Probing the Low-Energy Electronic Structure of Complex Systems by ARPES

Angle-resolved photoemission spectroscopy (ARPES) is one of the most direct methods of studying the electronic structure of solids. By measuring the kinetic energy and angular distribution of the electrons photoemitted from a sample illuminated with sufficiently high-energy radiation, one can gain information on both the energy and momentum of the electrons propagating inside a material. This is of vital importance in elucidating the connection between electronic, magnetic, and chemical structure of solids, in particular for those complex systems which cannot be appropriately described within the independent-particle picture. The last decade witnessed significant progress in this technique and its applications, thus ushering in a new era in photoelectron spectroscopy; today, ARPES experiments with 2 meV energy resolution and 0.2 degree angular resolution are a reality even for photoemission on solids. In this paper we will review the fundamentals of the technique and present some illustrative experimental results; we will show how ARPES can probe the momentum-dependent electronic structure of solids providing detailed information on band dispersion and Fermi surface, as well as on the strength and nature of those many-body correlations which may profoundly affect the one-electron excitation spectrum and, in turn, determine the macroscopic physical properties.Comment: Lecture notes for the 2003 Exciting Summer School (http://www.fysik4.fysik.uu.se/~thor/school.html). A HIGH-RESOLUTION pdf file is available at http://www.physics.ubc.ca/~damascel/ARPES_Intro.pdf, and related viewgraphs at http://www.physics.ubc.ca/~damascel/Exciting2003.pd

Optical spectroscopy of quantum spin systems

This thesis work illustrates the results obtained on a number of solid crystalline materials using optical spectroscopy. This experimental technique consists of shing light of different frequencies onto the sample under investigation, and of observing which frequencies are absorbed by the material itself. The experiments were performed in the frequency range extending from the far infrared to the ultra violet (i.e., from 4 meV to 4 eV). ... Zie: Summary

Time- and Angle-Resolved Photoemission Studies of Quantum Materials

Angle-resolved photoemission spectroscopy (ARPES) -- with its exceptional sensitivity to both the binding energy and momentum of valence electrons in solids -- provides unparalleled insights into the electronic structure of quantum materials. Over the last two decades, the advent of femtosecond lasers, which can deliver ultrashort and coherent light pulses, has ushered the ARPES technique into the time domain. Now, time-resolved ARPES (TR-ARPES) can probe ultrafast electron dynamics and the out-of-equilibrium electronic structure, providing a wealth of information otherwise unattainable in conventional ARPES experiments. This paper begins with an introduction to the theoretical underpinnings of TR-ARPES followed by a description of recent advances in state-of-the-art ultrafast sources and optical excitation schemes. It then reviews paradigmatic phenomena investigated by TR-ARPES thus far, such as out-of-equilibrium electronic states and their spin dynamics, Floquet-Volkov states, photoinduced phase transitions, electron-phonon coupling, and surface photovoltage effects. Each section highlights TR-ARPES data from diverse classes of quantum materials, including semiconductors, charge-ordered systems, topological materials, excitonic insulators, van der Waals materials, and unconventional superconductors. These examples demonstrate how TR-ARPES has played a critical role in unraveling the complex dynamical properties of quantum materials. The conclusion outlines possible future directions and opportunities for this powerful technique.Comment: To appear in Reviews of Modern Physic

Tracking local magnetic dynamics via high-energy charge excitations in a relativistic Mott insulator

We use time- and energy-resolved optical spectroscopy to investigate the coupling of electron-hole excitations to the magnetic environment in the relativistic Mott insulator Na$_2$IrO$_3$. We show that, on the picosecond timescale, the photoinjected electron-hole pairs delocalize on the hexagons of the Ir lattice via the formation of quasi-molecular orbital (QMO) excitations and the exchange of energy with the short-range-ordered zig-zag magnetic background. The possibility of mapping the magnetic dynamics, which is characterized by typical frequencies in the THz range, onto high-energy (1-2 eV) charge excitations provides a new platform to investigate, and possibly control, the dynamics of magnetic interactions in correlated materials with strong spin-orbit coupling, even in the presence of complex magnetic phases.Comment: 5 pages, 4 figures, supplementary informatio