2019, Luo, Yongkang, Pustogow, A., Guzman, P., Dioguardi, A.P., Thomas, S.M., Ronning, F., Kikugawa, N., Sokolov, D.A., Jerzembeck, F., Mackenzie, A.P., Hicka, C.W., Bauer, E.D., Mazin, I.I., Brown, S.E.

The effects of uniaxial compressive stress on the normal state O17 nuclear-magnetic-resonance properties of the unconventional superconductor Sr2RuO4 are reported. The paramagnetic shifts of both planar and apical oxygen sites show pronounced anomalies near the nominal a-axis strain μaaμv that maximizes the superconducting transition temperature Tc. The spin susceptibility weakly increases on lowering the temperature below T≃10 K, consistent with an enhanced density of states associated with passing the Fermi energy through a van Hove singularity. Although such a Lifshitz transition occurs in the γ band formed by the Ru dxy states hybridized with in-plane O pπ orbitals, the large Hund's coupling renormalizes the uniform spin susceptibility, which, in turn, affects the hyperfine fields of all nuclei. We estimate this "Stoner" renormalization S by combining the data with first-principles calculations and conclude that this is an important part of the strain effect, with implications for superconductivity. © 2019 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the »https://creativecommons.org/licenses/by/4.0/» Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

2018-6-18, Gradl, C., Winkler, R., Kempf, M., Holler, J., Schuh, D., Bougeard, D., Hernández-Mínguez, A., Biermann, K., Santos, P.V., Schüller, C., Korn, T.

The complex structure of the valence band in many semiconductors leads to multifaceted and unusual properties for spin-3/2 hole systems compared to common spin-1/2 electron systems. In particular, two-dimensional hole systems show a highly anisotropic Zeeman interaction. We have investigated this anisotropy in GaAs/AlAs quantum well structures both experimentally and theoretically. By performing time-resolved Kerr rotation measurements, we found a nondiagonal tensor g that manifests itself in unusual precessional motion, as well as distinct dependencies of hole-spin dynamics on the direction of the magnetic field B. We quantify the individual components of the tensor g for [113]-, [111]-, and [110]-grown samples. We complement the experiments by a comprehensive theoretical study of Zeeman coupling in in-plane and out-of-plane fields B. To this end, we develop a detailed multiband theory for the tensor g. Using perturbation theory, we derive transparent analytical expressions for the components of the tensor g that we complement with accurate numerical calculations based on our theoretical framework. We obtain very good agreement between experiment and theory. Our study demonstrates that the tensor g is neither symmetric nor antisymmetric. Opposite off-diagonal components can differ in size by up to an order of magnitude. The tensor g encodes not only the Zeeman energy splitting but also the direction of the axis about which the spins precess in the external field B. In general, this axis is not aligned with B. Hence our study extends the general concept of optical orientation to the regime of nontrivial Zeeman coupling.

2015, Trabattoni, A., Klinker, M., González-Vázquez, J., Liu, C., Sansone, G., Linguerri, R., Hochlaf, M., Klei, J., Vrakking, M. J. J., Martín, F., Nisoli, M., Calegari, F.

Studying the interaction of molecular nitrogen with extreme ultraviolet (XUV) radiation is of prime importance to understand radiation-induced processes occurring in Earth’s upper atmosphere. In particular, photoinduced dissociation dynamics involving excited states of N2+ leads to N and N+ atomic species that are relevant in atmospheric photochemical processes. However, tracking the relaxation dynamics of highly excited states of N2+ is difficult to achieve, and its theoretical modeling is notoriously complex. Here, we report on an experimental and theoretical investigation of the dissociation dynamics of N2+ induced by isolated attosecond XUV pulses in combination with few-optical-cycle near-infrared/visible (NIR/VIS) pulses. The momentum distribution of the produced N+ fragments is measured as a function of pump-probe delay with subfemtosecond resolution using a velocity map imaging spectrometer. The time-dependent measurements reveal the presence of NIR/VIS-induced transitions between N2+ states together with an interference pattern that carries the signature of the potential energy curves activated by the XUV pulse. We show that the subfemtosecond characterization of the interference pattern is essential for a semiquantitative determination of the repulsive part of these curves.

2017, Rose, B.C., Tyryshkin, A.M., Riemann, H., Abrosimov, N.V., Becker, P., Pohl, H.-J., Thewalt, M.L.W., Itoh, K.M., Lyon, S.A.

We achieve the strong-coupling regime between an ensemble of phosphorus donor spins in a highly enriched 28Si crystal and a 3D dielectric resonator. Spins are polarized beyond Boltzmann equilibrium using spin-selective optical excitation of the no-phonon bound exciton transition resulting in N=3.6×1013 unpaired spins in the ensemble. We observe a normal mode splitting of the spin-ensemble–cavity polariton resonances of 2g√N=580  kHz (where each spin is coupled with strength g) in a cavity with a quality factor of 75 000 (γ≪κ≈60  kHz, where γ and κ are the spin dephasing and cavity loss rates, respectively). The spin ensemble has a long dephasing time (T∗2=9  μs) providing a wide window for viewing the dynamics of the coupled spin-ensemble–cavity system. The free-induction decay shows up to a dozen collapses and revivals revealing a coherent exchange of excitations between the superradiant state of the spin ensemble and the cavity at the rate g√N. The ensemble is found to evolve as a single large pseudospin according to the Tavis-Cummings model due to minimal inhomogeneous broadening and uniform spin-cavity coupling. We demonstrate independent control of the total spin and the initial Z projection of the psuedospin using optical excitation and microwave manipulation, respectively. We vary the microwave excitation power to rotate the pseudospin on the Bloch sphere and observe a long delay in the onset of the superradiant emission as the pseudospin approaches full inversion. This delay is accompanied by an abrupt π-phase shift in the peusdospin microwave emission. The scaling of this delay with the initial angle and the sudden phase shift are explained by the Tavis-Cummings model.

2019, Hubert, Colin, Baruchi, Yifat, Mazuz-Harpaz, Yotam, Cohen, Kobi, Biermann, Klaus, Lemeshko, Mikhail, West, Ken, Pfeiffer, Loren, Rapaport, Ronen, Santos, Paulo

Dipolar coupling plays a fundamental role in the interaction between electrically or magnetically polarized species such as magnetic atoms and dipolar molecules in a gas or dipolar excitons in the solid state. Unlike Coulomb or contactlike interactions found in many atomic, molecular, and condensed-matter systems, this interaction is long-ranged and highly anisotropic, as it changes from repulsive to attractive depending on the relative positions and orientation of the dipoles. Because of this unique property, many exotic, symmetry-breaking collective states have been recently predicted for cold dipolar gases, but only a few have been experimentally detected and only in dilute atomic dipolar Bose-Einstein condensates. Here, we report on the first observation of attractive dipolar coupling between excitonic dipoles using a new design of stacked semiconductor bilayers. We show that the presence of a dipolar exciton fluid in one bilayer modifies the spatial distribution and increases the binding energy of excitonic dipoles in a vertically remote layer. The binding energy changes are explained using a many-body polaron model describing the deformation of the exciton cloud due to its interaction with a remote dipolar exciton. The surprising nonmonotonic dependence on the cloud density indicates the important role of dipolar correlations, which is unique to dense, strongly interacting dipolar solid-state systems. Our concept provides a route for the realization of dipolar lattices with strong anisotropic interactions in semiconductor systems, which open the way for the observation of theoretically predicted new and exotic collective phases, as well as for engineering and sensing their collective excitations.

2022, Schweika, W., Valldor, M., Reim, J.D., Rößler, U.K.

A chiral spin liquid state is discovered in the highly frustrated, noncentrosymmetric swedenborgite compound YBaCo3FeO7, a layered kagome system of hexagonal symmetry, by advanced polarized neutron scattering from a single domain crystalline sample. The observed diffuse magnetic neutron scattering has an antisymmetric property that relates to its specific chirality, which consists of three cycloidal waves perpendicular to the c axis, forming an entity of cylindrical symmetry. Chirality and symmetry agree with relevant antisymmetric exchanges arising from broken spatial parity. Applying a Fourier analysis to the chiral interference pattern, with distinction between kagome sites and the connecting trigonal interlayer sites of threefold symmetry, the chiral spin correlation function is determined. Characteristic chiral waves originate from the trigonal sites and extend over several periods in the kagome planes. The chiral spin liquid is remarkably stable at low temperatures despite strong antiferromagnetic spin exchange. The observation raises a challenge, since the commonly accepted ground states in condensed matter either have crystalline long-range order or form a quantum liquid. We show that, within the classical theory of magnetic order, a disordered ground state may arise from chirality. The present scenario, with antisymmetric exchange acting as a frustrating gauge background that stabilizes local spin lumps, is similar to the avoided phase transition in coupled gauge and matter fields for subnuclear particles.

2020, Portnichenko, P.Y., Akbari, A., Nikitin, S.E., Cameron, A.S., Dukhnenko, A.V., Filipov, V.B., Shitsevalova, N.Yu., Čermák, P., Radelytskyi, I., Schneidewind, A., Ollivier, J., Podlesnyak, A., Huesges, Z., Xu, J., Ivanov, A., Sidis, Y., Petit, S., Mignot, J.-M., Thalmeier, P., Inosov, D.S.

In contrast to magnetic order formed by electrons' dipolar moments, ordering phenomena associated with higher-order multipoles (quadrupoles, octupoles, etc.) are more difficult to characterize because of the limited choice of experimental probes that can distinguish different multipolar moments. The heavy-fermion compound CeB6 and its La-diluted alloys are among the best-studied realizations of the long-range-ordered multipolar phases, often referred to as "hidden order."Previously, the hidden order in phase II was identified as primary antiferroquadrupolar and field-induced octupolar order. Here, we present a combined experimental and theoretical investigation of collective excitations in phase II of CeB6. Inelastic neutron scattering (INS) in fields up to 16.5 T reveals a new high-energy mode above 14 T in addition to the low-energy magnetic excitations. The experimental dependence of their energy on the magnitude and angle of the applied magnetic field is compared to the results of a multipolar interaction model. The magnetic excitation spectrum in a rotating field is calculated within a localized approach using the pseudospin representation for the Γ8 states. We show that the rotating-field technique at fixed momentum can complement conventional INS measurements of the dispersion at a constant field and holds great promise for identifying the symmetry of multipolar order parameters and the details of intermultipolar interactions that stabilize hidden-order phases. © 2020 authors. Published by the American Physical Society.

2021, Pal, Shovon, Strkalj, Nives, Yang, Chia-Jung, Weber, Mads C., Trassin, Morgan, Woerner, Michael, Fiebig, Manfred

Soft modes are intimately linked to structural instabilities and are key for the understanding of phase transitions. The soft modes in ferroelectrics, for example, map directly the polar order parameter of a crystal lattice. Driving these modes into the nonlinear, frequency-changing regime with intense terahertz (THz) light fields is an efficient way to alter the lattice and, with it, the physical properties. However, recent studies show that the THz electric-field amplitudes triggering a nonlinear soft-mode response are surprisingly low, which raises the question on the microscopic picture behind the origin of this nonlinear response. Here, we use linear and two-dimensional terahertz (2D THz) spectroscopy to unravel the origin of the soft-mode nonlinearities in a strain-engineered epitaxial ferroelectric SrTiO3 thin film. We find that the linear dielectric function of this mode is quantitatively incompatible with pure ionic or pure electronic motions. Instead, 2D THz spectroscopy reveals a pronounced coupling of electronic and ionic-displacement dipoles. Hence, the soft mode is a hybrid mode of lattice (ionic) motions and electronic interband transitions. We confirm this conclusion with model calculations based on a simplified pseudopotential concept of the electronic band structure. It reveals that the entire THz nonlinearity is caused by the off-resonant nonlinear response of the electronic interband transitions of the lattice-electronic hybrid mode. With this work, we provide fundamental insights into the microscopic processes that govern the softness that any material assumes near a ferroic phase transition. This knowledge will allow us to gain an efficient all-optical control over the associated large nonlinear effects.

2019, Neufeld, Ofer, Ayuso, David, Decleva, Piero, Ivanov, Misha Y., Cohen, Oren

We propose and numerically demonstrate a new chiral spectroscopy method that is based on a universal system-independent mechanism of dynamical symmetry breaking in high harmonic generation (HHG). The proposed technique relies only on intense electric-dipole transitions and not on their interplay with magnetic dipole transitions. The symmetry breaking results in the emission of otherwise “forbidden” harmonics from chiral media (i.e., that are not emitted from achiral or racemic media), yielding a huge, nearly background-free, chiral-achiral signal that is correlated to the magnitude of the medium’s enantiomeric excess. The handedness of the medium can be directly detected by measuring the polarization helicity of the emitted harmonics. Moreover, the strength of the “allowed” harmonics (that are not related to symmetry breaking) is chirality independent; hence, they can be used as a reference to probe chiral degrees of freedom within a single measurement. We numerically demonstrate up to 99% chiral-achiral signal level (normalized difference between the chiral and achiral HHG spectra) from microscopic gas-phase emission using state-of-the-art models for HHG in bromochlorofluoromethane and propylene oxide. We expect the new method to give rise to precise tabletop characterization of chiral media in the gas phase and for highly sensitive time-resolved probing of dynamical chiral processes with femtosecond-to-attosecond temporal resolution.

2018, Pavlov, S. G., Deßmann, N., Redlich, B., van der Meer, A. F. G., Abrosimov, N. V., Riemann, H., Zhukavin, R. Kh., Shastin, V. N., Hübers, H.-W.

We report on an optically pumped laser where photons are simultaneously generated by population inversion and by stimulated Raman scattering in the same active medium, namely crystalline silicon doped by bismuth (SiBi). The medium utilizes three electronic levels: ground state [|1