Electronic correlations could have significant impact on the material properties. They are typically pronounced for localized orbitals and enhanced in low-dimensional systems, so two-dimensional (2D) transition metal compounds could be a good platfor
m to study their effects. Recently, a new class of 2D transition metal compounds, the MoSi$_2$N$_4$-family materials, have been discovered, and some of them exhibit intrinsic magnetism. Here, taking monolayer VSi$_{2}$P$_{4}$ as an example from the family, we investigate the impact of correlation effects on its physical properties, based on the first-principles calculations. We find that different correlation strength can drive the system into a variety of interesting ground states, with rich magnetic, topological and valley features. With increasing correlation strength, while the system favors a ferromagnetic semiconductor state for most cases, the magnetic anisotropy and the band gap type undergo multiple transitions, and in the process, the band edges can form single, two or three valleys for electrons or holes. Remarkably, there is a quantum anomalous Hall (QAH) insulator phase, which has a unit Chern number. The boundary of the QAH phase correspond to the half-valley semimetal state with fully valley polarized bulk carriers. We further show that for phases with the out-of-plane magnetic anisotropy, the interplay between spin-orbit coupling and orbital character of valleys enable an intrinsic valley polarization for electrons but not for holes. This electron valley polarization can be switched by reversing the magnetization direction, providing a new route of magnetic control of valleytronics. Our result sheds light on the possible role of correlation effects in the 2D transition metal compounds, and it will open new perspectives for spintronic, valleytronic and topological nanoelectronic applications based on these materials.
Measuring the photoionization time delay between electrons from different orbitals is one of the most important accomplishments of attosecond science. These measurements are typically done using attosecond pulses to photoionize a target inside a phot
oelectron spectrometer. In such experiments, the measured delay corresponds to the superposition of all possible paths to ionization and can include multiple sources of delay. These effects can be difficult to deconvolve. Here, we exploit the collision physics nature of recollision and show that, by perturbing recollision dynamics, photorecombination time delays due to electron dynamics and structure can be measured entirely optically and without obfuscation from molecular structure and propagation effects. While we concentrate on photorecombination delays in argon around the Cooper minimum our approach is general. Therefore, our work holds the potential to fundamentally change how attosecond measurement is performed and paves the way for the entirely optical measurement of ultrafast electron dynamics and photorecombination delays due to electronic structure, multielectron interaction, and strong-field driven dynamics in complex molecular systems and correlated solid-state systems.
Measuring the delay for an electron to emerge from different states is one of the major achievements of attosecond science. This delay can have two origins - the electron wave packet is reshaped during departure by the electrostatic field of the ioni
zing medium or it is modified by dynamic interaction with the remaining electrons. Most experiments have observed the former, but confirmation requires a complex calculation. A direct measurement of multielectron dynamics is needed. Photo-recombination - the inverse of photoionization - occurs naturally during electron recollision and can be measured by combining a perturbing beam to modify the recollision electron before recombination. These in situ methods allow us to unambiguously isolate multielectron dynamics - the reference being the spectral phase of an attosecond pulse simultaneously measured in spectral regions without multielectron interaction. Here, we measure the group delay of the recollision electron caused by plasmonic resonance dynamics in Xe, simulate the in situ measured spectral phase of a recollision electron generated in the presence of the plasmonic resonance in C$_{60}$ and present a corresponding semi-classical theory based on the strong-field approximation. Our results suggest that in situ techniques, together with 300 eV recollision electrons, will allow the ultimate time response of electronic matter to be measured.
Multiphoton-ionized electrons are born into a strong light field that will determine their short-term future. By controlling the infrared beam, we enable atoms or molecules to generate extreme ultraviolet (XUV) pulses and synthesize attosecond pulses
- the shortest controlled events ever produced. Here we show that a weak obliquely incident beam imposes an optical grating on the fundamental beam, resulting in a spatially modulated attosecond pulse. We observe the modulation on a spectrally resolved near-field XUV image, encoding all information of the spectral phase of the recollision electron and, therefore, the attosecond pulse produced by structureless atoms. Near-field imaging is an efficient method for measuring the duration of attosecond pulses, especially important for soft X-ray pulses created in helium. For more complex systems, it includes auto ionization and giant plasmon resonances.
When intense light irradiates a quantum system, an ionizing electron recollides with its parent ion within the same light cycle and, during that very brief (few femtosecond) encounter, its kinetic energy sweeps from low to high energy and back. There
fore, recollision offers unprecedented time resolution and it is the foundation on which attosecond science is built. For simple systems, recolliding trajectories are shaped by the strong field acting together with the Coulomb potential and they can be readily calculated and measured. However, for more complex systems, multielectron effects are also important because they dynamically alter the recolliding wave packet trajectories. Here, we theoretically study Fano resonances, one of the most accessible multielectron effects, and we show how multielectron dynamics can be unambiguously isolated when we use in situ measurement. The general class of in situ measurement can provide key information needed for time-dependent ab initio electronic structure theory and will allow us to measure the ultimate time response of matter.
