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A. V. Boris

Publications and source records attributed to A. V. Boris.

At least 19 recordsLinked to original sources

A crystal-field route to THz-driven magnetization

Light carries angular momentum, but the microscopic pathways that transform it into magnetization remain elusive. Here we establish that crystal-field excitations, historically viewed primarily as equilibrium spectroscopic fingerprints of localized 4$f$ electrons, constitute an active microscopic route through which circularly-polarized terahertz (THz) light creates magnetic polarization. Using wavelength-selective ultrafast Faraday spectroscopy on the paramagnetic insulator CeF$_3$, we show that resonant excitation of localized 4$f$ crystal-field transitions generates a helicity-dependent magnetization that survives for up to about 100 ps. Most strikingly, while the optical helicity is held fixed, the THz-driven response reverses sign as the excitation wavelength is tuned across the crystal-field resonance. The resulting dispersive spectral response follows the crystal-field excitation spectrum rather than that of optical phonons, and is captured by resonant electronic theory of the inverse Faraday effect. Our results identify crystal-field excitations as a previously unrecognized dynamical reservoir for optical angular momentum and broaden the microscopic pathways through which THz light can create and manipulate magnetic states.

cond-mat.mtrl-sci

Evolution of spin excitations in superconducting La$_{2-x}$Ca$_{x}$CuO$_{4-δ}$ from the underdoped to the heavily overdoped regime

We investigate high-energy spin excitations in hole-doped La$_{2-x}$Ca$_{x}$CuO$_{4-δ}$ films across a broad Ca doping range $x = 0.05-0.50$ using resonant inelastic x-ray scattering (RIXS). Polarization analysis and incident-photon energy detuning measurements confirm the persistence of collective paramagnon excitations up to $x = 0.50$. Consistent with previous studies on other cuprate families, we observe a pronounced crossover near $x = 0.15$, where paramagnon spectral weight is transferred to incoherent spin-flip excitations associated with the particle-hole continuum. The overall behavior of paramagnons in LCCO resembles that in other hole-doped cuprates and appears insensitive to the persistence of superconductivity at high doping levels in LCCO - up to at least $x = 0.50$, as demonstrated in prior work. These findings support the view that high-energy magnetic excitations probed by RIXS are not a major contributor to superconducting pairing, in line with theories of spin-fluctuation mediated superconductivity.

cond-mat.supr-con

Imprinted atomic displacements drive spin-orbital order in a vanadate perovskite

Perovskites with the generic composition ABO$_3$ exhibit an enormous variety of quantum states such as magnetism, orbital order, ferroelectricity and superconductivity. Their flexible and comparatively simple structure allows for facile chemical substitution and cube-on-cube combination of different compounds in atomically sharp epitaxial heterostructures. However, already in the bulk, the diverse physical properties of perovskites and their anisotropy are determined by small deviations from the ideal perovskite structure, which are difficult to control. Here we show that directional imprinting of atomic displacements in the antiferromagnetic Mott insulator YVO$_3$ is achieved by depositing epitaxial films on different facets of an isostructural substrate. These facets were chosen such that other control parameters, including strain and polarity mismatch with the overlayer, remain unchanged. We use polarized Raman scattering and spectral ellipsometry to detect signatures of staggered orbital and magnetic order, and demonstrate distinct spin-orbital ordering patterns on different facets. These observations can be attributed to the influence of specific octahedral rotation and cation displacement patterns, which are imprinted by the substrate facet, on the covalency of the bonds and the superexchange interactions in YVO$_3$. Well beyond established strain-engineering strategies, our results show that substrate-induced templating of lattice distortion patterns constitutes a powerful pathway for materials design.

cond-mat.mtrl-sci

Interplay between electronic and lattice superstructures in La$_{2-x}$Ca$_{x}$CuO$_{4}$

Complex oxides are well known to develop oxygen ordering patterns with well defined periodicities, but their interplay with electronic correlations remains largely unexplored. Here, we report resonant and non-resonant x-ray diffraction data indicating a four-unit-cell periodic superstructure related to oxygen vacancy ordering in La$_{2-x}$Ca$_{x}$CuO$_{4}$ films with doping levels from the underdoped ($x = 0.15$) to the extremely overdoped ($x = 0.50$) regime. Whereas the lattice superstructure is temperature independent up to 300 K, a strongly temperature dependent electronic charge density wave (CDW) is observed in the underdoped and slightly overdoped regimes ($x\leq0.20$). The periodicity, in-plane and out-of-plane correlation lengths of the CDW are locked in by the lattice superstructure. Our results highlight the necessity to consider lattice and electronic energetics on equal footing in the high-temperature oxygen-disordered phase to explain oxygen ordering phenomena in complex oxides.

cond-mat.str-el

Photoinduced phase switching at a Mott insulator-to-metal transition

Achieving fundamental understanding of insulator-to-metal transitions (IMTs) in strongly correlated systems and their persistent and reversible control via nonequilibrium drive are prime targets of current condensed matter research. Photoinduced switching between competing orders in correlated insulators requires a free-energy landscape with nearly degenerate ground states, which is commonly reached through doping, strain, or static electric field. The associated spatial inhomogeneity leads to a photoinduced phase transition that remains confined near the illuminated region. Here we report optical spectroscopy experiments at the first-order IMT in the 4d-electron compound Ca$_3$(Ru$_{0.99}$Ti$_{0.01}$)$_2$O$_7$ and show that specific Ru d-d interband transitions excited by light with a threshold fluence corresponding to the planar density of Ru atoms can trigger reversible, avalanche-like coherent propagation of phase interfaces across the full extent of a macroscopic sample, in the absence of assisting external stimuli. Based on detailed comparison of spectroscopic data to density functional calculations, we attribute the extraordinary photo-sensitivity of the IMT to an exceptionally shallow free-energy landscape generated by the confluence of electron-electron and electron-lattice interactions. Our findings suggest Ca$_3$(Ru$_{0.99}$Ti$_{0.01}$)$_2$O$_7$ as an ideal model system for building and testing a theory of Mott transition dynamics in the presence of strong electron-lattice coupling and may pave the way towards nanoscale devices with quantum-level photosensitivity.

cond-mat.str-el

Competing spin-orbital singlet states in the 4$d^4$ honeycomb ruthenate Ag$_3$LiRu$_2$O$_6$

When spin-orbit-entangled $d$-electrons reside on a honeycomb lattice, rich quantum states are anticipated to emerge, as exemplified by the $d^5$ Kitaev materials. Distinct yet equally intriguing physics may be realized with a $d$-electron count other than $d^5$. We found that the layered ruthenate Ag$_3$LiRu$_2$O$_6$ with $d^4$ Ru$^{4+}$ ions at ambient pressure forms a honeycomb lattice of spin-orbit-entangled singlets, which is a playground for frustrated excitonic magnetism. Under pressure, the singlet state does not develop the expected excitonic magnetism but experiences two successive transitions to other nonmagnetic phases, first to an intermediate phase with moderate distortion of honeycomb lattice, and eventually to a high-pressure phase with very short Ru-Ru dimer bonds. While the strong dimerization in the high-pressure phase originates from a molecular orbital formation as in the sister compound Li$_2$RuO$_3$, the intermediate phase represents a spin-orbit-coupled $J$-dimer state which is stabilized by the admixture of upper-lying $J_{\rm eff} = 1$-derived states. We argue that the $J$-dimer state is induced by a pseudo-Jahn-Teller effect associated with the low-lying spin-orbital excited states and is unique to spin-orbit-entangled $d^4$ systems. The discovery of competing singlet phases demonstrates rich spin-orbital physics of $d^4$ honeycomb compounds and paves the way for realization of unconventional magnetism.

cond-mat.str-el

Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO$_3$

In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic, and chemical constraints. Here, we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO$_3$, a material that exhibits only partial orbital polarization, an unsaturated low-temperature magnetic moment, and a suppressed Curie temperature, $T_c$ = 27 K. The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to $T_{neq} >$ 80 K, nearly three times the thermodynamic transition temperature. First-principles and model calculations of the nonlinear phonon-orbital-spin coupling reveal that these effects originate from dynamical changes to the orbital polarization and the makeup of the lowest quasi-degenerate Ti $t_{2g}$ levels. Notably, light-induced high temperature ferromagnetism in YTiO$_3$ is found to be metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.

cond-mat.str-el

Evolution of the metallic state of LaNiO$_3$/LaAlO$_3$ superlattices measured by $^8$Li $β$-detected NMR

Using ion-implanted $^8$Li $β$-detected NMR, we study the evolution of the correlated metallic state of LaNiO$_3$ in a series of LaNiO$_3$/LaAlO$_3$ superlattices as a function of bilayer thickness. Spin-lattice relaxation measurements in an applied field of 6.55 T reveal two equal amplitude components: one with metallic ($T$-linear) $1/T_{1}$, and a second with a more complex $T$-dependence. The metallic character of the slow relaxing component is only weakly affected by the LaNiO$_3$ thickness, while the fast component is much more sensitive, exhibiting the opposite temperature dependence (increasing towards low $T$) in the thinnest, most magnetic samples. The origin of this bipartite relaxation is discussed.

cond-mat.str-el

Approaching two-dimensional superconductivity in ultrathin DyBa$_2$Cu$_3$O$_{7-δ}$

The temperature dependence of the superfluid density $ρ_s(T)$ has been measured for a series of ultrathin MBE-grown DyBa$_2$Cu$_3$O$_{7-δ}$ superconducting (SC) films by sub-mm wave interferometry combined with time-domain THz spectroscopy and IR ellipsometry. We find that all films 10 u.c. and thicker show the same universal temperature dependence of $ρ_s(T)$, which follows the critical behavior characteristic of single crystal YBa$_2$Cu$_3$O$_{7-δ}$ as $T$ approaches $T_c$. In 7 u.c. thick films, $ρ_s(T)$ declines steeply upon approaching $T_c$, as expected for the Berezinskii-Kosterlitz-Thouless vortex unbinding transition. Our analysis provides evidence for a sharply defined 4 u.c. non-SC interfacial layer, leaving a quasi-2D SC layer on top. We propose that the SC state in this interfacial layer is suppressed by competing (possibly charge) order.

cond-mat.supr-con

Ultrafast phononic switching of magnetization

Identifying an efficient pathway to change the order parameter via a subtle excitation of the coupled high-frequency mode is the ultimate goal of the field of ultrafast phase transitions. This is an especially interesting research direction in magnetism, where the coupling between spin and lattice excitations is required for magnetization reversal. Despite several attempts however, the switching between magnetic states via resonant pumping of phonon modes has not yet been demonstrated. Here we show how an ultrafast resonant excitation of the longitudinal optical phonon modes in magnetic garnet films switches magnetization into a peculiar quadrupolar magnetic domain pattern, unambiguously revealing the magneto-elastic mechanism of the switching. In contrast, the excitation of strongly absorbing transverse phonon modes results in thermal demagnetization effect only.

cond-mat.mtrl-sci

Microwave response of interacting oxide two-dimensional electron systems

We present an experimental study on microwave illuminated high mobility MgZnO/ZnO based two-dimensional electron systems with different electron densities and, hence, varying Coulomb interaction strength. The photoresponse of the low-temperature dc resistance in perpendicular magnetic field is examined in low and high density samples over a broad range of illumination frequencies. In low density samples a response due to cyclotron resonance (CR) absorption dominates, while high density samples exhibit pronounced microwave-induced resistance oscillations (MIRO). Microwave transmission experiments serve as a complementary means of detecting the CR over the entire range of electron densities and as a reference for the band mass unrenormalized by interactions. Both CR and MIRO-associated features in the resistance permit extraction of the effective mass of electrons but yield two distinct values. The conventional cyclotron mass representing center-of-mass dynamics exhibits no change with density and coincides with the band electron mass of bulk ZnO, while MIRO mass reveals a systematic increase with lowering electron density consistent with renormalization expected in interacting Fermi liquids.

cond-mat.mes-hall

Ferromagnetism and conductivity in atomically thin SrRuO3

Atomically thin ferromagnetic and conducting electron systems are highly desired for spintronics, because they can be controlled with both magnetic and electric fields. We present (SrRuO3)1-(SrTiO3)5 superlattices and single-unit-cell-thick SrRuO3 samples that are capped with SrTiO3. We achieve samples of exceptional quality. In these samples, the electron systems comprise only a single RuO2 plane. We observe conductivity down to 50 mK, a ferromagnetic state with a Curie temperature of 25 K, and signals of magnetism persisting up to approximately 100 K.

cond-mat.mtrl-sci

Optical Characteristics of Charge Carrier Transfer across Interfaces between YBa$_2$Cu$_3$O$_{6+δ}$ and La$_{0.7}$Ca$_{0.3}$MnO$_3$

We report a spectral ellipsometry study of multilayers composed of superconducting YBa$_2$Cu$_3$O$_{6+δ}$ (YBCO) and ferromagnetic La$_{0.7}$Ca$_{0.3}$MnO$_3$ in the spectral range of 0.7 - 6.5 eV. With increasing YBCO sublayer thickness, the optical spectral weight is enhanced at photon energies of 1.5 - 3.5 eV. The spectral weight enhancement is proportional to the number of interfaces of each multilayer sample, indicating its association with the interfacial electronic structure. Based on calculations in the framework of a multilayer model, we find that the shape of the interface-induced spectral weight is consistent with transfer of hole-carriers from YBCO to LCMO. Our results imply that the holes that are transferred across the interfaces accumulate in the LCMO layers, rather than being pinned by interfacial defects or annihilated by electron donors such as oxygen vacancies. Optical spectroscopy can thus serve as a non-destructive probe of charge transfer across buried interfaces in metal-oxide heterostructures.

cond-mat.str-el

Infrared phonon spectra of quasi-one-dimensional Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$

Using a combination of infrared ellipsometry, time-domain terahertz spectroscopy, and far-infrared reflectometry we have obtained the $ac$-plane complex dielectric function of monoclinic ($C2/c$) Ta$_2$NiSe$_5$ and orthorhombic ($Cmcm$) Ta$_2$NiS$_5$ single crystals. The identified dipole-active phonon modes polarized along $a$ and $c$ axes are in good agreement with density functional theory calculations. With increasing temperature the $a$-axis phonon modes of Ta$_2$NiSe$_5$ become poorly discernible, as they are superimposed on the electronic background which gradually fills the energy gap near the monoclinic-to-orthorhombic phase transition temperature $T_c$ = 326 K. In Ta$_2$NiS$_5$, which does not exhibit such a structural transition and remains orthorhombic down to low temperatures, the $a$-axis phonon modes are superimposed on a persistent broad electronic mode centered near 16 meV. We attribute this difference to strongly overlapping exciton-phonon complexes in Ta$_2$NiSe$_5$, as opposed to isolated instances of the same in Ta$_2$NiS$_5$, and find this to be in good agreement with an excitonic insulator state below $T_c$ in the former, as compared to the absence of one in the latter.

cond-mat.str-el

Intrinsic charge dynamics in high-Tc AFeAs(O,F) superconductors

We report the first determination of the in-plane complex optical conductivity of 1111 high-Tc superconducting iron oxypnictide single crystals PrFeAsO0.6F0.35 and thin films SmFeAsO1-xFx by means of bulk-sensitive conventional and micro-focused infrared spectroscopy, ellipsometry, and time-domain THz transmission spectroscopy. A strong itinerant contribution is found to exhibit a dramatic difference in coherence between the crystal and the film. Using extensive temperature-dependent measurements of THz transmission we identify a previously undetected 2.5-meV collective mode in the optical conductivity of SmFeAs(O,F), which is strongly suppressed at Tc and experiences an anomalous T-linear softening and narrowing below T*=110K>>Tc. The suppression of the infrared absorption in the superconducting state reveals a large optical superconducting gap with a similar gap ratio 2D=kBTc=7 in both materials, indicating strong pairing.

cond-mat.supr-con

Superconductivity drives magnetism in delta-doped La2CuO4

The understanding of the interplay between different orders in a solid is a key challenge in highly correlated electronic systems. In real systems this is even more difficult since disorder can have a strong influence on the subtle balance between these orders and thus can obscure the interpretation of the observed physical properties. Here we present a study on delta-doped La2CuO4 superlattices. By means of molecular beam epitaxy whole LaO-layers were periodically replaced through SrO-layers providing a charge reservoir, yet reducing the level of disorder typically present in doped cuprates to an absolute minimum. The induced superconductivity and its interplay with the antiferromagnetic order is studied by means of low-energy muSR. We find a quasi-2D superconducting state which couples to the antiferromagnetic order in a non-trivial way. Below the superconducting transition temperature, the magnetic volume fraction increases strongly. The reason could be a charge redistribution of the free carriers due to the opening of the superconducting gap which is possible due to the close proximity and low disorder between the different ordered regions.

cond-mat.str-el

Giant exciton Fano resonance in quasi-one-dimensional Ta$_2$NiSe$_5$

We report the complex dielectric function of the quasi-one-dimensional chalcogenide Ta$_2$NiSe$_5$, which exhibits a structural phase transition that has been attributed to exciton condensation below $T_c = 326$ K, and of the isostructural Ta$_2$NiS$_5$ which does not exhibit such a transition. Using spectroscopic ellipsometry, we have detected exciton doublets with pronounced Fano lineshapes in both the compounds. The exciton Fano resonances in Ta$_2$NiSe$_5$ display an order of magnitude higher intensity than those in Ta$_2$NiS$_5$. In conjunction with prior theoretical work by E. Rashba, we attribute this observation to the giant oscillator strength of spatially extended exciton-phonon bound states in Ta$_2$NiSe$_5$. The formation of exciton-phonon complexes in Ta$_2$NiS$_5$ and Ta$_2$NiSe$_5$ is confirmed by the pronounced temperature dependence of sharp interband transitions in the optical spectra, whose peak energies and widths scale with the thermal population of optical phonon modes. The description of the optically excited states in terms of strongly overlapping exciton complexes is in good agreement with the hypothesis of an EI ground state.

cond-mat.str-el

Optical melting of the transverse Josephson plasmon: a comparison between bilayer and trilayer cuprates

We report on an investigation of the redistribution of interlayer coherence in the trilayer cuprate Bi2Sr2Ca2Cu3O10. The experiment is performed under the same apical-oxygen phonon excitation discussed in the past for the bilayer cuprate YBa2Cu3O6.5. In Bi2Sr2Ca2Cu3O10, we observe a similar spectral weight loss at the transverse plasma mode resonance seen in YBa2Cu3O6.5. However, this feature is not accompanied by light-enhanced interlayer coherence that was seen in YBa2Cu3O6+x, for which the transverse plasma mode is observed at equilibrium even in the normal state. These new observations offer new experimental perspective in the context of the physics of light-enhanced interlayer coupling in various cuprates.

cond-mat.supr-con