arXiv subjects

K. Ueda

Publications and source records attributed to K. Ueda.

At least 37 records · Page 2Linked to original sources

arXiv2019

Observation of spin-orbit excitations and Hund's multiplets in Ca$_2$RuO$_4$

We use Ru $L_3$-edge (2838.5 eV) resonant inelastic x-ray scattering (RIXS) to quantify the electronic structure of Ca$_2$RuO$_4$, a layered $4d$-electron compound that exhibits a correlation-driven metal-insulator transition and unconventional antiferromagnetism. We observe a series of Ru intra-ionic transitions whose energies and intensities are well described by model calculations. In particular, we find a $\rm{J}=0\rightarrow 2$ spin-orbit excitation at 320 meV, as well as Hund's-rule driven $\rm{S}=1\rightarrow 0$ spin-state transitions at 750 and 1000 meV. The energy of these three features uniquely determines the spin-orbit coupling, tetragonal crystal-field energy, and Hund's rule interaction. The parameters inferred from the RIXS spectra are in excellent agreement with the picture of excitonic magnetism that has been devised to explain the collective modes of the antiferromagnetic state. $L_3$-edge RIXS of Ru compounds and other $4d$-electron materials thus enables direct measurements of interactions parameters that are essential for realistic model calculations.

cond-mat.str-el↗

arXiv2019

Pressure induced evolution of band structure in black phosphorus studied by $^{31}$P-NMR

Two-dimensional layered semiconductor black phosphorus (BP), a promising pressure induced Dirac system as predicted by band structure calculations, has been studied by $^{31}$P-nuclear magnetic resonance. Band calculations have been also carried out to estimate the density of states $D(E)$. The temperature and pressure dependences of nuclear spin lattice relaxation rate $1/T_1$ in the semiconducting phase are well reproduced using the derived $D(E)$, and the resultant pressure dependence of semiconducting gap is in good accordance with previous reports, giving a good confirmation that the band calculation on BP is fairly reliable. The present analysis of $1/T_1$ data with the complemental theoretical calculations allows us to extract essential information, such as the pressure dependences of $D(E)$ and chemical potential, as well as to decompose observed $1/T_1$ into intrinsic and extrinsic contributions. An abrupt increase in $1/T_1$ at 1.63GPa indicates that the semiconducting gap closes, resulting in an enhancement of conductivity.

cond-mat.mtrl-sci↗

arXiv2019

Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Ruthenium compounds play prominent roles in materials research ranging from oxide electronics to catalysis, and serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin-liquids, and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including the Hund's-rule, spin-orbit, and exchange interactions) are comparable in magnitude, and their interplay is poorly understood - partly due to difficulties in synthesizing sizable single crystals for spectroscopic experiments. Here we introduce a resonant inelastic x-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of $4d$-electron materials. We present a comprehensive set of data on spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu$_{2}$O$_{6}$, which possesses an unusually high Néel temperature. The new RIXS method provides fresh insight into the unconventional magnetism of SrRu$_{2}$O$_{6}$, and enables momentum-resolved spectroscopy of a large class of $4d$ transition-metal compounds.

cond-mat.str-el↗

arXiv2019

Time-resolved observation of interatomic Coulombic decay induced by two-photon double excitation of Ne$_{2}$

The hitherto unexplored two-photon doubly-excited states [Ne$^{*}$($2p^{-1}3s$)]$_{2}$ were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD) which predominantly produces singly-ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne$_{2}^{+}$ ions was recorded as a function of delay between the XUV pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly-excited states, 390 (-130 / +450} fs, and of the short-lived ones, less than 150~fs, are in good agreement with \emph{ab initio} quantum mechanical calculations.

physics.atom-ph↗

arXiv2019

Evidence for gradual evolution of low-energy fluctuations underlying the first-order structural and valence order in YbPd

The valence orders at $T_a=125$ K and $T_b=105$ K in the cubic compound YbPd have been investigated by $^{105}$Pd-nuclear magnetic resonance (NMR) measurements. Significant decrease in the density of states at the Fermi energy below $T_a$ is evident from the measurement of nuclear spin lattice relaxation rate $1/T_1$, suggesting that the instabilities of Fermi surface are associated with the transitions. Moreover we observed the unusual evolution of low-energy fluctuations toward the valence transition at $T_a$ behind its drastic first-order nature. The structural transition accompanying the valence order may occur as a result of cooperative effect of Fermi surface and valence instabilities.

cond-mat.str-el↗

arXiv2019

Autoionization dynamics of He nanodroplets resonantly excited by intense XUV laser pulses

The ionization dynamics of helium droplets in a wide size range from 220 to 10^6 He atoms irradiated with intense femtosecond extreme ultraviolet (XUV) pulses of 10^9 ÷ 10^{12} W/cm2 power density is investigated in detail by photoelectron spectroscopy. Helium droplets are resonantly excited in the photon energy range from ~ 21 eV (corresponding to the atomic 1s2s state) up to the atomic ionization potential (IP) at ~ 25 eV. A complex evolution of the electron spectra as a function of droplet size and XUV intensity is observed, ranging from atomic-like narrow peaks due to binary autoionization, to an unstructured feature characteristic of electron emission from a nanoplasma. The experimental results are analyzed and interpreted with the help of numerical simulations based on rate equations taking into account various processes such as multi-step ionization, interatomic Coulombic decay (ICD), secondary inelastic collisions, desorption of electronically excited atoms, collective autoionization (CAI) and further relaxation processes.

physics.atm-clus↗

arXiv2017

Observation and Control of Laser-Enabled Auger Decay

Single photon laser enabled Auger decay (spLEAD) has been redicted theoretically [Phys. Rev. Lett. 111, 083004 (2013)] and here we report its first experimental observation in neon. Using coherent, bichromatic free-electron laser pulses, we have detected the process and coherently controlled the angular distribution of the emitted electrons by varying the phase difference between the two laser fields. Since spLEAD is highly sensitive to electron correlation, this is a promising method for probing both correlation and ultrafast hole migration in more complex systems.

physics.atom-ph↗

arXiv2017

Coherent control with a short-wavelength Free Electron Laser

XUV and X-ray Free Electron Lasers (FELs) produce short wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilised for many experiments previously possible at long wavelengths only: multiphoton ionization, pumping an atomic laser, and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because Self- Amplified Spontaneous Emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and two-colour emission is predicted to be coherent. Here we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5 nm ionized neon, and the asymmetry of the photoelectron angular distribution was controlled by adjusting the phase, with temporal resolution 3 attoseconds. This opens the door to new shortwavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity.

physics.optics↗

arXiv2016

Machine learning applied to single-shot x-ray diagnostics in an XFEL

X-ray free-electron lasers (XFELs) are the only sources currently able to produce bright few-fs pulses with tunable photon energies from 100 eV to more than 10 keV. Due to the stochastic SASE operating principles and other technical issues the output pulses are subject to large fluctuations, making it necessary to characterize the x-ray pulses on every shot for data sorting purposes. We present a technique that applies machine learning tools to predict x-ray pulse properties using simple electron beam and x-ray parameters as input. Using this technique at the Linac Coherent Light Source (LCLS), we report mean errors below 0.3 eV for the prediction of the photon energy at 530 eV and below 1.6 fs for the prediction of the delay between two x-ray pulses. We also demonstrate spectral shape prediction with a mean agreement of 97%. This approach could potentially be used at the next generation of high-repetition-rate XFELs to provide accurate knowledge of complex x-ray pulses at the full repetition rate.

physics.data-an↗

arXiv2015

Pressure and magnetic-field effects on metal-insulator transitions of bulk and domain-wall states in pyrochlore iridates

We have explored the critical metal-insulator phenomena for pyrochlore-type $R_2$Ir$_2$O$_7$, in which electron correlation strength and magnetic configuration are systematically controlled by varying the average rare-earth ionic radius ($R$=Nd$_{1-x}$Pr$_{x}$ and Sm$_{y}$Nd$_{1-y}$), external pressure, and magnetic field. Metal-insulator transitions in bulk are caused by increasing $x$ or tuning external pressure, indicating that the effective electron correlation is responsible for the transition. The metallic state intervenes between the paramagnetic insulating and antiferromagnetically ordered insulating phases for \SNIO ($y$=0.7-0.9), reminiscent of the first-order Mott transition. Furthermore, the metal-to-insulator crossover is observed (around $y$=0.7) for the charge transport on magnetic domain walls in the insulating bulk. An application of magnetic field also drives metal-insulator transitions for \NPIO in which a variety of exotic topological quantum states are potentially realized.

cond-mat.str-el↗

arXiv2015

Magnetic field-induced insulator-semimetal transition in a pyrochlore Nd2Ir2O7

We have investigated magneto-transport properties in a single crystal of pyrochore-type Nd2Ir2O7. The metallic conduction is observed on the antiferromagnetic domain walls of the all-in all-out type Ir-5d moment ordered insulating bulk state, that can be finely controlled by external magnetic field along [111]. On the other hand, an applied field along [001] induces the bulk phase transition from insulator to semimetal as a consequence of the field-induced modification of Nd-4f and Ir-5d moment configurations. A theoretical calculation consistently describing the experimentally observed features suggests a variety of exotic topological states as functions of electron correlation and Ir-5d moment orders which can be finely tuned by choice of rare-earth ion and by magnetic field, respectively.

cond-mat.mtrl-sci↗

arXiv2014

Watching the acetylene vinylidene intramolecular reaction in real time

It is a long-standing dream of scientists to capture the ultra-fast dynamics of molecular or chemical reactions in real time and to make a molecular movie. With free-electron lasers delivering extreme ultraviolet (XUV) light at unprecedented intensities, in combination with pump-probe schemes, it is now possible to visualize structural changes on the femtosecond time scale in photo-excited molecules. In hydrocarbons the absorption of a single photon may trigger the migration of a hydrogen atom within the molecule. Here, such a reaction was filmed in acetylene molecules (C2H2) showing a partial migration of one of the protons along the carbon backbone which is consistent with dynamics calculations on ab initio potential energy surfaces. Our approach opens attractive perspectives and potential applications for a large variety of XUV-induced ultra-fast phenomena in molecules relevant to physics, chemistry, and biology.

physics.atm-clus↗

arXiv2013

Time-Resolved Measurement of Interatomic Coulombic Decay in Ne_2

The lifetime of interatomic Coulombic decay (ICD) [L. S. Cederbaum et al., Phys. Rev. Lett. 79, 4778 (1997)] in Ne_2 is determined via an extreme ultraviolet pump-probe experiment at the Free-Electron Laser in Hamburg. The pump pulse creates a 2s inner-shell vacancy in one of the two Ne atoms, whereupon the ionized dimer undergoes ICD resulting in a repulsive Ne^{+}(2p^{-1}) - Ne^{+}(2p^{-1}) state, which is probed with a second pulse, removing a further electron. The yield of coincident Ne^{+} - Ne^{2+} pairs is recorded as a function of the pump-probe delay, allowing us to deduce the ICD lifetime of the Ne_{2}^{+}(2s^{-1}) state to be (150 +/- 50) fs in agreement with quantum calculations.

physics.atm-clus↗

arXiv2013

Efficient Site-specific Low-energy Electron Production via Interatomic Coulombic Decay Following Resonant Auger Decay

We identified interatomic Coulombic decay (ICD) channels in argon dimers after spectator-type resonant Auger decay $2p^{-1}~3d \to 3p^{-2}3d, 4d$ in one of the atoms, using momentum resolved electron-ion-ion coincidence. The results illustrate that the resonant core excitation is a very efficient way of producing slow electrons at a specific site, which may cause localized radiation damage. We find also that ICD rate for $3p^{-2}4d$ is significantly lower than that for $3p^{-2}3d$.

physics.chem-ph↗

arXiv2012

Deep inner-shell multiphoton ionization by intense x-ray free-electron laser pulses

We have investigated multiphoton multiple ionization dynamics of argon and xenon atoms using a new x-ray free electron laser (XFEL) facility, SPring-8 Angstrom Compact free electron LAser (SACLA) in Japan, and identified that highly charged Xe ions with the charge state up to +26 are produced predominantly via four-photon absorption as well as highly charged Ar ions with the charge state up to +10 are produced via two-photon absorption at a photon energy of 5.5 keV. The absolute fluence of the XFEL pulse, needed for comparison between theory and experiment, has been determined using two-photon processes in the argon atom with the help of benchmark ab initio calculations. Our experimental results, in combination with a newly developed theoretical model for heavy atoms, demonstrate the occurrence of multiphoton absorption involving deep inner shells.

physics.atom-ph↗

arXiv2012

Photoelectron Angular Distributions for Two-photon Ionization of Helium by Ultrashort Extreme Ultraviolet Free Electron Laser Pulses

Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.

physics.atom-ph↗

arXiv2012

Experimental Verification of the Chemical Sensitivity of Two-Site Double Core-Hole States Formed by an X-ray FEL

We have performed X-ray two-photon photoelectron spectroscopy (XTPPS) using the Linac Coherent Light Source (LCLS) X-ray free-electron laser (FEL) in order to study double core-hole (DCH) states of CO2, N2O and N2. The experiment verifies the theory behind the chemical sensitivity of two-site (ts) DCH states by comparing a set of small molecules with respect to the energy shift of the tsDCH state and by extracting the relevant parameters from this shift.

physics.chem-ph↗

arXiv2011

Distillation of hydrogen isotopes for polarized HD target

We have developed a cryogenic distillation system to purify Hydrogen-Deuteride (HD) gas for a polarized HD target in LEPS experiments at SPring-8. A small amount of ortho-H$_2$ ($\sim$0.01%) in the HD gas plays an important role in efficiently polarizing the HD target. Since there are 1$\sim$5% impurities of H$_2$ and D$_2$ in commercially available HD gases, it is inevitable that the HD gas is purified up to $\sim$99.99%. The distillation system has a cryogenic pot (17$\sim$21 K) containing many small stainless steel cells called Heli-pack. Commercial HD gas with an amount of 5.2 mol is fed into the pot. We carried out three distillation runs by changing temperatures (17.5 K and 20.5 K) and gas extraction speeds (1.3 ml/min and 5.2 ml/min). The extracted gas was analyzed by using a gas analyzer system combining a quadrupole mass spectrometer with a gas chromatograph. The HD gas of 1 mol with a purity better than 99.99% has been successfully obtained. The effective NTS (Number of Theoretical Stages), which is an indicator of the distillator performances, is obtained as 37.2$\pm$0.6. This value is in reasonable agreement with a designed value of 37.9. The HD target is expected to be efficiently polarized under a well-controlled condition by doping an optimal amount of ortho-H$_2$ to the purified HD gas.

physics.ins-det↗