Huailiang Xu

Remote time-resolved filament-induced breakdown spectroscopy of biological materials

We report, for what we believe to be the first time, on the feasibility of remote time-resolved filament-induced breakdown spectroscopy (FIBS) of biological materials. The fluorescence from egg white and yeast powder, induced by femtosecond laser pulse filamentation in air, was detected in the backward direction with targets located 3.5 m away from the detection system. The remarkably distinct spectra of egg white and yeast allow us to propose that this technique, time-resolved FIBS, could be potentially useful for remote detection and identification of harmful biological agents.

Understanding the advantage of remote femtosecond laser-induced breakdown spectroscopy of metallic targets

We analyze the advantages of remotely sensing metallic targets using femtosecond laser-induced breakdown spectroscopy by studying the temperature and electron density of the plasma ejected from a lead target produced by femtosecond laser pulse filamentation in ambient air. The electron density of 8×1017cm−3 and the plasma temperature of 6794K were obtained for a 20ns time delay with respect to the laser pulse arriving on the target. With these values the signal is high, while the continuum blackbody radiation is low. The continuum emission in the fluorescence spectra is mainly associated with the supercontinuum of the distorted pulse during filamentation (white light laser) in air and this can be controlled. Extrapolation of the single-shot detection limit shows that this technique of filament-induced breakdown spectroscopy could be extended up to the kilometer range, opening up potential applications in metallurgic industry for remote material analysis and process controls.

Explosive photodissociation of methane induced by ultrafast intense laser

A new type of molecular fragmentation induced by femtosecond intense laser at the intensity of 2 x 10(14) W/cm2 is reported. For the parent molecule of methane, ethylene, n-butane, and 1-butene, fluorescence from H (n = 3-->2), CH (A 2Delta, B 2Sigma-, and C 2Sigma+-->X 2Pi), or C2 (d 3Pi g-->a 3Pi u) is observed in the spectrum. It shows that the fragmentation is a universal property of neutral molecule in the intense laser field. Unlike breaking only one or two chemical bonds in conventional UV photodissociation, the fragmentation caused by the intense laser undergoes vigorous changes, breaking most of the bonds in the molecule, like an explosion. The fragments are neutral species and cannot be produced through Coulomb explosion of multiply charged ion. The laser power dependence of CH (A-->X) emission of methane on a log-log scale has a slope of 10 +/- 1. The fragmentation is thus explained as multiple channel dissociation of the superexcited state of parent molecule, which is created by multiphoton excitation.

Simultaneous detection and identification of multigas pollutants using filament-induced nonlinear spectroscopy

The authors report on an approach for simultaneous monitoring of multigas pollutants based on fluorescence emission of trace gases, induced by the filamentation of intense femtosecond laser pulses in air. The high intensity inside a filament can dissociate the gas molecules into small fragments which emit characteristic fluorescence. This method is illustrated for simultaneously sensing atmospheric trace gases, methane and acetylene. The spectra of an “unknown” mixture were analyzed by using a genetic algorithm, showing good concentration agreement with the experimental results within an error of 25%.

Communication: Two stages of ultrafast hydrogen migration in methanol driven by intense laser fields

Hydrogen migration in methanol induced by an intense laser field (0.2 PW/cm(2)) is investigated in real time by a pump-probe coincidence momentum imaging method. The observed temporal evolution of the kinetic energy spectra reveals that there are two distinctively different stages in the hydrogen migration processes in the singly charged methanol: ultrafast hydrogen migration occurring within the intense laser field ( approximately 38 fs) and slower postlaser pulse hydrogen migration ( approximately 150 fs).

Tracing ultrafast hydrogen migration in allene in intense laser fields by triple-ion coincidence momentum imaging.

Ultrafast hydrogen migration in allene (CH(2)=C=CH(2)) in intense laser fields was investigated by triple-ion coincidence momentum imaging. The migrating proton covering the entire range of an allene molecule was visualized by the momentum correlation maps and by the geometrical structure of triply charged allene reconstructed from the observed momentum vectors of fragment ions. The extent of hydrogen migration was found to play a decisive role in breaking selectively one of the two initially equivalent C-C chemical bonds that become inequivalent in the course of the hydrogen migration.

Time-resolved laser-induced fluorescence lifetime measurements and relativistic Hartree–Fock calculations of transition probabilities in Sm II

Radiative lifetime measurements were performed with time-resolved laserinduced fluorescence techniques for 47 levels of the astrophysically important ion Sm 1+ over the energy range 21 000–36 000 cm −1 .T henew results have been compared with previous measurements but also with theoretical calculations taking configuration interactions and core-polarization effects into account, and as atisfying agreement has been found for many levels of this complex ion. New calculated transition probabilities are deduced from the experimental lifetimes and from the theoretical branching fractions for 162 transitions of astrophysical interest. These results will help astrophysicists in the quantitative investigation of the chemical composition of CP stars.

Sub-10-fs population inversion in N2+ in air lasing through multiple state coupling

Laser filamentation generated when intense laser pulses propagate in air has been an attractive phenomenon having a variety of potential applications such as detection and spectroscopy of gases at far distant places. It was discovered recently that the filamentation in air induces ‘lasing, showing that electronically excited N2+ is population-inverted, exhibiting marked contrast to the common understanding that molecular ions generated by intense laser fields are prepared mostly in their electronic ground states. Here, to clarify the mechanism of the population inversion, we adopt few-cycle laser pulses, and experimentally demonstrate that the lasing at 391u2009nm occurs instantaneously after N2+ is produced. Numerical simulations clarify that the population inversion is realized by the post-ionization couplings among the lowest three electronic states of N2+. Our results shed light on the controversy over the mechanism of the air lasing, and show that this post-ionization coupling can be a general mechanism of the atmospheric lasing.

Two-proton migration in 1,3-butadiene in intense laser fields

Ultrafast proton migration in 1,3-butadiene in an intense laser field (40 fs, 4.5 × 10(14) W cm(-2)) is investigated by using Coulomb explosion coincidence momentum imaging. The spatial distribution maps of a migrating proton reconstructed for the two three-body Coulomb explosion pathways, C(4)H(6)(3+)→ H(+) + CH(3)(+) + C(3)H(2)(+) and C(4)H(6)(3+)→ H(+) + C(2)H(+) + C(2)H(4)(+), reveal that two protons migrate within a 1,3-butadiene molecule, prior to the three body decomposition.

Direct observation of super-excited states in methane created by a femtosecond intense laser field

We report, for the first time, a direct observation of the super-excited states of CH4 in femtosecond intense laser fields using a pump (800 nm)–probe (1338 nm) technique. An unambiguous depletion of the CH (A 2 � → X 2 �) fluorescence signal as a function of the delay time is attributed to the de-excitation of the super-excited states by the probe laser pulse. The lifetime of the super-excited state is measured to be about 160 fs. (Some figures in this article are in colour only in the electronic version)