Fluorescence Time Delay in Multistep Auger Decay as an Internal Clock.

Differences in postcollision interaction (PCI) effects on Kr L_{3}M_{4,5}M_{4,5} Auger electron spectra were observed, depending on whether the initial photoionization occurred slightly above the K threshold or slightly above the L_{3} threshold. For the former, KL fluorescence emission most likely happens and then Auger processes due to the L_{3} hole follow. The time delay due to fluorescence causes a reduced shift of the Auger peak and tailing toward lower energy, since the Auger overtaking of the photoelectron happens later in time and at a location farther away from the ionic core, compared to the case for the simple one-step L_{3}M_{4,5}M_{4,5} Auger decay after L-shell photoionization. Time-dependent theory for PCI in multistep processes agrees well with experiment, illustrating the effect as an internal clock for the time-sequence of the dynamical process.

Evidence for Weakly Correlated Oxygen Holes in the Highest-T_{c} Cuprate Superconductor HgBa_{2}Ca_{2}Cu_{3}O_{8+δ}.

We study the electronic structure of HgBa_{2}Ca_{2}Cu_{3}O_{8+δ} (Hg1223; T_{c}=134 K) using photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS). Resonant valence band PES across the O K edge and Cu L edge identifies correlation satellites originating in O 2p and Cu 3d two-hole final states, respectively. Analyses using the experimental O 2p and Cu 3d partial density of states show quantitatively different on-site Coulomb energy for the Cu site (U_{dd}=6.5±0.5 eV) and O site (U_{pp}=1.0±0.5 eV). Cu_{2}O_{7}-cluster calculations with nonlocal screening explain the Cu 2p core level PES and Cu L-edge XAS spectra, confirm the U_{dd} and U_{pp} values, and provide evidence for the Zhang-Rice singlet state in Hg1223. In contrast to other hole-doped cuprates and 3d-transition metal oxides, the present results indicate weakly correlated oxygen holes in Hg1223.

Resonant inelastic x-ray scattering and photoemission measurement of O2: Direct evidence for dependence of Rydberg-valence mixing on vibrational states in O 1s → Rydberg states.

High-resolution resonant inelastic x-ray scattering (RIXS) and low-energy photoemission spectra of oxygen molecules have been measured for investigating the electronic structure of Rydberg states in the O 1s → σ* energy region. The electronic characteristics of each Rydberg state have been successfully observed, and new assignments are made for several states. The RIXS spectra clearly show that vibrational excitation is very sensitive to the electronic characteristics because of Rydberg-valence mixing and vibronic coupling in O2. This observation constitutes direct experimental evidence that the Rydberg-valence mixing characteristic depends on the vibrational excitation near the avoided crossing of potential surfaces. We also measured the photoemission spectra of metastable oxygen atoms (O*) from O2 excited to 1s → Rydberg states. The broadening of the 4p Rydberg states of O* has been found with isotropic behavior, implying that excited oxygen molecules undergo dissociation with a lifetime of the order of 10 fs in 1s → Rydberg states.

Quantifying the critical thickness of electron hybridization in spintronics materials.

In the rapidly growing field of spintronics, simultaneous control of electronic and magnetic properties is essential, and the perspective of building novel phases is directly linked to the control of tuning parameters, for example, thickness and doping. Looking at the relevant effects in interface-driven spintronics, the reduced symmetry at a surface and interface corresponds to a severe modification of the overlap of electron orbitals, that is, to a change of electron hybridization. Here we report a chemically and magnetically sensitive depth-dependent analysis of two paradigmatic systems, namely La1-xSrxMnO3 and (Ga,Mn)As. Supported by cluster calculations, we find a crossover between surface and bulk in the electron hybridization/correlation and we identify a spectroscopic fingerprint of bulk metallic character and ferromagnetism versus depth. The critical thickness and the gradient of hybridization are measured, setting an intrinsic limit of 3 and 10 unit cells from the surface, respectively, for (Ga,Mn)As and La1-xSrxMnO3, for fully restoring bulk properties.

Charge transfer to ground-state ions produces free electrons.

Inner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters.

Carotid plaque characterization using 3D T1-weighted MR imaging with histopathologic validation: a comparison with 2D technique.

BACKGROUND AND PURPOSE: 3D FSE T1WI has recently been used for carotid plaque imaging, given the potential advantages in contrast and spatial resolutions. However, its diagnostic performance remains unclear. Hence, we compared the ability of this technique to readily assess plaque characteristics with that of conventional images and validated the results with histologic classification. MATERIALS AND METHODS: We prospectively examined 34 patients with carotid stenosis who underwent carotid endarterectomy by using 1.5T scanners and obtained 3D-FSE T1WI and 2D spin-echo T1WI scans. After generating reformatted images obtained from the 3D-FSE T1-weighted images, we calculated the contrast ratios for the plaques and the adjacent muscles and compared these findings with the pathologic classifications. RESULTS: Carotid plaques were histologically classified as types VII, VIII, IV-V, or VI. With 3D-FSE T1WI, the range of contrast ratios for each classification was the following: 0.94-0.97 (median, 0.95), 0.95-1.29 (median, 1.10), 1.33-1.54 (median, 1.42), and 1.53-2.12 (median, 1.80), respectively. With 2D imaging, the range of contrast ratios for each classification was the following: 0.79-1.02 (median, 0.90), 0.88-1.19 (median, 1.01), 1.17-1.46 (median, 1.23), and 1.55-2.51 (median, 2.07), respectively. Results were significantly different among the 4 groups (P < .001). Sensitivity and specificity for discriminating vulnerable plaques (IV-VI) from stable plaques (VII, VIII) were both 100% for the 3D technique and 100% and 91%, respectively, for the 2D technique. CONCLUSIONS: 3D-FSE T1WI accurately characterizes intraplaque components of the carotid artery, with excellent sensitivity and specificity compared with those of 2D-T1WI.

Temperature Dependence of Magnetically Active Charge Excitations in Magnetite across the Verwey Transition.

We study the electronic structure of bulk single crystals and epitaxial films of Fe_{3}O_{4}. Fe 2p core level spectra show clear differences between hard x-ray (HAX) and soft x-ray photoemission spectroscopy (PES). The bulk-sensitive spectra exhibit temperature (T) dependence across the Verwey transition, which is missing in the surface-sensitive spectra. By using an extended impurity Anderson full-multiplet model-and in contrast to an earlier peak assignment-we show that the two distinct Fe species (A and B site) and the charge modulation at the B site are responsible for the newly found double peaks in the main peak above T_{V} and its T-dependent evolution. The Fe 2p HAXPES spectra show a clear magnetic circular dichroism (MCD) in the metallic phase of magnetized 100-nm-thick films. The model calculations also reproduce the MCD and identify the contributions from magnetically distinct A and B sites. Valence band HAXPES shows a finite density of states at E_{F} for the polaronic half metal with a remnant order above T_{V} and a clear gap formation below T_{V}. The results indicate that the Verwey transition is driven by changes in the strongly correlated and magnetically active B-site electronic states, consistent with resistivity and optical spectra.

Observation of quadrupole helix chirality and its domain structure in DyFe3(BO3)4.

Resonant X-ray diffraction (RXD) uses X-rays in the vicinity of a specific atomic absorption edge and is a powerful technique for studying symmetry breaking by motifs of various multipole moments, such as electric monopoles (charge), magnetic dipoles (spin) and electric quadrupoles (orbital). Using circularly polarized X-rays, this technique has been developed to verify symmetry breaking effects arising from chirality, the asymmetry of an object upon its mirroring. Chirality plays a crucial role in the emergence of functionalities such as optical rotatory power and multiferroicity. Here we apply spatially resolved RXD to reveal the helix chirality of Dy 4f electric quadrupole orientations and its domain structure in DyFe3(BO3)4, which shows a reversible phase transition into an enantiomorphic space-group pair. The present study provides evidence for a helix chiral motif of quadrupole moments developed in crystallographic helix chirality.

Existence of orbital order and its fluctuation in superconducting Ba(Fe(1-x)Co(x))2As2 single crystals revealed by x-ray absorption spectroscopy.

We performed temperature dependent x-ray linear dichroism (XLD) experiments on an iron pnictide system, Ba(Fe(1-x)Co(x))2As2 with x=0.00, 0.05, 0.08, and 0.10 to experimentally verify the existence of orbital ordering (OO). Substantial XLD was observed in polarization dependent x-ray absorption spectra of Fe L edges. By exploiting the difference in the temperature dependent behaviors, OO, and structure contributions to XLD could be clearly separated. The observed OO signal indicates different occupation numbers for d(yz) and d(zx) orbitals and supports the existence of ferro-OO. The results are also consistent with the theoretical prediction. Moreover, we find substantial OO signal well above the structural and magnetic transition temperatures, which suggests the existence of strong OO fluctuations up to high temperatures.

Development of automated 3-dimensional tissue fabrication system Tissue Factory - Automated cell isolation from tissue for regenerative medicine.

We have developed a new automated cell isolation system as one of the modules of automated cell sheet production system named Tissue-Factory (T-Factory). This system enables isolation of the target cells from tissue. Using this new system, we successfully isolated skeletal myoblast from skeletal muscle tissue. The cell isolation system makes us stably prepare cell suspension from each tissue automatically and safely. Isolation of skeletal myoblasts will contribute to labor-saving cell cultivation and operational stability, and lead further process in tissue engineering and regenerative medicine.

Role of Ti 3d carriers in mediating the ferromagnetism of Co∶TiO2 anatase thin films.

We study the surface and bulk electronic structure of the room-temperature ferromagnet Co∶TiO(2) anatase films using soft- and hard-x-ray photoemission spectroscopy with probe sensitivities of ∼1 and ∼10 nm, respectively. We obtain direct evidence of metallic Ti(3+) states in the bulk, which get suppressed to give a surface semiconductor, thus indicating the difference in electronic structure between surface and bulk. X-ray absorption and resonant photoemission spectroscopy reveal Ti(3+) electrons at the Fermi level (E(F)) and high-spin Co(2+) electrons occurring away from E(F). The results show the importance of the charge neutrality condition: Co(2+)+V(O)(2-)+2Ti(4+)↔Co(2+)+2Ti(3+) (V(O) is oxygen vacancy), which gives rise to the elusive Ti 3d carriers mediating ferromagnetism via the Co 3d-O 2p-Ti 3d exchange interaction pathway of the occupied orbitals.

Analysis of sexually dimorphic expression of genes at early gonadogenesis of pejerrey Odontesthes bonariensis using a heterologous microarray.

The process of morphological development of a differentiated gonad from an undifferentiated primordium is a very important step of gonadogenesis. Studies on sexually dimorphic gene expression are important to increase our understanding of this process and to investigate how environmental factors such as temperature can regulate gonadal development. The aim of this study was to identify putative genes involved in sex differentiation in pejerrey (Odontesthes bonariensis) reared at male- and female-producing temperatures (MPT and FPT, respectively) using a microarray heterologous from the medaka (Oryzias latipes), a closely phylogenetic species. Genes related to numerous processes presented higher expression at MPT, including those involved in muscular contraction, metabolic pathways, developmental processes, and reproduction. Genes induced by FPT were classified under the gene ontology terms of response to stimulus, transport and proteolysis. From genes selected for validation, at MPT ndrg3 expression was observed in the somatic cells, whereas pen-2 was detected in germ cells in the caudal portion of the gonads, where no apoptotic signals were observed. Finally, hsp90 was highly expressed in somatic cells of the gonads at the FPT. The results suggest that the interplay of pro-apoptotic and anti-apoptotic genes is important during the masculinization process and for the prevention of sterility following exposure to warm temperatures.

Development of cell culture monitoring system and novel non-contact pH measurement.

This paper describes a cell culture monitoring system for regenerative medicine. To realize this monitoring system, a new culture vessel and a removable measurement unit were proposed. The measurement unit was installed in the culture vessel and it was used to measure important cell culture parameters (e.g., temperature, CO(2) level, and pH). Thus, the status of the culture could be monitored. In addition, we developed a novel noninvasive method based on spectrophotometry for measuring pH. This method is a non-contact method that permits noninvasive and contamination-free pH measurement. The spectroscopic pH measurements agreed well with pH measurements using an electrode. The error was within 0.02; thus, the new pH measurement method is sufficiently accurate for cell culture. This new system is expected to contribute to advances in tissue engineering and regenerative medicine.

Evidence for a correlated insulator to antiferromagnetic metal transition in CrN.

We investigate the electronic structure of chromium nitride (CrN) across the first-order magnetostructural transition at T(N)∼286 K. Resonant photoemission spectroscopy (PES) shows a gap in the 3d partial density of states at the Fermi level and an on-site Coulomb energy U∼4.5 eV, indicating strong electron-electron correlations. Bulk-sensitive high-resolution (6 meV) laser PES reveals a clear Fermi edge indicating an antiferromagnetic metal below T(N). Hard x-ray Cr 2p core-level PES shows T-dependent changes across T(N) which originate from screening due to coherent states as substantiated by cluster model calculations using the experimentally observed U. Electrical resistivity confirms an insulator above T(N) (E(g)∼70 meV) becoming a disordered metal below T(N). Thus, CrN transforms from a correlated insulator to an antiferromagnetic metal, coupled to the magnetostructural transition.

Out-of-plane nesting driven spin spiral in ultrathin Fe/Cu(001) films.

Epitaxial ultrathin Fe films on fcc Cu(001) exhibit a spin spiral (SS), in contrast to the ferromagnetism of bulk bcc Fe. We study the in-plane (IP) and out-of-plane (OP) Fermi surfaces (FSs) of the SS in 8 monolayer Fe/Cu(001) films using energy-dependent soft-x-ray momentum-resolved photoemission spectroscopy. We show that the SS originates in nested regions confined to OP FSs, which are drastically modified compared to IP FSs. From precise reciprocal-space maps in successive zones, we obtain the associated real space compressive strain of 1.5+/-0.5% along c axis. An autocorrelation analysis quantifies the incommensurate ordering vector q=(2pi/a)(0,0, approximately 0.86), favoring a SS and consistent with magneto-optic Kerr effect experiments. The results reveal the importance of IP and OP FS mapping for ultrathin films.

Establishment of a strain inheriting a sex-linked SNP marker in Patagonian pejerrey (Odontesthes hatcheri), a species with both genotypic and temperature-dependent sex determination.

The Patagonian pejerrey Odontesthes hatcheri is an atherinopsid species presenting genotypic sex determination (GSD) at intermediate temperatures and temperature-dependent sex determination at the low and high ranges of thermal tolerance. A recent study revealed the presence of a sex-linked SNP marker in some males of this species, but a strain which inherits the marker faithfully has not been established. This research was conducted to develop such a strain, for use as a tool to study the molecular mechanisms of gonadal sex differentiation and sexual dimorphism, and to obtain basic information on the GSD mode in this species. For these purposes, we performed backcrosses and full-sibling crosses using males and females whose presumptive genotypic sex was inferred from the presence of the sex-linked SNP marker. Four backcrosses between SNP(-) daughters and their SNP(+) father generated balanced sex ratios with the phenotypic sex matching the genotypic sex in most cases (98.21%) at an intermediate, sexually neutral temperature (21 degrees C). Full-sibling crosses between these four SNP(-) females and their SNP(+) brothers produced three progenies with balanced sex ratios and one with 94.4% males. The results of this study confirm that a strain inheriting the sex-linked SNP marker was successfully developed. Moreover, the inheritance pattern of the marker and the sex ratios of the progenies provide strong evidence that the GSD mode in O. hatcheri is the XX-XY system.

Calibration system for pulse spectrophotometry using a double-layer pulsation flow-cell.

We have studied noninvasive devices for measuring total hemoglobin and hemoglobin derivatives such as carboxyhemoglobin (COHb) and methemoglobin (MetHb). A calibration procedure needs to be developed to evaluate or calibrate these devices and pulse oximeters for clinical practice. However, people and animals are sometimes exposed to risk when they are used for calibration. In this paper, we propose a new in vitro calibration system for a pulse photometer. This system has a novel double-layer pulsation flow-cell that incorporates both venous and arterial blood flow. Using the calibration system, we are able to measure the in vitro pulsatile optical density ratio (Phivt). The measured Phivt agrees well with the in vivo pulsatile optical density ratio (Phivi). This system simulates an in vivo environment with high accuracy and enables safe calibration. Consequently, the calibration system is able to standardize the performance and accuracy of pulse photometry.

An ultrahigh-vacuum apparatus for resonant diffraction experiments using soft x rays (hnu=300-2000 eV).

We have developed an ultrahigh-vacuum instrument for resonant diffraction experiments using polarized soft x rays in the energy range of hnu=300-2000 eV at beamline BL17SU of SPring-8. The diffractometer consists of modified differentially pumped rotary feedthroughs for theta-2theta stages, a sample manipulator with motor-controlled x-y-z-, tilt (chi)-, and azimuth (phi)-axes, and a liquid helium flow-type cryostat for temperature dependent measurements between 30 and 300 K. Test results indicate that the diffractometer exhibits high reproducibility (better than 0.001 degrees ) for a Bragg reflection of alpha-quartz 100 at a photon energy of hnu=1950 eV. Typical off- and on-resonance Bragg reflections in the energy range of 530-1950 eV could be measured using the apparatus. The results show that x-ray diffraction experiments with energy-, azimuth-, and incident photon polarization-dependence can be reliably measured using soft x rays in the energy range of approximately 300-2000 eV. The facility can be used for resonant diffraction experiments across the L-edge of transition metals, M-edge of lanthanides, and up to the Si K-edge of materials.

Recoil effect of photoelectrons in the Fermi edge of simple metals.

High energy resolution photoelectron spectroscopy of conduction electrons in the vicinity of the Fermi edge in Al and Au at excitation energies of 880 and 7940 eV was carried out using synchrotron radiation. For the excitation energy of 7940 eV, the observed Fermi energy of Al shows a remarkable shift to higher binding energy as compared with that of Au, with accompanying broadening. This is due to the recoil effect of the emitted photoelectrons. The observed spectra are well reproduced by a simple model of Bloch electrons based on the isotropic Debye model.

Development of a compact mock circulation system and a new flow-cell model for pulse spectrophotometry.

We have developed an extremely compact mock circulation system. This system can simulate artery blood circulation and generate a pulse wave with a very small amount of blood. We were also able to measure the in vitro pulsatile optical density ratio (Phivt) using this system with a flow cell [1]. Results showed a difference between Phivt and the in vivo pulsatile optical density ratio (Phivi) for the same oxygen saturations. To explain this difference, we proposed a new flow-cell model that includes venous flow and arterial flow. Because these systems can simulate the in vivo environment with very accurately, they can be applied to various pulse spectrophotometry studies. Moreover, the required blood volume is very small so the system can evaluate artificial blood or artificial red cells at very low cost. Thus, this system can reduce the time and cost of developing new pulse photometry techniques and other medical equipment.