometer. The potential of this method is demonstrated by applying it to the yellow exciton series of Cu2O. Besides even parity states with S− and D− envelope, we also observe odd parity, P − excitons with linewidths down to 100 µeV, despite of the broad excitation laser spectrum with a full width at half maximum of 14 meV. The underlying light-matter interaction mechanisms of SHG are elaborated by a group theoretical analysis which allows us to determine the linear and circular polarization dependences, in good agreement with experiment. arXiv:1806.06854v1 [physics.optics]

The optical properties of colloidal semiconductor nanocrystals are largely influenced by the trapping of charge carriers on the nanocrystal surface. Different concentrations of electron and hole traps and different rates of their capture to the traps provide dynamical charging of otherwise neutral nanocrystals. We study the photocharging formation and evolution dynamics in CdS colloidal quantum dots with native oleic acid surface ligands. A time-resolved technique with three laser pulses (pump, orientation, and probe) is developed to monitor the photocharging dynamics with picosecond resolution on wide time scales ranging from picoseconds to milliseconds. The detection is based on measuring the coherent spin dynamics of electrons, allowing us to distinguish the type of carrier in the QD core (electron or hole). We find that although initially negative photocharging happens because of fast hole trapping, it eventually evolves to positive photocharging due to electron trapping and hole detrapping. The positive photocharging lasts up to hundreds of microseconds at room temperature. These findings give insight into the photocharging process and provide valuable information for understanding the mechanisms responsible for the emission blinking in colloidal nanostructures.

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We report on the experimental and theoretical investigation of magnetic-field-induced second harmonic generation (SHG) and two-photon absorption (TPA) of excited exciton states (n 3) of the yellow series in the cuprous oxide Cu2O. In this centrosymmetric material, SHG can occur due to constructive interplay of electric dipole and electric quadrupole/magnetic dipole transitions for light propagating along the low-symmetry directions [111] or [112]. By application of a magnetic field in Voigt configuration, SHG gets also allowed for excitation along the [110]-axis and even the high-symmetry cubic direction [001]. Combining a symmetry analysis and a microscopic theory, we uncover the two key contributions to the magnetic-field-induced SHG: the Zeeman effect and the magneto-Stark effect. We demonstrate systematic dependencies of the SHG intensity on the linear polarization angles of the ingoing fundamental laser and the outgoing SHG beam, complementary to the manuscript by Rommel et al. [1]. In general, the resulting contour plots in combination with a symmetry analysis allow one to determine uniquely the character of involved transitions. Moreover, we can separate in magnetic field the Zeeman and the magneto-Stark effect through appropriate choice of the experimental geometry and polarization configuration. We present a microscopic theory of the second harmonic generation of excitons in a centrosymmetric cubic semiconductor taking into account the symmetry and the band structure of cuprous oxide. Based on the developed microscopic theory we identify the main contributions to the second-order nonlinear susceptibility of S-, P -and D-excitons. We analyze the redistribution of SHG intensities between the excitonic states both in the absence and presence of the magnetic field and show good agreement with the experimental data. With increasing exciton principal quantum number the magneto-Stark effect overpowers the influence of the Zeeman effect. arXiv:2002.11560v1 [cond-mat.mes-hall]

Recently Second Harmonic Generation (SHG) for the yellow exciton series in cuprous oxide has been demonstrated [J. Mund et al., Phys. Rev. B 98, 085203 (2018)]. Assuming perfect O h symmetry, SHG is forbidden along certain high-symmetry axes. Perturbations can break this symmetry and forbidden transitions may become allowed. We investigate theoretically the effect of external magnetic fields on the yellow exciton lines of cuprous oxide. We identify two mechanisms by which an applied magnetic field can induce a second harmonic signal in a forbidden direction. First of all, a magnetic field by itself generally lifts the selection rules. In the Voigt configuration, an additional magneto-Stark electric field appears. This also induces certain SHG processes differing from those induced by the magnetic field alone. Complementary to the manuscript by A. Farenbruch et al. [Phys. Rev. B, submitted], we perform a full numerical diagonalization of the exciton Hamiltonian including the complex valence band structure. Numerical results are compared with experimental data. :2002.12064v1 [cond-mat.mes-hall] arXiv