Polarization- and time-resolved nonlinear multi-photon spectroscopy for confocal microscopy of semiconductor nanostructures

We present a versatile confocal microscopy setup for optical second harmonic generation (SHG) and multi-photon spectroscopy that enables polarization-resolved studies of semiconductor bulk crystals and low-dimensional structures. The setup offers full polarization control in both excitation and detection, spatial scanning with micrometer resolution, and spectrally tunable excitation over a broad energy range from 0.5 to 4.0 eV, using femtosecond and picosecond laser pulses. Samples are mounted in a helium-flow cryostat, allowing temperature control from 4 to 300 K. Magnetic fields up to 0.625 T can be applied in the Voigt geometry using an electromagnet. The nonlinear optical signals are analyzed using a high-resolution spectrometer with a spectral resolution of 60 μeV. We demonstrate the potential of the setup by means of SHG polarization tomography measurements on a Cu2O crystal and through a SHG spectral scan of a ZnSe crystal over a wide energy range from 1.4 to 3.1 eV. Polarization-resolved confocal SHG mapping of various twisted mono- and bilayer MoS2 structures is also presented. In addition, time-resolved two-color pump–probe experiments are shown for a Cs2AgBiBr6 crystal, illustrating the potential of the system for investigating coherent exciton and phonon dynamics.