arXiv subjects

J. P. Hill

Publications and source records attributed to J. P. Hill.

At least 19 recordsLinked to original sources

arXiv2021

Laser-Induced Transient Magnons in Sr3Ir2O7 Throughout the Brillouin Zone

Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic x-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets, and that they persist for several picoseconds which is opposite to what is observed in nearly gapless magnets. Our work suggests that materials with isotropic magnetic interactions are preferred to achieve rapid manipulation of magnetism.

cond-mat.str-el↗

arXiv2018

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective

Many remarkable properties of quantum materials emerge from states with intricate coupling between the charge, spin and orbital degrees of freedom. Ultrafast photo-excitations of these materials hold great promise for understanding and controlling the properties of these states. Here we introduce time-resolved resonant inelastic X-ray scattering (trRIXS) as a means of measuring charge, spin and orbital excitations out of equilibrium. These excitations encode the correlations and interactions that determine the detailed properties of the states generated. After outlining the basic principles and instrumentation of tr-RIXS, we review our first observations of transient antiferromagnetic correlations in quasi-two dimensions in a photo-excited Mott insulator and present possible future routes of this fast-developing technique. The increasing number of X-ray free electron laser facilities not only enables tackling long-standing fundamental scientific problems, but also promises to unleash novel inelastic X-ray scattering spectroscopies

cond-mat.str-el↗

arXiv2017

Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism.

cond-mat.str-el↗

arXiv2016

Doping dependence of the magnetic excitations in La$_{2-x}$Sr$_x$CuO$_4$

The magnetic correlations within the cuprates have undergone intense scrutiny as part of efforts to understand high temperature superconductivity. We explore the evolution of the magnetic correlations along the nodal direction of the Brillouin zone in La2-xSrxCuO4, spanning the doping phase diagram from the anti-ferromagnetic Mott insulator at x = 0 to the metallic phase at x = 0.26. Magnetic excitations along this direction are found to be systematically softened and broadened with doping, at a higher rate than the excitations along the anti-nodal direction. This phenomenology is discussed in terms of the nature of the magnetism in the doped cuprates. Survival of the high energy magnetic excitations, even in the overdoped regime, indicates that these excitations are marginal to pairing, while the influence of the low energy excitations remains ambiguous.

cond-mat.str-el↗

arXiv2016

Restoring Interlayer Josephson Coupling in La_{1.885}Ba_{0.115}CuO_4 by Charge Transfer Melting of Stripe Order

We show that disruption of charge-density-wave (stripe) order by charge transfer excitation, enhances the superconducting phase rigidity in La_{1.885}Ba_{0.115}CuO_4 (LBCO). Time-Resolved Resonant Soft X-Ray Diffraction demonstrates that charge order melting is prompt following near-infrared photoexcitation whereas the crystal structure remains intact for moderate fluences. THz time-domain spectroscopy reveals that, for the first 2 ps following photoexcitation, a new Josephson Plasma Resonance edge, at higher frequency with respect to the equilibrium edge, is induced indicating enhanced superconducting interlayer coupling. The fluence dependence of the charge-order melting and the enhanced superconducting interlayer coupling are correlated with a saturation limit of about 0.5 mJ/cm2. Using a combination of x-ray and optical spectroscopies we establish a hierarchy of timescales between enhanced superconductivity, melting of charge order and rearrangement of the crystal structure.

cond-mat.supr-con↗

arXiv2016

Ultrafast energy and momentum resolved dynamics of magnetic correlations in photo-doped Mott insulator Sr$_2$IrO$_4$

Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high $T_C$ superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant inelastic X-ray scattering at a free electron laser, and directly determine the magnetization dynamics after photo-doping the Mott insulator Sr$_2$IrO$_4$. We find that the non-equilibrium state 2~ps after the excitation has strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. The magnetism recovers its two-dimensional (2D) in-plane Néel correlations on a timescale of a few ps, while the three-dimensional (3D) long-range magnetic order restores over a far longer, fluence-dependent timescale of a few hundred ps. The dramatic difference in these two timescales, implies that characterizing the dimensionality of magnetic correlations will be vital in our efforts to understand ultrafast magnetic dynamics.

cond-mat.str-el↗

arXiv2015

Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7

The rich physics manifested by 5d oxides falls outside the Mott-Hubbard paradigm used to successfully explain the electronic and magnetic properties of 3d oxides. Much consideration has been given to the extent to which strong spin-orbit coupling (SOC), in the limit of increased bandwidth and reduced electron correlation, drives the formation of novel electronic states, as manifested through the existence of metal-insulator transitions (MITs). SOC is believed to play a dominant role in 5d5 systems such as iridates (Ir4+), undergoing MITs which may or may not be intimately connected to magnetic order, with pyrochlore and perovksite systems being examples of the former and latter, respectively. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (e.g Os5+) systems are expected to have an orbital singlet and consequently a reduced effect of SOC in the groundstate. The pyrochlore osmate Cd2Os2O7 nonetheless exhibits a MIT intimately entwined with magnetic order with phenomena similar to pyrochlore iridates. Here we report the first resonant inelastic X-ray scattering (RIXS) measurements on an osmium compound, allowing us to determine the salient electronic and magnetic energy scales controlling the MIT in Cd2Os2O7, which we benchmark against detailed quantum chemistry calculations. In particular, we reveal the emergence at the MIT of a magnetic excitation corresponding to a superposition of multiple spin-flip processes from an Ising-like all-in/all-out magnetic groundstate. We discuss our results with respect to the role of SOC in magnetically mediated MITs in 5d systems

cond-mat.str-el↗

arXiv2015

Wavelength dependent optical enhancement of superconducting interlayer coupling in La1.885Ba0.115CuO4

We analyze the pump wavelength dependence for the photo-induced enhancement of interlayer coupling in La1.885Ba0.115CuO4, which is promoted by optical melting of the stripe order. In the equilibrium superconducting state (T < Tc = 13 K), in which stripes and superconductivity coexist, time-domain THz spectroscopy reveals a photo-induced blue-shift of the Josephson Plasma Resonance after excitation with optical pulses polarized perpendicular to the CuO2 planes. In the striped, non-superconducting state (Tc < T < T_SO = 40 K) a transient plasma resonance similar to that seen below Tc appears from a featureless equilibrium reflectivity. Most strikingly, both these effects become stronger upon tuning of the pump wavelength from the mid-infrared to the visible, underscoring an unconventional competition between stripe order and superconductivity, which occurs on energy scales far above the ordering temperature.

cond-mat.supr-con↗

arXiv2015

Spatially resolved ultrafast magnetic dynamics launched at a complex-oxide hetero-interface

Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across hetero-interfaces dynamically. Here, by exciting large amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a hetero-interface. Femtosecond Resonant Soft X-ray Diffraction is used to determine the spatial and temporal evolution of the magnetic disordering. We observe a magnetic melt front that grows from the substrate interface into the film, at a speed that suggests electronically driven propagation. Light control and ultrafast phase front propagation at hetero-interfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

cond-mat.str-el↗

arXiv2015

Femtosecond x rays link melting of charge-density wave correlations and light-enhanced coherent transport in YBa2Cu3O6.6

We use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge density wave correlations in underdoped YBa2Cu3O6.6. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

cond-mat.supr-con↗

arXiv2015

Melting of Charge Stripes in Vibrationally Driven La1.875Ba0.125CuO4: Assessing the Respective Roles of Electronic and Lattice Order in Frustrated Superconductors

We report femtosecond resonant soft X-ray diffraction measurements of the dynamics of the charge order and of the crystal lattice in non-superconducting, stripe-ordered La1.875Ba0.125CuO4. Excitation of the in-plane Cu-O stretching phonon with a mid-infrared pulse has been previously shown to induce a transient superconducting state in the closely related compound La1.675Eu0.2Sr0.125CuO4. In La1.875Ba0.125CuO4, we find that the charge stripe order melts promptly on a sub-picosecond time scale. Surprisingly, the low temperature tetragonal distortion is only weakly reduced, reacting on significantly longer time scales that do not correlate with light-induced superconductivity. This experiment suggests that charge modulations alone, and not the LTT distortion, prevent superconductivity in equilibrium.

cond-mat.supr-con↗

arXiv2015

Probing single magnon excitations in Sr$_2$IrO$_4$ using O $K$-edge resonant inelastic X-ray scattering

Resonant inelastic X-ray scattering (RIXS) at the $L$-edge of transition metal elements is now commonly used to probe single magnon excitations. Here we show that single magnon excitations can also be measured with RIXS at the $K$-edge of the surrounding ligand atoms when the center heavy metal elements have strong spin-orbit coupling. This is demonstrated with oxygen $K$-edge RIXS experiments on the perovskite Sr$_2$IrO$_4$, where low energy peaks from single magnon excitations were observed. This new application of RIXS has excellent potential to be applied to a wide range of magnetic systems based on heavy elements, for which the $L$-edge RIXS energy resolutions in the hard X-ray region is usually poor.

cond-mat.mtrl-sci↗

arXiv2014

Itinerant effects and enhanced magnetic interactions in Bi-based multilayer cuprates

The cuprate high temperature superconductors exhibit a pronounced trend in which the superconducting transition temperature, $T_{\rm c}$, increases with the number of CuO$_2$ planes, $n$, in the crystal structure. We compare the magnetic excitation spectrum of Bi$_{2+x}$Sr$_{2-x}$CuO$_{6+δ}$ (Bi-2201) and Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10 + δ}$ (Bi-2223), with $n=1$ and $n=3$ respectively, using Cu $L_3$-edge resonant inelastic x-ray scattering (RIXS). Near the anti-nodal zone boundary we find the paramagnon energy in Bi-2223 is substantially higher than that in Bi-2201, indicating that multilayer cuprates host stronger effective magnetic exchange interactions, providing a possible explanation for the $T_{\rm c}$ vs.\ $n$ scaling. In contrast, the nodal direction exhibits very strongly damped, almost non-dispersive excitations. We argue that this implies that the magnetism in the doped cuprates is partially itinerant in nature.

cond-mat.supr-con↗

arXiv2014

Optically induced superconductivity in striped La2-xBaxCuO4 by polarization-selective excitation in the near infrared

We show that superconducting interlayer coupling, which coexists with and is depressed by stripe order in La1.885Ba0.115CuO4, can be enhanced by excitation with near-infrared laser pulses. For temperatures lower than Tc = 13 K, we observe a blue-shift of the equilibrium Josephson plasma resonance, detected by terahertz-frequency reflectivity measurements. Key to this measurement is the ability to probe the optical properties at frequencies as low as 150 GHz, detecting the weak interlayer coupling strengths. For T > Tc a similar plasma resonance, absent at equilibrium, is induced up to the spin-ordering temperature TSO = 40 K. These effects are reminiscent but qualitatively different from the light-induced superconductivity observed by resonant phonon excitation in La1.675Eu0.2Sr0.125CuO6.5. Importantly, enhancement of the below-Tc interlayer coupling and its appearance above Tc are preferentially achieved when the near-infrared pump light is polarized perpendicular to the superconducting planes, likely due to more effective melting of stripe order and the less effective excitation of quasiparticles from the Cooper pair condensate when compared to in-plane excitation.

cond-mat.supr-con↗

arXiv2014

Femtosecond Time-resolved MeV Electron Diffraction

We report the experimental demonstration of femtosecond electron diffraction using high-brightness MeV electron beams. High-quality, single-shot electron diffraction patterns for both polycrystalline aluminum and single-crystal 1T-TaS2 are obtained utilizing a 5 femto-Coulomb (~3x10^4 electrons) pulse of electrons at 2.8 MeV. The high quality of the electron diffraction patterns confirm that electron beam has a normalized emittance of ~50 nm-rad. The corresponding transverse and longitudinal coherence length are ~11 nm and ~2.5 nm, respectively. The timing jitter between the pump laser and probe electron beam was found to be ~ 100 fs (rms). The temporal resolution is demonstrated by observing the evolution of Bragg and superlattice peaks of 1T-TaS2 following an 800 nm optical pump and was found to be 130 fs. Our results demonstrate the advantages of MeV electron diffraction: such as longer coherent lengths, large scattering cross-section and larger signal-to-noise ratio, and the feasibility of ultimately realizing 10 fs time-resolved electron diffraction.

physics.ins-det↗

arXiv2013

Structural phase transition induced by van Hove singularity in 5d transition metal compound IrTe2

Comprehensive studies of the electronic states of Ir 5d and Te 5p have been performed to elucidate the origin of the structural phase transition in IrTe2 by combining angle-resolved photoemission spectroscopy and resonant inelastic X-ray scattering. While no considerable changes are observed in the configuration of the Ir 5d electronic states across the transition, indicating that the Ir 5d orbitals are not involved in the transition, we reveal a van Hove singularity at the Fermi level (EF) related to the Te px+py orbitals, which is removed from EF at low temperatures. The wavevector connecting the adjacent saddle points is consistent with the in-plane projection of the superstructure modulation wavevector. These results can be qualitatively understood with the Rice-Scott "saddle-point" mechanism, while effects of the lattice distortions need to be additionally involved.

cond-mat.supr-con↗

arXiv2013

Persistence of magnetic excitations in La2-xSrxCuO4 from the undoped insulator to the heavily overdoped non-superconducting metal

One of the most intensely studied scenarios of high-temperature superconductivity (HTS) postulates pairing by exchange of magnetic excitations [1]. Indeed, such excitations have been observed up to around optimal doping in the cuprates [2-7]. In the heavily overdoped regime neutron scattering measurements indicate that magnetic excitations have effectively disappeared [8-10], and this was argued to cause the demise of HTS with overdoping [1, 8, 10]. Here we use resonant inelastic x-ray scattering (RIXS), which is sensitive to complementary parts of reciprocal space, to measure the evolution of the magnetic excitations in La2-xSrxCuO4 across the entire phase diagram, from a strongly correlated insulator (x = 0) to a non-superconducting metal (x = 0.40). For x = 0, well-defined magnon excitations are observed [11]. These magnons broaden with doping, but they persist with a similar dispersion and comparable intensity all the way to the non-superconducting, heavily overdoped metallic phase. The destruction of HTS with overdoping is therefore caused neither by the general disappearance nor by the overall softening of magnetic excitations; other factor(s), such as the redistribution of spectral weight, must be considered.

cond-mat.supr-con↗

arXiv2013

Momentum dependence in K-edge resonant inelastic x-ray scattering and its application to screening dynamics in CE-phase La$_{0.5}$Sr$_{1.5}$MnO$_4$

We present a formula for the calculation of K-edge resonant inelastic x-ray scattering on transition metal compounds, based on a local interaction between the valence shell electrons and the $1s$ core hole. Extending a previous result, we include explicit momentum dependence and a basis with multiple core-hole sites. We apply this formula to a single-layered charge, orbital and spin ordered manganite, La$_{0.5}$Sr$_{1.5}$MnO$_4$, and obtain good agreement with experimental data, in particular with regards to the large variation of the intensity with momentum. We find that the screening in La$_{0.5}$Sr$_{1.5}$MnO$_4$ is highly localized around the core-hole site and demonstrate the potential of K-edge resonant inelastic x-ray scattering as a probe of screening dynamics in materials.

cond-mat.mtrl-sci↗