Polarization-Resolved Extreme-Ultraviolet Second-Harmonic Generation from LiNbO_{3}.

Second harmonic generation (SHG) spectroscopy ubiquitously enables the investigation of surface chemistry, interfacial chemistry, as well as symmetry properties in solids. Polarization-resolved SHG spectroscopy in the visible to infrared regime is regularly used to investigate electronic and magnetic order through their angular anisotropies within the crystal structure. However, the increasing complexity of novel materials and emerging phenomena hampers the interpretation of experiments solely based on the investigation of hybridized valence states. Here, polarization-resolved SHG in the extreme ultraviolet (XUV-SHG) is demonstrated for the first time, enabling element-resolved angular anisotropy investigations. In noncentrosymmetric LiNbO_{3}, elemental contributions by lithium and niobium are clearly distinguished by energy dependent XUV-SHG measurements. This element-resolved and symmetry-sensitive experiment suggests that the displacement of Li ions in LiNbO_{3}, which is known to lead to ferroelectricity, is accompanied by distortions to the Nb ion environment that breaks the inversion symmetry of the NbO_{6} octahedron as well. Our simulations show that the measured second harmonic spectrum is consistent with Li ion displacements from the centrosymmetric position while the Nb─O bonds are elongated and contracted by displacements of the O atoms. In addition, the polarization-resolved measurement of XUV-SHG shows excellent agreement with numerical predictions based on dipole-induced SHG commonly used in the optical wavelengths. Our result constitutes the first verification of the dipole-based SHG model in the XUV regime. The findings of this work pave the way for future angle and time-resolved XUV-SHG studies with elemental specificity in condensed matter systems.

Ultrafast Subpicosecond Magnetization of a 2D Ferromagnet.

Strong spin-charge interactions in several ferromagnets are expected to lead to subpicosecond (sub-ps) magnetization of the magnetic materials through control of the carrier characteristics via electrical means, which is essential for ultrafast spin-based electronic devices. Thus far, ultrafast control of magnetization has been realized by optically pumping a large number of carriers into the d or f orbitals of a ferromagnet; however, it is extremely challenging to implement by electrical gating. This work demonstrates a new method for sub-ps magnetization manipulation called wavefunction engineering, in which only the spatial distribution (wavefunction) of s (or p) electrons is controlled and no change is required in the total carrier density. Using a ferromagnetic semiconductor (FMS) (In,Fe)As quantum well (QW), instant enhancement, as fast as 600 fs, of the magnetization is observed upon irradiating a femtosecond (fs) laser pulse. Theoretical analysis shows that the instant enhancement of the magnetization is induced when the 2D electron wavefunctions (WFs) in the FMS QW are rapidly moved by a photo-Dember electric field formed by an asymmetric distribution of the photocarriers. Because this WF engineering method can be equivalently implemented by applying a gate electric field, these results open a new way to realize ultrafast magnetic storage and spin-based information processing in present electronic systems.