Bonding in liquid carbon studied by time-resolved x-ray absorption spectroscopy

Even the most basic properties of liquid carbon have long been debated due to the challenge of studying the material at the required high temperature and pressure. Liquid carbon is volatile and thus inherently transient in an unconstrained environment. In this paper we use a new technique of picosecond time-resolved x-ray absorption spectroscopy to study the bonding of liquid carbon at densities near that of the solid. As the density of the liquid increases, we see a change from predominantly sp-bonded atomic sites to a mixture of sp, sp2, and sp3 sites and compare these observations with molecular dynamics simulations.     

Properties of liquid silicon observed by time-resolved x-ray absorption spectroscopy

Time-resolved x-ray spectroscopy at the Si L edges is used to probe the electronic structure of an amorphous Si foil as it melts following absorption of an ultrafast laser pulse. Picosecond temporal resolution allows observation of the transient liquid phase before vaporization and before the liquid breaks up into droplets. The melting causes changes in the spectrum that match predictions of molecular dynamics and ab initio x-ray absorption codes.     

Pulsed-laser annealing of GaAs surface studied by time-resolved second-harmonic generation in reflection

Experimental results are presented on the time dependence of the second-harmonic generation (SHG) of a mode-locked Q-switched Nd: YAG laser in reflection from both amorphous and crystalline GaAs surfaces during the pulsed-laser annealing under ruby laser irradiation. A dramatic increase of SHG by more than two orders of magnitude due to recrystallization of the noncentrosymmetric GaAs lattice in the process of pulsed-laser annealing is observed and the duration of surface recrystallization is measured to be not greater than 30–40 ns. The results can be fully understood in terms of the melting model of laser annealing.     

Ultrafast structural dynamics studied by kilohertz time-resolved x-ray diffraction

Ultrashort multi-ke V x-ray pulses are generated by electron plasma produced by the irradiation of femtosecond pulses on metals. These sub-picosecond x-ray pulses have extended the field of x-ray spectroscopy into the femtosecond time domain. However, pulse-to-pulse instability and long data acquisition time restrict the application of ultrashort x-ray systems operating at low repetition rates. Here we report on the performance of a femtosecond laser plasma-induced hard x-ray source that operates at 1-k Hz repetition rate, and provides a flux of 2.0 × 1010 photons/s of Cu Kαradiation. Using this system for time-resolved x-ray diffraction experiments, we record in real time, the transient processes and structural changes induced by the interaction of 400-nm femtosecond pulse with the surface of a 200-nm thick Au(111) single crystal.     

Local structure of LiCoO(2) nanoparticles studied by Co K-edge x-ray absorption spectroscopy

We have studied the local structure of LiCoO(2) nanoparticles by Co K-edge x-ray absorption spectroscopy as a function of particle size. Extended x-ray absorption fine structure data reveal substantial changes in the near neighbor distances and the associated mean square relative displacements with decreasing particle size. X-ray absorption near edge structure spectra show clear local geometrical changes with decreasing particle size, similar to those that appear in the charging (delithiation) process. The results suggest that the LiCoO(2) nanoparticles are characterized by a large atomic disorder confined to the Co-O octahedra, similar to the distortions generated during the delithiation, and this disorder should be the primary limiting factor for a reversible diffusion of Li ions when nanoparticles of LiCoO(2) are used as cathode material in rechargeable Li ion batteries.     

Ultrasoft x-ray Bremsstrahlung isochromatic spectra from 300-2000 eV electrons on Ar and Kr

For the first time the bremsstrahlung effect was studied experimentally in the spectral region of 6.5-10 nm with 300-2000 eV electron scattering on Ar and Kr atoms. The isochromatic curves displayed maxima at electron energies of approximately = 0.7 keV (Ar) and approximately =1 keV (Kr); their positions are almost independent of the radiation wavelength in the range studied. These experimental data cannot be treated in the framework of theory based on the first Born approximation. A phenomenological modification of the quasiclassical (soft-photon) approximation is proposed which gives a qualitative treatment of data.     

Pulsed-laser photolysis of Mn2(CO)10: A time-resolved fluorescence study

Mn₂(CO)₁₀ was photolysed in the gas phase by the XeCl-excimer laser with fluence in the range 25–300 mJ/cm² and a dye laser. The UV/VIS emission of the products was probed on a nanosecond time scale. The emission from excited states of metal atoms was detected only. The Mn atoms are predominantly formed in their ground statea ⁶ S _{2 1/2}. The absorption of one photon and the subsequent relaxation process leads to the formation ofz ⁶ P _J ⁰ (J = 11/2, 21/2, 31/2) states and emission of photons at a wavelength of 403 nm. The formation of the excited statese ⁸ D _{5 1/2},z ⁶ F _{4 1/2} ⁰ ande ⁶ D _{4 1/2} and the subsequent emission observed at wavelengths of 357, 383 and 446 nm requires the absorption of two photons by the ground-state Mn atoms. In addition, transition from thea ⁶ D _j (J = 11/2, 21/2) lower states were observed in the wavelength-resolved Laser-Induced Fluorescence (LIF) spectra.     

Radical cations of n-alkanes in irradiated solutions as studied by time-resolved magnetic field effects

The time-resolved magnetic field effect in the recombination fluorescence of spin-correlated radical ion pairs has been measured to study n-alkane radical cations in irradiated solutions at room temperature. The magnetic field effect was recorded as a ratio of fluorescence decay curves in the 0.1 T and zero magnetic fields for solutions of C₈, C₉, C₁₀, C₁₂, and C₁₆ n-alkanes in n-hexane with addition of 3 × 10^?5 M p-terphenyl-d ₁₄. A distinct maximum at 10–30 ns followed by a slowly decaying plateau was observed for all the solutions. Simulation shows that the maximum corresponds to an unresolved ESR spectrum with the peak-to-peak line-width ranging from about 1.6mT to 0.5mT for C₈ to C₁₆ radical cations. The unresolved structure is believed to result from the hyperfine couplings with many protons of the radical cation, the increase in the number of interacting protons compared with low temperature matrices being caused by the methyl group rotation and conformational motion of the carbon chain. With increase in concentration of dissolved n-alkane, the maximum in the curves first moves to longer times and finally disappears; this was attributed to the narrowing of ESR spectrum contour due to degenerate electron exchange.     

Large local disorder in superconducting K(0.8)Fe(1.6)Se2 studied by extended x-ray absorption fine structure

We have measured the local structure of superconducting K(0.8)Fe(1.6)Se(2) chalcogenide (T(c) = 31.8 K) by temperature dependent polarized extended x-ray absorption fine structure (EXAFS) at the Fe and Se K-edges. We find that the system is characterized by a large local disorder. The Fe-Se and Fe-Fe distances are found to be shorter than the distances measured by diffraction, while the corresponding mean square relative displacements reveal large Fe-site disorder and relatively large c-axis disorder. The local force constant for the Fe-Se bondlength (k ~ 5.8 eV ?(-2)) is similar to the one found in the binary FeSe superconductor, however, the Fe-Fe bondlength appears to be flexible (k ~ 2.1 eV ?(-2)) in comparison to the binary FeSe (k ~ 3.5 eV ?(-2)), an indication of partly relaxed Fe-Fe networks in K(0.8)Fe(1.6)Se(2). The results suggest a glassy nature for the title system, with the superconductivity being similar to that in the granular materials.     

Electronic structure of warm dense copper studied by ultrafast x-ray absorption spectroscopy

We use time-resolved x-ray absorption spectroscopy to investigate the unoccupied electronic density of states of warm dense copper that is produced isochorically through the absorption of an ultrafast optical pulse. The temperature of the superheated electron-hole plasma, which ranges from 4000 to 10?000 K, was determined by comparing the measured x-ray absorption spectrum with a simulation. The electronic structure of warm dense copper is adequately described with the high temperature electronic density of state calculated by the density functional theory. The dynamics of the electron temperature is consistent with a two-temperature model, while a temperature-dependent electron-phonon coupling parameter is necessary.     

利用x射线小角散射技术研究微晶硅薄膜的微结构

采用x射线小角散射（SAXS）技术研究了由射频等离子体增强化学气相沉积（rf-PECVD）、 热丝化学气相沉积(HWCVD)和等离子体助热丝化学气相沉积(PE-HWCVD)技术制备的微晶硅（ μc-Si:H）薄膜的微结构.实验发现，在相同晶态比的情况下，PECVD沉积的μc-Si:H薄膜微 空洞体积比小，结构较致密，HWCVD沉积的μ-Si:H薄膜微空洞体积比大，结构较为疏松，PE -HWCVD沉积的μc-Si:H薄膜，由于等离子体的敲打作用，与HWCVD样品相比，微结构得到明 显改善.采用HWCVD二步法和PE-HWCVD加适量Ar离子分别沉积μc-Si:H薄膜，实验表明，微结 构参数得到了进一步改善.45°倾角的SAXS测量显示，不同方法制备的μc-Si:H薄膜中微空 洞分布都呈各向异性.红外光谱测量也证实了SAXS的结果. 关键词： 微晶硅薄膜 微结构 微空洞 x射线小角散射     

The coordination of aluminum and silicon in zeolites as studied by x-ray spectrometry

The aluminum K_β line was used to determine the coordination state of aluminum in acid forms of zeolite Y. The A1K_β line of sodium zeolite A was used as a reference in the determination of the line shift, zinc spinel was used as the standard for hexacoordinated Al. The difference in the position of the AlK_β line between these two samples is about 0.240° 2θ. The energy of the AlK_β line differed slightly with Si/Al ratio and crystal structure. Therefore, the sodium form of the zeolite to be investigated, in this instance NaY, was the preferred standard for tetracoordinated Al.All the aluminum in a true hydrogen zeolite Y was found to be tetracoordinated. About 19% of the aluminum in a stabilized hydrogen zeolite Y was hexacoordinated, other samples contained 10 and 12% hexacoordinated Al. It is likely that mixed forms of true HY and stable HY with 0 to 25% hexacoordinated Al can be prepared. The samples of dehydroxylated zeolite Y investigated contained between 30 and 50% hexacoordinated Al, while the silicon remained tetracoordinated.     

Backscattering of low-energy (0–8 eV) electrons by a silicon surface

An experimental apparatus and method for investigating elastic and inelastic backscattering (180°) of low-energy (0–8 eV) monoenergetic electrons by a solid surface are described and the first results are presented for the reflection of electrons by samples of pure single-crystalline silicon with a polished surface (Si), doped p-type single-crystalline silicon with a porous surface (Si-p) as well as H₂O and H₂O₂ passivated porous samples, Si-p + H₂O and Si-p + H₂O₂. A structure due to the excitation of surface plasmons has been observed for the first time in the loss spectra. Features corresponding to a resonance excited state of molecular nitrogen adsorbed on the surface of porous silicon have been observed in the constant residual energy spectra. Zh. Tekh. Fiz. 67, 103–108 (May 1997)     

5f Localization in light actinide compounds studied by L3-edge x-ray absorption

L₃-edge x-ray absorption spectroscopy was applied to electronic structure studies in compounds of U, Np, and Pu. Single-peaked white lines are observed at the L₃ thresholds, which exhibit shifts up to 6 eV to lower energies for the monopnictides and monochalcogenides relative to the tetravalent dioxides. These chemical shifts increase systematically from U to Np and Pu, reflecting an increasing localization of the 5f states.     

Three-dimensional bulk fermiology of CeRu2Ge2 in the paramagnetic phase by soft x-ray hnu-dependent (700-860 eV) ARPES

By virtue of the soft x-ray angle-resolved photoelectron spectroscopy, the three-dimensional bulk fermiology has been successfully performed for a strongly correlated Ce compound, ferromagnet CeRu2Ge2 in the paramagnetic phase. A clear difference of the Fermi surface topology from either band calculation or de Haas-van Alphen results in the ferromagnetic phase is observed and interpreted by considering the difference of the 4f contribution to the Fermi surfaces in the paramagnetic phase.     

Structure of multiple-vacancy (oxygen) centers in irradiated silicon

Analysis of a new paramagnetic spin 1 spectrum, labeled Si-S1, indicates that it corresponds to the neutral charge state of the Si-B1 center in an excited spin-triplet state. An extension of this analysis to the Si-P1, -P2, -P3, -P4, and -P5 centers suggest that these centers comprise a family of defects which consist of a string of neighboring vacancies in a single (110) plane. In particular, it appears that the Si-P1 center is an odd ( 3)-vacancy defect; the Si-P2 center is a 2-vacancy, oxygen defect; the Si-P3 center is a 4-vacancy defect; the Si-P4 center is a 3-vacancy, oxygen defect of symmetry lower than C_2v ; and the Si-P5 center is a 3-vacancy, oxygen defect having C_2v symmetry.     

Femtosecond electron and spin dynamics in Gd(0001) studied by time-resolved photoemission and magneto-optics

Femtosecond electron and spin dynamics of the Gd(0001) surface are investigated by time-resolved photoemission and second harmonic generation. Upon optical excitation the spin polarization of the surface state is reduced by half while its exchange splitting remains nearly unchanged. Electron-magnon interaction is proposed to facilitate electron-spin-flip scattering among spin-mixed surface and bulk states, which provides a mechanism for ultrafast demagnetization.     

Nearest-neighbor configuration in (GaIn)(NAs) probed by x-ray absorption spectroscopy

Ga(1-x)In(x)N(y)As(1-y) is a promising material system for the fabrication of inexpensive "last-mile" optoelectronic components. However, details of its atomic arrangement and the relationship to observed optical properties is not fully known. Particularly, a blueshift of emission wavelength is observed after annealing. In this work, we use x-ray absorption fine structure to study the chemical environment around N atoms in the material before and after annealing. We find that as-grown molecular beam epitaxy material consists of a nearly random distribution of atoms, while postannealed material shows segregation of In toward N. Ab initio simulations show that this short-range ordering creates a more thermodynamically stable alloy and is responsible for blueshifting the emission.