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  1. Abstract

    The future of modern optoelectronics and spintronic devices relies on our ability to control the spin and charge degrees of freedom at ultrafast timescales. Rashba spin-split quantum well states, 2D states that develop at the surface of strong spin-orbit coupling materials, are ideal given the tunability of their energy and spin states. So far, however, most studies have only demonstrated such control in a static way. In this study, we demonstrate control of the spin and energy degrees of freedom of surface quantum well states on Bi2Se3at picosecond timescales. By means of a focused laser pulse, we modulate the band-bending, producing picosecond time-varying electric fields at the material’s surface, thereby reversibly modulating the quantum well spectrum and Rashba effect. Moreover, we uncover a dynamic quasi-Fermi level, dependent on the Lifshitz transition of the second quantum well band bottom. These results open a pathway for light-driven spintronic devices with ultrafast switching of electronic phases, and offer the interesting prospect to extend this ultrafast photo-gating technique to a broader host of 2D materials.

  2. Metal-metal bonding interactions can engender outstanding magnetic properties in bulk materials and molecules, and examples abound for the transition metals. Extending this paradigm to the lanthanides, herein we report mixed-valence dilanthanide complexes (Cp iPr5 ) 2 Ln 2 I 3 (Ln is Gd, Tb, or Dy; Cp i Pr5 , pentaisopropylcyclopentadienyl), which feature a singly occupied lanthanide-lanthanide σ-bonding orbital of 5 d z 2 parentage, as determined by structural, spectroscopic, and computational analyses. Valence delocalization, wherein the d electron is equally shared by the two lanthanide centers, imparts strong parallel alignment of the σ-bonding and f electrons on both lanthanides according to Hund’s rules. The combination of a well-isolated high-spin ground state and large magnetic anisotropy in (Cp iPr5 ) 2 Dy 2 I 3 gives rise to an enormous coercive magnetic field with a lower bound of 14 tesla at temperatures as high as 60 kelvin.
    Free, publicly-accessible full text available January 14, 2023
  3. The theory behind the electrical switching of antiferromagnets is premised on the existence of a well-defined broken symmetry state that can be rotated to encode information. A spin glass is, in many ways, the antithesis of this state, characterized by an ergodic landscape of nearly degenerate magnetic configurations, choosing to freeze into a distribution of these in a manner that is seemingly bereft of information. Here, we show that the coexistence of spin glass and antiferromagnetic order allows a novel mechanism to facilitate the switching of the antiferromagnet Fe 1/3 + δ NbS 2 , rooted in the electrically stimulated collective winding of the spin glass. The local texture of the spin glass opens an anisotropic channel of interaction that can be used to rotate the equilibrium orientation of the antiferromagnetic state. Manipulating antiferromagnetic spin textures using a spin glass’ collective dynamics opens the field of antiferromagnetic spintronics to new material platforms with complex magnetic textures.
  4. Abstract

    The appearance of topologically protected spin-momentum locked surface states in topological insulators gives rise to robust room temperature spin currents making them ideal candidates for the realization of spintronic devices. New methods are needed to access and manipulate such currents with timescales that are compatible with modern electronics. Here we reveal that an optically induced long-lived (~10 ns), spin-polarized surface state excitation in topological insulators can be easily tuned in both magnitude and duration. Time-resolved angle-resolved photoemission spectroscopy, together with a quantitative model, reveals the ideal conditions for a surface photovoltage in two different topological insulators. Our model predicts that the reported effects are an intrinsic property of topological insulators, as long as the chemical potential falls within the band gap. This work demonstrates that persistent excited topological surface states are photon-accessible and easily tuned in both magnitude and duration, merging photonics- and spintronics-based devices in the same material.

  5. Abstract

    Co$$_{3}$$3Sn$$_{2}$$2S$$_{2}$$2is a ferromagnetic Weyl semimetal that has been the subject of intense scientific interest due to its large anomalous Hall effect. We show that the coupling of this material’s topological properties to its magnetic texture leads to a strongly exchange biased anomalous Hall effect. We argue that this is likely caused by the coexistence of ferromagnetism and geometric frustration intrinsic to the kagome network of magnetic ions, giving rise to spin-glass behavior and an exchange bias.