Effects of the carrier-envelope phase in the multiphoton ionization regime

We theoretically investigate the effects of the carrier-envelope phase of few-cycle laser pulses in the multiphoton ionization regime. For atoms with low ionization potential, total ionization yield barely exhibits phase dependence, as expected. However, population of some bound states clearly shows phase dependence. This implies that the measurement of the carrier-envelope phase would be possible through the photoemission between bound states without energy-and-angle-resolved photoelectron detection. The considered scheme could be particularly useful to measure the carrier-envelope phase for a light source without an amplifier, such as a laser oscillator, which cannot provide sufficient pulse energy to induce tunneling ionization.     

Mass spectrometric study of the mechanism of the ionization of nitrogen-containing organic compounds on the surface of a molybdenum microalloyed alloy

Experimental studies of the mechanism of surface ionization of amines on the surface of a microalloyed molybdenum alloy in the air at atmospheric pressure were performed. The products of surface ionization of triethanolamine, Dimedrol, and papaverine were studied using a high-resolution mass spectrometer. The physicochemical parameters of surface ionization of some organic nitrogen compounds were measured. It was shown experimentally that the ionization of organic compounds of this type on the surface of the heated molybdenum alloy in air at atmospheric pressure occurs by a mechanism involving Brønsted sites (Brønsted).     

Mass Spectrometry,Review of the Basics: Ionization

Abstract: Mass spectrometry (MS) has become an integral tool in life sciences. The first step in MS analysis is ion formation (ionization). Many ionization methods currently exist; electrospray ionization (ESI) and matrix-assisted laser desorption ionization (MALDI) are the most commonly used. ESI relies on the formation of charged droplets releasing ions from the surface (ion evaporation model) or via complete solvent evaporation (charge residual model). MALDI ionization, however, is facilitated via laser energy and the use of a matrix. Despite wide use, ESI cannot efficiently ionize nonpolar compounds. Atmospheric pressure chemical ionization (APCI) and atmospheric pressure photo ionization (APPI) are better suited for such tasks. APPI requires photon energy and a dopant, whereas APCI is similar to chemical ionization. In 2004, ambient MS was introduced in which ionization occurs at the sample in its native form. Desorption electrospray ionization (DESI) and direct analysis in real time (DART) are the most widely used methods. In this mini-review, we provide an overview of the main ionization methods and the mechanisms of ion formation. This article is educational and intended for students/researchers who are not very familiar with MS and would like to learn the basics; it is not for MS experts.     

Probing the mechanisms of ambient ionization by laser-induced fluorescence spectroscopy

The ionization mechanisms of several atmospheric pressure ion sources based on desorption and ionization of samples deposited on a surface were studied. Home-built desorption electrospray ionization (DESI), laserspray ionization (LSI), and atmospheric pressure matrix-assisted laser desorption/ionization (AP-MALDI) sources were characterized using low-molecular-weight compounds, in particular fluorescent dyes. Detection of the desorbed and ionized species was performed by laser-induced fluorescence and ion cyclotron resonance mass spectrometry. The dependences of the signal intensities on various experimental parameters were studied. The data obtained reveals common features, such as formation of solvated species and clusters in the ionization processes, in all of the techniques considered.     

Comparison of the laser desorption/ionization methods for detecting metal complexes

The results of comparative analysis of laser desorption/ionization, matrix-assisted laser desorption/ ionization, and new laser-induced electron transfer desorption/ionization methods, used to detect chlorophyll A; mercury complex with thiuram; platinum complex with mercaptoquinoline; and lutetium complex with phthalocyanine, modified by crown ether, are presented. The new method is found to have a better ionization efficiency for complex compounds than the conventional laser desorption/ionization methods.     

Comparative analysis of the strong-field ionization of a quantum system with the Coulomb and short-range potentials

The dynamics of a hydrogen atom and a 3D model quantum system with a short-range potential is investigated using the direct numerical integration of the nonstationary Schrödinger equation in a wide range of laser intensities and frequencies. The simulation data are compared with the predictions of variants of the Keldysh-type theories. It is demonstrated that, in the low-frequency (tunnel) limit, the ionization rates of the systems with the Coulomb and short-range potentials and the same values of the ionization potential significantly differ from each other whereas, in the high-frequency (single-photon) limit, we do not observe a substantial difference between the ionization rates. Specific features of the angular distribution of the photoelectron emission and the photoelectron energy spectra are investigated in detail. In addition, the ionization suppression is studied for both Coulomb- and short-range-potential atoms. The stabilization is due to the dramatic reconstruction of the atom in the presence of a strong laser field and the formation of a new system (Kramers-Henneberger atom) that exhibits an increasing resistance to the ionization upon an increase in the laser intensity. In the two-photon ionization regime, the stabilization phenomenon is substantially more pronounced for the system with the Coulomb potential. This results from the effective excitation of the Rydberg states of the dressed atom in the strong-field limit.     

Electron transfer in the reflection of atoms from metal surfaces

The resonance mechanism for positive and negative ionization of an atom reflected from a metal surface is treated in the time-dependent Hartree-Fock approximation assuming that the atom moves on its classical trajectory. A simple model is parameterized to describe 30–500 eV Na atoms reflected from tungsten, and the ionization probabilities are calculated by numerical integration of the equation of motion of the time evolution operator. Significant ionization can only occur if either the ionization level, or the affinity level of the atom crosses the Fermi level beyond the range of the atom-metal hopping interaction. On clean tungsten, the former situation applies, and the probability of positive ionization is nearly unity, and of negative ionization nearly zero.     

Numerical simulation of the ionization dynamics of a two-electron quantum system in a femtosecond pulse

The ionization of a simple two-electron model system, viz., the one-dimensional negative hydrogen ion, is investigated using direct numerical integration of the time-dependent Schrödinger equation. The one-and two-electron ionization probabilities as functions of frequency and radiation intensity are obtained. It is shown that two-electron ionization is mediated by both direct and sequential mechanisms. The stabilization of the two-electron system against the ionization process is investigated. The data obtained are compared with calculations performed within the one-dimensional single-particle model of H^?. The photoelectron spectrum is analyzed in the region of parameters corresponding to the single-electron ionization regime.     

Theoretical and experimental investigations on the threshold of a laser-induced breakdown of air

The threshold of a laser-induced breakdown of air is determined experimentally and theoretically. We find that the ionization of air has two steps: the first step is a multi-photon ionization process, which provides enough"seed electrons" to initiate the next step, and the second one is predominated by cascade ionization, which continues to produce free electrons geometrically until the critical free-electron density for breakdown is reached. So a two-step model based on the Morgan ionization model is established to describe the breakdown process. It is found that the time node dividing the two steps is about 9.8 ns in atmospheric air, and the threshold derived from the two-step model proposed here is more consistent with the experimental results than traditional ionization model.     

Effect of the multi-electron ionization on the impurity behaviour in tokamaks

The effect of multi-electron ionization processes on the distribution of ionic stages in tokamak discharges is studied using an impurity diffusion code. It is concluded that the effect will be negligibly small as multi-electron ionization rates for a given stage become significant only at temperatures when it has already been depleted by single-electron ionization processes.     

利用强场多光子电离技术实现对多原子分子离子振动量子态的光学操控

利用飞秒光电子影像技术研究了碘甲烷分子在飞秒强激光场作用下的多光子电离动力学,在实验上实现了运用飞秒强场多光子电离技术对多原子分子离子的振动量子态进行光学操控.提高了飞秒激光的强度,从1.6×1013W/cm2提高到2.5×1013W/cm2.在增大的激光强度范围内,发现了新的能量组分,并对此进行归属.通过采集光电离的光电子影像可以得到强场电离后光电子的动能分布和角度分布两方面的信息,前期的研究主要侧重于讨论光电子动能随光强的变化,重点讨论了光电子角度分布随光强的变化,通过观察光电子角度分布的变化趋势对振动量子态调控机理进一步认识.     

Calculation of cross sections of simultaneous ionization in ion-atom collisions by the generalized geometrical model

The geometrical model (GM) of ionization in ion—atom collisions [8, 9] was generalized to describe ionization of both colliding particles (simultaneous ionization) due to electron—electron interaction. The generalized GM (GGM) allows calculation of the cross sections for electron loss by an incident particle with simultaneous target ionization at collision velocities higher than characteristic electron velocities, accurate within a factor of two with respect to the Born or impulse approximation. An advantage of the GGM, except for its simplicity, is easy calculation of p(b) (p is the ionization probability and b is the impact parameter), which makes it possible to include the contribution of simultaneous ionization into more general approximate schemes for calculating cross sections of multielectron ionization of atoms or ions.     

Sequential over-barrier ionization of multi-electron atoms in the tens-to-hundreds keV/u energy range

Our previous work on the classical over-barrier ionization model for helium double ionization is extended to the complex multi-electron system of Ne.The total and q-fold ionization cross sections are calculated at energies ranging from a few tens to several hundred keV/u.The calculation results are in good agreement with the experimental data,and the energy dependence of the cross sections suggests that the multi-ionization of a strong perturbated complex atom is probably the sequential over-barrier ionization process.     

基于光场离化电流机制产生强太赫兹辐射的参数优化研究

基于超短激光脉冲与气体作用通过光场离化电流产生太赫兹(THz)辐射的模型, 研究了用双色激光脉冲的方法产生强THz辐射的优化参数条件. 数值计算表明, 导致THz辐射产生的离化电流主要是由一阶电离过程产生的, 高阶离化对该电流产生的贡献很小. 通过调节基频光与倍频光的配比、相位差都能增大离化电流, 从而可以提高THz辐射振幅. 将激光波长拓展到中红外波段, 也有利于提高离化电流. 此外,改变作用气体的种类也能改变离化电流. 在激光和密度参数相等的情况下, 在氦气中可以产生高于氮气中2倍左右的离化电流.     

Electron-impact ionization and dissociative ionization of sulfur in the gas phase

We describe the methods and the results of investigation of the yield of positive ions formed as a result of electron-impact ionization of sulfur. The ionization energy for the basic molecule and the energies corresponding to the emergence of fragment ions are obtained from the ionization efficiency curves. The dynamics of formation of molecular sulfur ions in the temperature range 320–700 K is investigated. The energy dependences of efficiency S _n of the ion formation for n = 1–6 are analyzed, and their appearance energies are determined. The total cross section of sulfur ionization by a monochromatic electron beam is also investigated. Using the linear approximation method, we marked out features on the ionization function curve, which correspond to the ionization and excitation energies for multiply charged ions. The total cross section of the formation of negative sulfur ions is measured in the energy range 0–9 eV.     

电离能下降对于硅等离子体辐射不透明度影响的研究

电离能下降的现象与等离子体的成分、电离分布、热力学、输运性质息息相关,其精确测量值对于整个实验的模型检验和方案设计都至关重要.本文考虑粒子数的涨落,对经典的Stewart和Pyatt的模型进行修正,并耦合进先前发展的等离子体模型.利用修正的模型对熊刚等人的实验进行了解释,发现当前模型所得结果要优于其他理论结果,与实验更加一致.     

Adiabatic approximation of the correlation function in the density-functional treatment of ionization processes

The ionization of a one-dimensional model helium atom in short laser pulses using time-dependent density-functional theory is investigated. We calculate ionization probabilities as a function of laser intensity by approximating the correlation function of the system adiabatically with an explicit dependence on the fractional number of bound electrons. For the correlation potential we take the derivative discontinuity at integer numbers of bound electrons explicitly into account. This approach reproduces ionization probabilities from the solution of the time-dependent Schr?dinger equation, in particular, the so-called knee due to nonsequential ionization.     

Influence of the photoionization process on the fragmentation of laser desorbed polycyclic aromatic hydrocarbons

Characterization of polycyclic aromatic hydrocarbons (PAHs) samples has been performed by laser desorption combined with multi-photon ionization technique using two different geometries of the ionization laser beam. This comparative study evidences the strong influence of ionization laser fluence on PAH fragmentation. Through a ∼10³ enlargement of the ionization probe volume and 10⁴ reduction of laser fluence over previous studies, fragment free mass spectra are obtained with higher sensitivity and selectivity. The ability to measure fragment free PAH mass spectra is a very important step in the end goal of measuring complex unknown mixtures of PAH desorbed from solid surface such as soot samples.     

On the interpretation of the photoelectron spectrum of CO chemisorbed on Ni

A LCAO-SCF calculation on the NiCO molecule is reported. In addition to the ionization potentials the vibrational structure due to ionization is calculated. The computed ionization potentials are compared with those of recent semiempirical calculations on the CO — Ni system and with the photoelectron spectra of CO chemisorbed on nickel surfaces. We produce further evidence that the first peak in the photoelectron spectrum relates to the 5σ and 1π orbitals of CO and that the peak at higher ionization energy represents the 4σ orbital.     

Electron impact ionization cross sections of the CO2 clusters

The modified Jain–Khare semi-empirical formalism for the evaluation of differential and integral electron impact ionization cross sections for molecules has been extended to the evaluation of cross sections for the electron ionization of CO₂ clusters: (CO₂)₂₄₀ and (CO₂)₁₇₀₀. The energy dependent differential cross sections are evaluated at the incident electron energies of 50, 100 and 200 eV. The integral total ionization cross sections have been calculated in the energy range varying from ionization thresholds to 1000 eV which revealed a good agreement with the available experimental and the theoretical data. The ionization rate coefficients have also been evaluated using the presently calculated ionization cross sections and Maxwell–Boltzmann energy distributions.