Optically Addressing Exciton Spin and Pseudospin in Nanomaterials for Spintronics Applications.

Oriented exciton spins that can be generated and manipulated optically are of interest for a range of applications, including spintronics, quantum information science, and neuromorphic computing architectures. Although materials that host such excitons often lack practical coherence times for use on their own, strategic transduction of the magnetic information across interfaces can combine fast modulation with longer-term storage and readout. Several nanostructure systems have been put forward due to their interesting magneto-optical properties and their possible manipulation using circularly polarized light. These material systems are presented here, namely two-dimensional (2D) systems due to the unique spin-valley coupling properties and quantum dots for their exciton fine structure. 2D magnets are also discussed for their anisotropic spin behavior and extensive 2D magnetic states that are not yet fully understood but could pave the way for emergent techniques of magnetic control. This review also details the experimental and theoretical tools to measure and understand these systems along with a discussion on the progress of optical manipulation of spins and magnetic order transitions.

Hyperbolic exciton polaritons in a van der Waals magnet.

Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

A theory for colors of strongly correlated electronic systems.

Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters-a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF2 with pink color, and employ two kinds of ab initio many body Green's function theories; the first, a perturbative theory based on low-order extensions of the GW approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF2 is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how 'bright' these excitons are, but they are not fundamental to their existence.

Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS3.

Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

Controlling T_{c} through Band Structure and Correlation Engineering in Collapsed and Uncollapsed Phases of Iron Arsenides.

Recent observations of selective emergence (suppression) of superconductivity in the uncollapsed (collapsed) tetragonal phase of LaFe_{2}As_{2} has rekindled interest in understanding what features of the band structure control the superconducting T_{c}. We show that the proximity of the narrow Fe-d_{xy} state to the Fermi energy emerges as the primary factor. In the uncollapsed phase this state is at the Fermi energy, and is most strongly correlated and a source of enhanced scattering in both single and two particle channels. The resulting intense and broad low energy spin fluctuations suppress magnetic ordering and simultaneously provide glue for Cooper pair formation. In the collapsed tetragonal phase, the d_{xy} state is driven far below the Fermi energy, which suppresses the low-energy scattering and blocks superconductivity. A similar source of broad spin excitation appears in uncollapsed and collapsed phases of CaFe_{2}As_{2}. This suggests controlling coherence provides a way to engineer T_{c} in unconventional superconductors primarily mediated through spin fluctuations.

Electron-phonon-driven three-dimensional metallicity in an insulating cuprate.

The role of the crystal lattice for the electronic properties of cuprates and other high-temperature superconductors remains controversial despite decades of theoretical and experimental efforts. While the paradigm of strong electronic correlations suggests a purely electronic mechanism behind the insulator-to-metal transition, recently the mutual enhancement of the electron-electron and the electron-phonon interaction and its relevance to the formation of the ordered phases have also been emphasized. Here, we combine polarization-resolved ultrafast optical spectroscopy and state-of-the-art dynamical mean-field theory to show the importance of the crystal lattice in the breakdown of the correlated insulating state in an archetypal undoped cuprate. We identify signatures of electron-phonon coupling to specific fully symmetric optical modes during the buildup of a three-dimensional (3D) metallic state that follows charge photodoping. Calculations for coherently displaced crystal structures along the relevant phonon coordinates indicate that the insulating state is remarkably unstable toward metallization despite the seemingly large charge-transfer energy scale. This hitherto unobserved insulator-to-metal transition mediated by fully symmetric lattice modes can find extensive application in a plethora of correlated solids.

Feasibility of a metamagnetic transition in correlated systems.

The long-standing issue of the competition between the magnetic field and the Kondo effect, favoring, respectively, triplet and singlet ground states, is addressed using a cluster slave-rotor mean-field theory for the Hubbard model and its spin-correlated, spin-frustrated extensions in two dimensions. The metamagnetic jump is established and compared with earlier results of dynamical mean-field theory. This approach also reproduces the emergent super-exchange energy scale in the insulating side. A scaling is found for the critical Zeeman field in terms of the intrinsic coherence scale just below the metal-insulator transition, where the critical spin fluctuations are soft. The conditions required for metamagnetism to appear at a reasonable field are also underlined. Gutzwiller analysis on the two-dimensional Hubbard model and a quantum Monte Carlo calculation on the Heisenberg spin system are performed to check the limiting cases of the cluster slave-rotor results for the Hubbard model. Low-field scaling features for magnetization are discussed.