The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the $a$ and $b$ axes. This feature eliminates the need for uniaxial strain that is usually required to stabilize large single domains in the electronic nematic state that exists in the vicinity of magnetic order in the iron-based superconductors. We report detailed structural symmetry measurements of 112-type Ca$_{0.73}$La$_{0.27}$FeAs$_{2}$ using rotational anisotropy optical second harmonic generation. This technique is complementary to diffraction experiments and enables a precise determination of the point group symmetry of a crystal. By combining our measurements with density functional theory calculations, we uncover a strong optical second harmonic response of bulk electric dipole origin from the Fe and Ca $3d$-derived states that enables us to assign $C_2$ as the crystallographic point group. This makes the 112-type materials high-temperature superconductors without a center of inversion, allowing for the possible mixing of singlet and triplet Cooper pairs in the superconducting state. We also perform pump-probe transient reflectivity experiments that reveal a 4.6 THz phonon mode associated with the out-of-plane motion of As atoms in the FeAs layers. We do not observe any suppression of the optical second harmonic response or shift in the phonon frequency upon cooling through the reported monoclinic-to-triclinic transition at 58 K. This allows us to identify $C_1$ as the low-temperature crystallographic point group but suggests that structural changes induced by long-range magnetic order are subtle and do not significantly affect electronic states near the Fermi level.

We present a method of performing high-speed rotational anisotropy nonlinear optical harmonic generation experiments at rotational frequencies of several hertz by projecting the harmonic light reflected at different angles from a sample onto a stationary position-sensitive detector. The high rotational speed of the technique, 10(3) to 10(4) times larger than existing methods, permits precise measurements of the crystallographic and electronic symmetries of samples by averaging over low frequency laser-power, beam-pointing, and pulse-width fluctuations. We demonstrate the sensitivity of our technique by resolving the bulk fourfold rotational symmetry of GaAs about its [001] axis using second-harmonic generation.

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd₂Re₂O₇ using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of the multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd₂Re₂O₇ and induces a parity-breaking lattice distortion as a secondary order.

Chemical substitution plays a key role in controlling the electronic and magnetic properties of complex materials. For instance, in EuO, carrier doping can induce a spin-polarized metallic state, colossal magnetoresistance, and significantly enhance the Curie temperature. Here, we employ a combination of molecular-beam epitaxy, angle-resolved photoemission spectroscopy, and an effective model calculation to investigate and understand how semi-localized states evolve in lightly electron doped Eu$_{1-x}$Gd$_{x}$O above the ferromagnetic Curie temperature. Our studies reveal a characteristic length scale for the spatial extent of the donor wavefunctions which remains constant as a function of doping, consistent with recent tunneling studies of doped EuO. Our work sheds light on the nature of the semiconductor-to-metal transition in Eu$_{1-x}$Gd$_{x}$O and should be generally applicable for doped complex oxides.

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr_{2}RuO_{4} and its isoelectronic counterpart Ba_{2}RuO_{4} using oxide molecular beam epitaxy, in situ angle-resolved photoemission spectroscopy, and transport measurements. Near the topological transition of the γ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.