Electron Wave Packet Interference in Atomic Inner-Shell Excitation.

We report the observation of quantum interference between electron wave packets launched from the inner-shell 4d orbital of the Xe atom. Using pairs of femtosecond radiation wave packets from a synchrotron light source, we obtain time-domain interferograms for the inner-shell excitations. This approach enables the experimental verification and control of the quantum interference between the electron wave packets. Furthermore, the femtosecond Auger decay of the inner-shell excited state is tracked. To the best of our knowledge, this is the first observation of wave packet interference in an atomic inner-shell process, and also the first time-resolved experiment on few-femtosecond Auger decay using a synchrotron light source.

Controlling the Orbital Alignment in Atoms Using Cross-Circularly Polarized Extreme Ultraviolet Wave Packets.

We report on the use of pairs of 10-cycle extreme ultraviolet wave packets with attosecond-controlled spacing emitted by individual relativistic electrons within an electron bunch passing through a tandem undulator. Based on the temporal coherent control technique with circular polarization, we succeeded in controlling the excited state alignment in the photoexcitation of helium atoms, which we verified through the observation of oscillation in fluorescence yield depending on the attosecond-controlled delay time. Our work demonstrates the potential of undulator radiation for the generation of longitudinally coherent wave packets suitable for attosecond coherent control, an application which has hitherto been hidden in the incoherent nature of the radiation pulse emitted by a bunch of electrons.

Angular Momentum of Twisted Radiation from an Electron in Spiral Motion.

We theoretically demonstrate for the first time that a single free electron in circular or spiral motion emits twisted photons carrying well-defined orbital angular momentum along the axis of the electron circulation, in adding to spin angular momentum. We show that, when the electron velocity is relativistic, the radiation field contains harmonic components and the photons of lth harmonic carry lℏ total angular momentum for each. This work indicates that twisted photons are naturally emitted by free electrons and are more ubiquitous in laboratories and in nature than ever thought.

Single, double, and triple Auger decays from 1s shake-up states of the oxygen molecule.

The single, double, and triple Auger decays from the 1s shake-up states of O2 have been studied using a multi-electron coincidence method. Efficient populations of two-hole final states are observed in single Auger decays of the π-π* shake-up states, which is understood as a characteristic property of the Auger transitions from shake-up states of an open-shell molecule. The O23+ populations formed by double Auger decays show similar profiles for both the O1s-1 and shake-up states, which is due to the contributions from cascade double Auger processes. While the cascade contributions to the double Auger decays increase with the initial shake-up energy, the probability of direct double Auger processes remains unchanged between the O1s-1 and shake-up states, which implies a weak influence of the excited electron on the double Auger emission that originates from the electron correlation effect.

Stability and dissociation dynamics of N2 (++) ions following core ionization studied by an Auger-electron-photoion coincidence method.

An Auger-electron-photoion coincidence (AEPICO) method has been applied to study the stability and dissociation dynamics of dicationic states after the N K-shell photoionization of nitrogen molecules. From time-of-flight and kinetic energy analyses of the product ions, we have obtained coincident Auger spectra associated with metastable states of N2 (++) ions and dissociative states leading to N2 (++) → N(+) + N(+) and N(++) + N. To investigate the production of dissociative states, we present two-dimensional AEPICO maps which reveal the correlations between the binding energies of the Auger final states and the ion kinetic energy release. These correlations have been used to determine the dissociation limits of individual Auger final states.

Time domain double slit interference of electron produced by XUV synchrotron radiation.

We present a new realization of the time-domain double-slit experiment with photoelectrons, demonstrating that spontaneous radiation from a bunch of relativistic electrons can be used to control the quantum interference of single-particles. The double-slit arrangement is realized by a pair of light wave packets with attosecond-controlled spacing, which is naturally included in the spontaneous radiation from two undulators in series. Photoelectrons emitted from helium atoms are observed in the energy-domain under the condition of detecting them one by one, and the stochastic buildup of the quantum interference pattern on a detector plane is recorded.

Frequency-domain interferometry for the determination of time delay between two extreme-ultraviolet wave packets generated by a tandem undulator.

Synchrotron radiation, emitted by relativistic electrons traveling in a magnetic field, has poor temporal coherence. However, recent research has proved that time-domain interferometry experiments, which were thought to be enabled by only lasers of excellent temporal coherence, can be implemented with synchrotron radiation using a tandem undulator. The radiation generated by the tandem undulator comprises pairs of light wave packets, and the longitudinal coherence within a light wave packet pair is used to achieve time-domain interferometry. The time delay between two light wave packets, formed by a chicane for the electron trajectory, can be adjusted in the femtosecond range by a standard synchrotron technology. In this study, we show that frequency-domain spectra of the tandem undulator radiation exhibit fringe structures from which the time delay between a light wave packet pair can be determined with accuracy on the order of attoseconds. The feasibility and limitations of the frequency-domain interferometric determination of the time delay are examined.

Double-pulsed wave packets in spontaneous radiation from a tandem undulator.

We verify that each wave packet of spontaneous radiation from two undulators placed in series has a double-pulsed temporal profile with pulse spacing which can be controlled at the attosecond level. Using a Mach-Zehnder interferometer operating at ultraviolet wavelengths, we obtain the autocorrelation trace for the spontaneous radiation from the tandem undulator. The results clearly show that the wave packet has a double-pulsed structure, consisting of a pair of 10-cycle oscillations with a variable separation. We also report the characterization of the time delay between the double-pulsed components in different wavelength regimes. The excellent agreement between the independent measurements confirms that a tandem undulator can be used to produce double-pulsed wave packets at arbitrary wavelength.

Dissociation of core-valence doubly excited states in NO followed by atomic Auger decay.

The decay processes of core-valence doubly excited states near the N K edge of NO have been studied using electron spectroscopy. Electron yields measured as a function of photon energy and kinetic energy enable the clear identification of atomic Auger lines associated with the dissociation of doubly excited states. The atomic Auger lines exhibit Doppler profiles, allowing the entire reaction scheme of such dissociation processes to be determined.

Coherent control in the extreme ultraviolet and attosecond regime by synchrotron radiation.

Quantum manipulation of populations and pathways in matter by light pulses, so-called coherent control, is currently one of the hottest research areas in optical physics and photochemistry. The forefront of coherent control research is moving rapidly into the regime of extreme ultraviolet wavelength and attosecond temporal resolution. This advance has been enabled by the development of high harmonic generation light sources driven by intense femtosecond laser pulses and by the advent of seeded free electron laser sources. Synchrotron radiation, which is usually illustrated as being of poor temporal coherence, hitherto has not been considered as a tool for coherent control. Here we show an approach based on synchrotron radiation to study coherent control in the extreme ultraviolet and attosecond regime. We demonstrate this capability by achieving wave-packet interferometry on Rydberg wave packets generated in helium atoms.

Helical Phase Structure of Radiation from an Electron in Circular Motion.

We theoretically show that a single free electron in circular motion radiates an electromagnetic wave possessing helical phase structure, which is closely related to orbital angular momentum carried by it. We experimentally demonstrate it by interference and double-slit diffraction experiments on radiation from relativistic electrons in spiral motion. Our results indicate that photons carrying orbital angular momentum should be created naturally by cyclotron/synchrotron radiations or Compton scatterings in various situations in cosmic space. We propose promising laboratory vortex photon sources in various wavelengths ranging from radio wave to gamma-rays.

Removal of phosphorus from oyster farm mud sediment using a photosynthetic bacterium, Rhodobacter sphaeroides IL106.

Removal of phosphorous compounds from the mud sediment of an oyster farm was carried out by a series of bio-processes under anaerobic conditions. Anaerobic acidogenic fermentation of a mud sediment suspension (200 g wet wt/l artificial sea water) was initially carried out. With the addition of vitamins such as thiamine, nicotinic acid and biotin, acidogenic fermentation was enhanced to yield acetic acid of approximately 2 g/l. Furthermore, approximately 20 mg/l of PO4(3-) (10% of total phosphorus on mud weight) and 5300 mg/l of COD(Cr) (82% of organic matter on mud weight) were released into the culture broth after fermentation for 7 d. The supernatant of this culture broth was used to cultivate Rhodobacter sphaeroides IL106, a denitrifying photosynthetic bacterium. After 4 d, 3.32 g/l of biomass containing carotenoid and ubiquinone was obtained, and COD(Cr) and acetic acid were reduced by 58% and 72%, respectively. In addition, PO4(3-) was reduced by 97%, suggesting that the removal of PO4(3-) from the mud sediment might be possible by combining anaerobic acidogenic fermentation with R. sphaeroides cultivation.

Energy correlation of the three electrons emitted during the triple photoionization of Ar.

We report on an experimental investigation of energy correlation among three electrons emitted in valence triple photoionization (TPI) of Ar. The energy correlations reveal a predominant contribution from sequential TPI processes involving intermediate Ar2+ formation, which suggests that such indirect contributions should be included in the formulation of the threshold law for TPI cross sections. The differential cross section for direct TPI at about 150 eV above threshold producing one slow electron with a few eV kinetic energy is found to have a deeply hollow U-shaped profile in energy sharing between the other two electrons.

X-ray absorption measured in the resonant Auger scattering mode.

We report both experimental and theoretical studies on x-ray absorption measured in the resonant Auger scattering mode of gas phase carbon monoxide near the O1s-->2pi region. Both experiment and theory display a crucial difference between the x-ray absorption profiles obtained in the conventional and resonant scattering modes. Lifetime vibrational interference is the main source of the difference. It is demonstrated that such interference, which arises from a coherent excitation to overlapping intermediate levels, ruins the idea for obtaining x-ray absorption spectra in a lifetime broadening free regime.

Mechanisms of spontaneous two-electron emission from core-excited states of molecular CO.

We demonstrate that the observation of slow electrons emitted in the decay of molecular core-excited states can be a sensitive probe of the double Auger processes, and that in combination with electron-electron coincidence spectroscopy, it can provide clear insight into the mechanisms involved. The present study identifies all cascade Auger paths from the C1s-to-Rydberg states in CO to final states of CO2+. One pathway includes the first directly identified case of molecular level-to-level autoionization of a cation and shows remarkable selectivity for a specific final state.

Multielectron coincidence spectroscopy for core-valence doubly ionized states of CO.

Double photoionization into states which have holes in one core and one valence orbitals has been observed in CO using a state-of-the-art multielectron coincidence method. The core-valence CO2+ structures exhibited on the electron coincidence spectra are assigned by comparison with the available calculation [H. Schulte et al., J. Chem. Phys. 105, 11108 (1996)]. Features of the spectrum confirm that the properties of the CO2+ states are characterized by the interaction between the localized valence holes and the core holes.

Double photoionization into double core-hole states in Xe.

Double photoionization (DPI) leading to double core-hole states of Xe2+ 4d(-2) has been studied using a magnetic bottle time-of-flight spectrometer. The assignments of the Xe2+ 4d(-2) states are confirmed by the Auger lines extracted from fourfold coincidences including two photoelectrons and two Auger electrons. It is estimated that the core-core DPI into Xe2+ 4d(-2) at a photon energy of 301.6 eV has a favored cross section of about 0.3 MB. The intense core-core DPI is due to mixing of the 4d(-2) continuum with the 4p single photoionization, which is manifested in the relative intensities of the Xe2+ 4d(-2) components.

Synthesis and properties of ApU analogues containing 2'-halo-2'-deoxyadenosines. Effects of 2' substituents on oligonucleotide conformation.

Five A-U analogues containing deoxyadenosine or 2'-halo-2'-deoxyadenosines, which are known to have widely different C3'-endo conformer populations according to their electronegativities of the halogen substituents, dAfl-U, dAcl-U, dAbr-U, dAio-U, and dA-U, were synthesized chemically. Characterization of these dimers has been performed by UV absorption, circular dichroism, and proton nuclear magnetic resonance spectroscopy. The results show that the dimers containing 2'-halo-2'-deoxyadenosines have stacked conformations with a geometry similar to that of A-U and the degree of stacking decreases in the order dAfl-U greater than dAcl-U greater than dAbr-U greater than dAio-U. dAcl-U is assumed to have the same degree of stacking as A-U. dA-U takes a more stacked conformation than does dAio-U, but the mode of stacking is different from those of the other dimers. The effects of the 2' substituents on dimer conformation are discussed in terms of electronegativity, molecular size, and hydrophobicity.