Photoelectron spectroscopy of ammonia via a fast predissociative state

We report a study on resonance enhanced multiphoton ionization photoelectron spectroscopy (REMPI-PES) involving the fast predissociative (A) over tilde state of ammonia, using nano- and femtosecond lasers. The multiphoton scheme involves (1 + 1), (2 + 2), (2 + 2) + 1 and (2 + 2) + 2 photon processes. We have found a progression of stretching vibrations nu(1) in the PE spectrum when pumping NH3 (A) over tilde upsilon(2) = 0, 1 and 3 as intermediate states. The stretching vibration intensity distributions in the photoelectron spectrum are calculated by using the Chebychev method of the wavepacket propagation. The femtosecond spectrum shows a similar feature to the nanosecond spectrum. However, high laser power also causes band broadening and shifting effect as well as above threshold multiphoton ionization.

Covariance analysis of the Coulomb explosion of ammonia induced by intense nanosecond laser at 532 nm

The Coulomb explosion of ammonia clusters induced by nanosecond laser at 532 not with an intensity of similar to 10(12) Wcm(-2) has been studied by time of flight mass spectrometry. The dominant multiply charged ions are N3+ and N2+ with kinetic energies of 110 and 50 eV respectively. The electrons generated from the multiphoton ionization are heated through inverse bremsstrahlung by the laser field when colliding with neutral or ionic particles. When their energies surpass the corresponding ionization potentials of the molecules or ions, the subsequent electron impact ionization may take place thus resulting in multi-charged nitrogen ions. Covariance analysis is made to study the possible pathways of the Coulomb explosion.

Autler-townes splitting in the multiphoton resonance ionization spectrum of molecules produced by ultrashort laser pulses

We report for the first time the proper conditions to observe Autler-Townes splitting (ac-Stark splitting) from vibrationally coherent states belonging to the different electronic terms of a diatomic molecule. Wave packet dynamics simulations demonstrate that such a process is feasible by multiphoton resonance ionization of the molecule Na-2 with a single ultrashort intense laser pulse. With the ultrahigh time resolution of a femtosecond laser pulse, one can directly measure the absolute value of the transition dipole moment between any kinds of molecular states by this kind of Autler-Townes splitting, which is a function of the internuclear distance R.

Angular distributions of multiphoton detachment of H- in various infrared laser fields

Using a nonperturbative quantum scattering theory, the photoelectron angular distributions (PADs) from the multiphoton detachment of H- ions in strong, linearly polarized infrared laser fields are obtained to interpret recent experimental observations. In our theoretical treatment, the PADs in n-photon detachment are determined by the nth-order generalized phased Bessel (GPB) functions X-n(Z(f),eta). The advantage of using the GPB scenario to calculate PADs is its simplicity: a single special function (GPB) without any mixing coefficient can express PADs observed by recent experiments. Thus, the GPB scenario can be called a parameterless scenario.

High-order harmonic generation and multi-photon ionization of Na-2 in laser fields

In this paper high-order harmonic generation (HHG) spectra and the ionization probabilities of various charge states of small cluster Na-2 in the multiphoton regimes are calculated by using time-dependent local density approximation (TDLDA) for one-colour (1064 nm) and two-colour (1064 nm and 532 nm) ultrashort (25 fs) laser pulses. HHG spectra of Na2 have not the large extent of plateaus due to pronounced collective effects of electron dynamics. In addition, the two-colour laser field can result in the breaking of the symmetry and generation of the even order harmonic such as the second order harmonic. The results of ionization probabilities show that a two-colour laser field can increase the ionization probability of higher charge state.

Identification of high-lying odd energy levels of uranium by resonant ionization mass spectrometry

Single-colour and two-colour multiphoton resonant ionization spectra of uranium atom were studied extensively with a Nd: YAG laser-pumped dye laser atomic beam apparatus time-of-flight mass spectrometer in our laboratory. The energy locations of high-lying odd-parity levels in the region 33 003-34 264 cm(-1),mearured by a two-colour three-step ionization technique, were reported here. The angular momentum quantum number J was uniquely assigned for these levels by using angular momentum selection rules.

Statistical-theory of multiphoton excitation of polyatomic-molecules based on the wigner function

This paper is aimed at establishing a statistical theory of rotational and vibrational excitation of polyatomic molecules by an intense IR laser. Starting from the Wigner function of quantum statistical mechanics, we treat the rotational motion in the classical approximation; the vibrational modes are classified into active ones which are coupled directly with the laser and the background modes which are not coupled with the laser. The reduced Wigner function, i.e., the Wigner function integrated over all background coordinates should satisfy an integro-differential equation. We introduce the idea of ``viscous damping'' to handle the interaction between the active modes and the background. The damping coefficient can be calculated with the aid of the well-known Schwartz–Slawsky–Herzfeld theory. The resulting equation is solved by the method of moment equations. There is only one adjustable parameter in our scheme; it is introduced due to the lack of precise knowledge about the molecular potential. The theory developed in this paper explains satisfactorily the recent absorption experiments of SF6 irradiated by a short pulse CO2 laser, which are in sharp contradiction with the prevailing quasi-continuum theory. We also refined the density of energy levels which is responsible for the muliphoton excitation of polyatomic molecules.

A shock tube method in the kinetic study of nonequilibrium ionization-recombination by rarefaction wave cooling

A shock tube method is introduced to study the ionization–recombination kinetics of high temperature gas, in which a test gas is heated and ionized by a reflected shock wave and subsequently quenched by a strong rarefaction wave reflected on the end wall of the driver section as the main cooling wave associated with a rarefaction wave incident back into region 5 when the reflected shock wave interacts with the contact surface. As the quenching rate of the strong rarefaction wave reaches 106 K/s, a nonequilibrium ionization-recombination process occurs, during which the ion recombination with electrons dominates.

Ionization suppression of diatomic molecules in strong laser fields

The ionization rate of molecules in intense laser fields may be much lower than that of atoms with similar binding energy. This phenomenon is termed the ionization suppression of molecules and is caused by the molecular inner structure. In this paper, we perform a comprehensive study of the ionization suppression of homonuclear diatomic molecules in intense laser fields of linear and circular polarizations. We find that for linear polarization the total ionization rate and the ionization suppression depend greatly on the molecular alignment, and that for circular polarization the ionization suppression of molecules in the antibonding (bonding) shells disappears (appears) for laser intensities around 10(15) W/cm(2). We also find that the molecular photoelectron energy spectra are greatly changed by the interference effect, even though the total ionization rate of molecules remains almost the same as that of their companion atoms.

Reduced deep-tissue image degradation in three-dimensional multiphoton microscopy with concentric two-color two-photon fluorescence excitation

We theoretically demonstrate that enhanced penetration depth in three-dimensional multiphoton microscopy can be achieved using concentric two-color two-photon (C2C2P) fluorescence excitation in which the two excitation beams are separated in space before reaching their common focal spot. Monte Carlo simulation shows that, in comparison with the one-color two-photon excitation scheme, the C2C2P fluorescence microscopy provides a significantly greater penetration depth for imaging into a highly scattering medium. (C) 2008 Optical Society of America.

Quantum interference in laser-induced nonsequential double ionization in diatomic molecules: Role of alignment and orbital symmetry

We address the influence of the orbital symmetry and the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules, in the length and velocity gauges. We work within the strong-field approximation and assume that the second electron is dislodged by electron-impact ionization, and also consider the classical limit of this model. We show that the electron-momentum distributions exhibit interference maxima and minima due to electron emission at spatially separated centers. The interference patterns survive integration over the transverse momenta for a small range of alignment angles, and are sharpest for parallel-aligned molecules. Due to the contributions of the transverse-momentum components, these patterns become less defined as the alignment angle increases, until they disappear for perpendicular alignment. This behavior influences the shapes and the peaks of the electron-momentum distributions.

Coherent population accumulations of multiphoton transitions induced by an ultrashort pulse train in polar molecules

Coherent population accumulations of multiphoton transitions induced by an ultrashort pulse train in a two-level polar molecule are investigated theoretically by solving the density-matrix equations without invoking any of the standard approximations. It is shown due to the effects of permanent dipole moments, that the population accumulation of multiphoton transitions can be obtained in the polar molecule. Moreover, the population accumulations depend crucially on the relative phase between two sequential pulses, and the period in which the maximum population accumulation occurs is 2 pi/N in N-photon transitions.

Ionization induced scattering of femtosecond intense laser pulses in cluster plasmas

The 45 degrees scattering of a femtosecond (60 fs) intense laser pulse with a 20 nm FWHM (the full width at half maximum) spectrum centered at 790 nm has been studied experimentally while focused in argon clusters at intensity similar to 10(16) W/cm(2). Scattering spectra under different backing pressures and laser-plasma interaction lengths were obtained, which showed spectral blueshifting, beam refraction and complex modulation. These ionization-induced effects reveal the modulation of laser pulses propagating in plasmas and the existing obstacle in laser cluster interaction at high laser intensity and high electron density.

Interaction of oblique incident electromagnetic wave with relativistic ionization front

Interactions of oblique incident probe wave with oncoming ionization fronts have been investigated using moving boundary conditions. Field conversion coefficients of reflection, transmission and magnetic modes produced in the interactions are derived. Phase matching conditions at the front and frequency up-shifting formulas for the three modes are also presented.

Single attosecond pulse generation in He+ by controlling the instant ionization rate using attosecond pulse trains combined with an intense laser pulse

High-order harmonics and single attosecond pulse generation by using an infrared laser pulse combined with attosecond pulse trains (APT) interacting with He+ have been investigated. We show that the ionization for different instant time intervals can be controlled by altering the time delay between the APT and the infrared pulse. Consequently, APT can be used as a tool to control the efficiency of high-order harmonics emitted at different times. By choosing appropriate APT and time delay, the driving pulse width for single attosecond pulse generation can be extended up to six optical cycles. (c) 2007 Optical Society of America.