Photoelectron imaging of resonance-enhanced multiphoton ionization and above-threshold ionization of ammonia molecules in a strong 800-nm laser pulse

In this work, we mainly investigate the NH3 molecular multiphoton ionization process by using the photoelectron velocity map imaging technique. Under the condition of femtosecond laser(wavelength at 800 nm), the photoelectron images are detected. The channel switching and above-threshold ionization(ATI) effect are also confirmed. The kinetic energy spectrum(KES) and the photoelectron angular distributions(PADs) are obtained through the anti-Abel transformation from the original images, and then three ionization channels are confirmed successfully according to the Freeman resonance effect in a relatively low laser intensity region. In the excitation process, the intermediate resonance Rydberg states are C^1 A 1(6 + 2 photons process), B^1 E(6 + 2 photons process) and C^1 A 1(7 + 2 photons process), respectively. At the same time, we also find that the photoelectron angular distributions are independent of laser intensity. In addition, the electrons produced by different processes interfere with each other and they can produce a spider-like structure. We also find ac-Stark movement according to the Stark-shift-induced resonance effect when the laser intensity is relatively high.

Resonance-enhanced multiphoton ionization of NO via X^2II-A^2Σ transition

The resonance-enhanced multiphoton ionization (REMPI) spectrum of NO has been obtained in the range of 420 - 480 nm with a Nd:YAG pumped optical parametric generator and amplifier. The spectral lines can be attributed to NO X2II(v=0,1)-A2(v' = 0,1) transitions. In this wavelength range, NO molecules are ionized via the resonant intermediate state A2E+ and by a (2 + 2) REMPI process. The dependence of ion signals on laser intensity and gas pressure is discussed. The variation of the ionization signal versus laser intensity is near quartic. This is in good agreement with theory.

Wavelength-and ellipticity-dependent photoelectron spectra from multiphoton ionization of atoms

We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schr ¨odinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the(2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.

Resonance-enhanced two-photon ionization of hydrogen atom in intense laser field investigated by Bohmian-mechanics

Resonance enhanced two-photon ionization process of hydrogen atom via the resonant laser pulse is studied by Bohmian mechanics (BM) method. By analyzing the trajectories and energies of Bohmian particles (BPs), we find that under the action of high frequency and low intensity multi-circle resonant laser pulses, the ionized BPs first absorb one photon completing the excitation, and then absorb another photon, completing the ionization after staying in the first excited state for a period of time. The analysis of work done by the forces shows that the electric field force and quantum force play a major role in the whole ionization process. At the excitation moment and in the excitation-ionization process, the effect of the quantum force is greater than that of the electric field force. Finally, we discuss the principle of work and energy for BPs, and find that the electric field force and quantum force are non-conservative forces whose work is equal to the increment of mechanical energy of the system. In addition, it is proved that the quantum potential energy actually comes from the kinetic energy of the system and the increment of kinetic energy is equal to that of the kinetic energy of the system.

Multiphoton and tunneling ionization of atoms in an intense laser field

We study the ionization probabilities of atoms by a short laser pulse with three different theoretical methods, i.e., the numerical solution of the time-dependent SchrSdinger equation （TDSE）, the Perelomov-Popov Terent＇ev （PPT） theory, and the Ammosov-Delone-Krainov （ADK） theory. Our results show that laser intensity dependent ionization probabilities of several atoms （i.e., H, He, and Ne） obtained from the PPT theory accord quite well with the TDSE results both in the multiphoton and tunneling ionization regimes, while the ADK results fit well to the TDSE data only in the tunneling ionization regime. Our calculations also show that laser intensity dependent ionization probabilities of a H atom at three different laser wavelengths of 600 nm, 800 nm, and 1200 nm obtained from the PPT theory are also in good agreement with those from the TDSE, while the ADK theory fails to give the wavelength dependence of ionization probability. Only when the laser wavelength is long enough, will the results of ADK be close to those of TDSE.

Understanding Tunneling Ionization of Atoms in Laser Fields using the Principle of Multiphoton Absorption

The elaborate energy and momentum spectra of ionized electrons from atoms in laser fields suggest that the ionization dynamics described by tunneling theory should be modified. Although great efforts have been carried out within semiclassical models, there are few discussions describing the multiphoton absorption process within a quantum framework. Comparing the results obtained with the time-dependent Schr?dinger equation(TDSE)and the Keldysh–Faisal–Reiss(KFR) theory, we study the nonperturbative effects of ionization dynamics beyond the KFR theory. The difference in momentum spectra between multiphoton and tunneling regimes is understood in a unified picture with virtual multiphoton absorption processes. For the multiphoton regime, the momentum spectra can be obtained by coherent interference of each periodic contribution. However, the interference of multiphoton absorption peaks will result in a complex structure of virtual multiphoton bands in the tunneling regime. It is shown that the virtual spectra will be almost continuous in the tunneling regime instead of the discrete levels found in the multiphoton regime. Finally, with a model combining the TDSE and the KFR theory,we try to understand the different effects of virtual multiphoton processes on ionization dynamics.

Multiphoton resonant ionization of hydrogen atom exposed to two-colour laser pulses

This paper studies the multiphoton resonant ionization by two-colour laser pulses in the hydrogen atom by solving the time-dependent Schroedinger equation. By fixing the parameters of fundamental laser field and scanning the frequency of second laser field, it finds that the ionization probability shows several resonance peaks and is also much larger than the linear superposition of probabilities by applying two lasers separately. The enhancement of the ionization happens when the system is resonantly pumped to the excited states by absorbing two or more colour photons non-sequentially.

Multiphoton ionization of the hydrogen atom exposed to circularly or linearly polarized laser pulses

This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent SchrSdinger equation. It finds that the ratio of the ionization probabilities by linearly and circularly polarized laser pulses varies with the numbers of absorbing photons. With the same laser intensity, the circularly polarized laser pulse favors to ionize the atom with more ease than the linearly polarized laser pulse if only two or three photons are necessary to be absorbed. For the higher order multiphoton ionization, the linearly polarized laser pulse has the advantage over circularly polarized laser pulse to ionize the atom.

Two-colour coherent control of multiphoton ionization： a comparison between long-range and short-range potential model atoms

Using the numerical solution of the time-dependent SchrSdinger equation of a one-dimensional model atom in a two-colour laser field, we have investigated the effects of the potential models on coherent control of atomic multiphoton ionization. It is found that the photoelectron spectra are obviously different for the long-range （Coulomb-like） and short-range （with no excited bound states） potential model atoms, which are produced by two-colour coherent control of atomic multiphoton ionization in a few laser cycles. Our results indicate that two-colour coherent control of atomic multiphoton ionization can be observed in simulations, depending on the choice of the model potentials.

Laser Induced Photoelectron Impact Ionization In Multiphoton Ionization Process

Multiply charged ions of Ar and NO were observed in MPI experiment Of NO/Ar with TOF-MS. A delayable pulsed acceleration field wn applied tO investigate the effect of the photoelectrons on the formation of the multiply charged ions. The multiply charged ions were suggested to be produced by photoelectron impact ionization, in the region bentween the extractor grid and the repeller plate, step by step, from neutral species and lower charged ions. The 50-60ns of FWHM of the ion peaks implies that the pulse width of the photoelectrons should be shorter considering the broadening effect during the ionization process.

Development of Multiphoton Ionization Technique for Detection of Polycyclic Aromatic Hydrocarbon (PAH) in Solution

A simple low-cost system for detection of polycyclic aromatic hydrocarbon (PAH) in solution based on multiphoton ionization configuration is designed using a circulating ionization cell of 0.1 × 2 × 5 mm dimension with quartz optical window. Fourth harmonic emission of Nd:YAG laser (266 nm, 6 ns, 10 Hz, and 2 mJ) and second harmonic generation of distributed feedback dye laser (278 - 286 nm, 20 ps, 10 Hz, and 300 μJ) were used as the ionization source. A high voltage of 800 V was applied to separate the ions after ionization. The photocurrent includes a sharp peak and a broad tail indexed to electron and ion currents, respectively. The lowest concentration of anthraxcene (C14H10) in order of few nano-grams per milliliter was detected by this multiphoton ionization configuration.

Multiphoton Ionization of Potassium Atoms in Femtosecond Laser Fields

We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields.In the 800 nm laser field,the potassium atom absorbs three photons and emits one electron via one photon resonance with the 4p intermediate state with the help of the ac-Stark shift.The resonance feature is clearly shown as an Autler-Townes(AT) splitting and is mapped out in the electron kinetic energy spectrum.In a 400 nm laser field,although one photon resonance is possible with the 5p state,no splitting is observed.The different transition amplitudes between 4s-4p and 4s-5p explain the observed results.Due to the AT effect,an unexpected peak in the photoelectron energy spectrum that violates the dipole transition rule is observed.A preliminary explanation involving the spin-orbit interaction in the p state is given to account for this component.The observed ATsplitting in the electron kinetic energy distribution can be used as an effective method to calibrate the intensity of a laser field.

Time-dependent theoretical approach to the influence of laser fields on the resonance enhanced multi-photon ionization of SH radical

This paper reports that the （2＋1） resonance enhanced multi-photon ionization spectra of SH radical in external fields are simulated using the split-operator scheme of time-dependent wave-packet method. Two ionic states, i.e. a1△ and b1∑＋, are involved in the simulation. It gives the simulated photoelectron spectra, the population in each electronic state, as well as the projection of the wave-packet in each electronic state on different vibrational states. These results show that the so-called four-state model can represent the experimental results well.

Ionization Process of Atoms by Intense Femtosecond Chirped Laser Pulses

We numerically investigate the ionization mechanism in a real hydrogen atom under intense fem to second chirped laser pulses. The central carrier frequency of the pulses is chosen to be 6.2 eV (λ = 200 nm), which corresponds to the fourth-harmonic of the Ti:Sapphire laser. Our simulation of the laser-atom interaction consists on numerically solving the three-dimensional time-dependent Schrodinger equation with a spectral method. The unperturbed wave functions and electronic energies of the atomic system were found by using an L2 discretization technique based on the expansion of the wave functions on B-spline functions. The presented results of kinetic energy spectra of the emitted electrons show the sensitivity of the ionization process to the chirp parameter. Particular attention is paid to the important role of the excited bound states involved in the ionization paths.

Nonlinear Ionization of Molecules by Intense Transform-Limited Gaussian Laser Pulses

We present in this paper an investigation of the nonlinear process of above-threshold ionization. The process arises when an atomic or molecular system, exposed to an intense laser pulse, continues to absorb more photons than that needed for the ionization to occur. We trigger this nonlinear process in a simple molecular system by exposing it to an intense transform-limited Gaussian laser pulse of 267-nm wavelength which is the third harmonic of an 800-nm wavelength Tisapphire laser. We explore the characteristics of the process by analyzing the kinetic-energy spectra of the electrons ejected from the molecular system under different laser peak intensities.

短波自由电子激光在原子分子和团簇中的应用

短波自由电子激光产生的从极紫外(XUV)至硬X射线范围内连续可调的超强、超快和高相干性的脉冲辐射,为研究原子、分子和团簇中的超快电子和结构动力学过程开辟了新的途径。从原子的少光子单电离、少光子多电离和多光子多电离过程,到单脉冲的分子结构成像和时间分辨的分子动力学,再到团簇中的超快能量和质子转移过程,短波自由电子激光的应用非常广泛,并且取得了一系列重大的成果。通过一些科学案例,梳理了短波自由电子激光在原子、分子和团簇领域的研究进展。最后,总结了短波自由电子激光目前在该领域取得的成就,并展望了未来发展趋势。

Multiphoton quantum dynamics of many-electron atomic and molecular systems in intense laser fields

We present the recent new developments of time-dependent Schrödinger equation and time-dependent density-functional theory for accurate and efficient treatment of the electronic structure and time-dependent quantum dynamics of many-electron atomic and molecular systems in intense laser fields.We extend time-dependent generalized pseudospectral(TDGPS)numerical method developed for time-dependent wave equations in multielectron systems.The TDGPS method allows us to obtain highly accurate time-dependent wave functions with the use of only a modest number of spatial grid point for complex quantum dynamical calculations.The usefulness of these procedures is illustrated by a few case studies of atomic and molecular processes of current interests in intense laser fields,including multiphoton ionization,above-threshold ionization,high-order harmonic generation,attosecond pulse generation,and quantum dynamical processes related to multielectron effects.We conclude this paper with some open questions and perspectives of multiphoton quantum dynamics of many-electron atomic and molecular systems in intense laser fields.

铥原子激发态光电离截面的实验研究

本文采用激光烧蚀技术和超声分子束技术相结合,制备了高密度、低能态的自由铥(Tm)原子束。由可调谐激光制备原子电子激发态同时实现从激发态的光电离,由飞行时间质谱来探测来自不同电子激发态的光电离信号在245-266.3nm范围扫描激光波长,获得Tm原子UV区共振增强多光子电离光谱(REMPI光谱)。对于确定的激光共振波长,实验测定了不同激光能量下的光电离信号强度,进而得到Tm原子相应电子激发态的绝对光电离截面,测得的绝对光电离截面值在6.01±0.31~15.65±0.7Mb范围内。

窄脉冲分子束系统的发展与表征

本文结合高速分子斩波器与温度可调的脉冲阀,搭建了一套制备脉冲宽度窄且速度连续可调的分子束装置.通过共振增强多光子电离方法对分子束的脉冲宽度与速度进行了表征.测量表明斩波器可将氢气分子束在脉冲阀下游约193 mm处的脉冲宽度从20.0μs缩短到6.3 us.为了精确测量氢气分子的速度,实验采用了受激拉曼泵浦和共振增强多光子电离结合的泵浦-探测方法,利用纳秒级的受激拉曼泵浦脉冲激光作为测量时间零点,在标记分子飞行固定距离(193 mm)后精确测量分子到达时间以获得分子束速度同时通过改变脉冲阀的温度,实现氢气分子束速度在1290~3550 m/s之间的连续调节.本文搭建的系统在化学反应动力学领域有多种潜在应用,包括与离子阱以及分子束表面散射装置结合进行实验研究.