Abstract: Unraveling the exact nature of nonequilibrium and correlated interactions is paramount for continued progress in many areas of condensed matter science. Such insight is a prerequisite to develop an engineered approach for smart materials with targeted properties designed to address standing needs such as efficient light harvesting, energy storage, or information processing. For this goal, it is critical to unravel the dynamics of the energy conversion processes between carriers in the earliest time scales of the excitation dynamics. We discuss the implementation and benefits of attosecond soft x-ray core-level spectroscopy up to photon energies of 600 eV for measurements in solid-state systems. In particular, we examine how the pairing between coherent spectral coverage and temporal resolution provides a powerful new insight into the quantum dynamic interactions that determine the macroscopic electronic and optical response. We highlight the different building blocks of the methodology and point out the important aspects for its application from condensed matter studies to materials as thin as 25 nm. Furthermore,we discuss the technological developments in the field of tabletop attosecond soft x-ray sources with time-resolved measurements at the near and extended edge simultaneously and investigate the exciting prospective of extending such technique to the study of 2-dimensional materials.
Abstract: A universal mechanism of ultrafast 2-electron orbital swap is discovered through 2-photon sequential double ionization of Li. After a 1s electron in Li is ionized by absorbing an extreme ultraviolet photon, the other 2 bound electrons located on 2 different shells have either parallel or antiparallel spin orientations.In the latter case, these 2 electrons are in the superposition of the singlet and triplet states with different energies, forming a quantum beat and giving rise to the 2-electron orbital swap with a period of several hundred attoseconds. The orbital swap mechanism can be used to manipulate the spin polarization of photoelectron pairs by conceiving the attosecond-pump attosecond-probe strategy and thus serves as a knob to control spin-resolved multielectron ultrafast dynamics.
Abstract: Ultrafast extreme ultraviolet (XUV) transient absorption spectroscopy measures the time- and frequencydependent light losses after light–matter interactions. In the linear region, the matter response to an XUV light field is usually determined by the complex refractive index ̃n. The absorption signal is directly related to the imaginary part of ̃n, namely, the absorption index. The real part of ̃n refers to the real refractive index, which describes the chromatic dispersion of an optical material. However, the real refractive index information is usually not available in conventional absorption experiments. Here, we investigate the refractive index line shape in ultrafast XUV transient absorption spectroscopy by using a scheme that the XUV pulse traverses the target gas jet off-center. The jet has a density gradient in the direction perpendicular to the gas injection direction, which induces deflection on the XUV radiation. Our experimental and theoretical results show that the shape of the frequency-dependent XUV deflection spectra reproduces the refractive index line profile. A typical dispersive refractive index line shape is measured for a single-peak absorption; an additional shoulder structure appears for a doublet absorption.Moreover, the refractive index line shape is controlled by introducing a later-arrived near-infrared pulse to modify the phase of the XUV free induction decay, resulting in different XUV deflection spectra. The results promote our understanding of matter-induced absorption and deflection in ultrafast XUV spectroscopy.
Abstract: Optical logic gates call for materials with giant optical nonlinearity to break the current performance bottleneck. Metal–organic frameworks (MOFs) provide an intriguing route to achieve superior optical nonlinearity benefitting from structural diversity and design flexibility. However, the potential of MOFs for optoelectronics has been largely overlooked and their applications in optical logic have not been exploited. Here, through temporally manipulating the nonlinear optical absorption process in porphyrin-based MOFs, we have successfully developed AND and XOR logic gates with an ultrafast speed approaching 1 THz and an on–off ratio above 90%. On this basis, all-optical information encryption is further demonstrated using transmittance as primary codes, which shows vast prospects in avoiding the disclosure of security information. To the best of our knowledge, this is the first exploration of MOFs for applications in ultrafast optical logic devices and information encryption.