Polarization-resolved Pump-probe Spectroscopy Research Articles

Violet phosphorus with high-index and low-loss: A promising candidate for nanophotonics applications

The recent synthesis and characterization of violet phosphorus (VP) demonstrate that it is the most stable allotrope of phosphorus, which could become a promising 2D layered semiconductor with potential applications in optoelectronic and electronic devices. However, experiments exploring the complex refractive index or permittivity have yet to be performed, hindering further application access. Due to the small size of the VP crystal sample available by the current growth method, the measurement for the complex refractive index is challenging. In this work, coherent acoustic phonon spectroscopy was performed first in the a–b plane using polarization-resolved pump-probe spectroscopy, revealing negligible anisotropy in the refractive index in the VIS–NIR regime (400–1000 nm). Then, the non-polarized reflectance spectra of VP films with different thicknesses on Si in the VIS–NIR regime were collected. The complex refractive index spectra were obtained by fitting the reflectance spectra with Fresnel's law considering multiple reflections in thin films. It was found that VP has high refractive indices and low extinction coefficients in the spectral range of 560–1000 nm, based on which a metasurface with VP nanodisks could achieve a high reflection band in the VIS–NIR regime by simulation. These results unveil the striking potential of VP for nanophotonics applications.

Nature of hydrated proton vibrations revealed by nonlinear spectroscopy of acid water nanodroplets.

We use polarization-resolved femtosecond pump-probe spectroscopy to investigate the vibrations of hydrated protons in anionic (AOT) and cationic (CTAB/hexanol) reverse micelles in the frequency range 2000-3500 cm-1. For small AOT micelles the dominant proton hydration structure consists of H3O+ with two OH groups donating hydrogen bonds to water molecules, and one OH group donating a weaker hydrogen bond to sulfonate. For cationic reverse micelles, we find that the absorption at frequencies >2500 cm-1 is dominated by asymmetric proton-hydration structures in which one of the OH groups of H3O+ is more weakly hydrogen-bonded to water than the other two OH groups.

Slow Noncollinear Coulomb Scattering in the Vicinity of the Dirac Point in Graphene.

The Coulomb scattering dynamics in graphene in energetic proximity to the Dirac point is investigated by polarization resolved pump-probe spectroscopy and microscopic theory. Collinear Coulomb scattering rapidly thermalizes the carrier distribution in k directions pointing radially away from the Dirac point. Our study reveals, however, that, in almost intrinsic graphene, full thermalization in all directions relying on noncollinear scattering is much slower. For low photon energies, carrier-optical-phonon processes are strongly suppressed and Coulomb mediated noncollinear scattering is remarkably slow, namely on a ps time scale. This effect is very promising for infrared and THz devices based on hot carrier effects.

Polarization-resolved pump–probe spectroscopy with high harmonics

High harmonic generation in gases can be used as a probe of the electronic structure of the emitting medium, with attosecond temporal resolution and angström spatial resolution. The prospect of measuring molecular dynamics by pump–probe spectroscopy with such precision is attracting a lot of interest. An important issue in pump–probe spectroscopy lies in the ability to detect small signals: the detected signal can be easily dominated by the contributions from non-excited molecules or from a carrier gas. In this paper, we demonstrate that polarization-resolved pump–probe spectroscopy can be used to overcome this issue. We study high harmonic generation from rotationally excited molecules. We show that by measuring the harmonic field that is generated orthogonally to the driving laser field, the contrast in the detection of alignment revivals in nitrogen can be increased by a factor 4. We use this configuration to measure alignment revivals in an argon–nitrogen mixture, in which the total harmonic signal is dominated by the contributions from argon.