Photodissociation Efficiency Spectroscopy Study of the Rydberg Excited Ion-Pair States of Carbon Dioxide

Photodissociation efficiency spectrum of anionic oxygen atom produced via ion-pair dissociations of carbon dioxide is recorded by means of the synchrotron radiation excitation （XUV photon energy 17.40-20.00eV）. The present spectrum is assigned as the Rydberg-like excited ion-pair states, i.e., Tanaka-Ogawa and Henning series, -↑C^2∑g^＋ （CO2^＋） vibrational ground-state and excitation series. Three Rydberg series, npσu, npπu, and nfu, converging to -↑C^2∑g^＋ （0, 0, 0）, show the higher cross sections.     

Structural Deformation of CO22+ in Intense Femtosecond Laser Fields

The angular distributions of CO^＋ from the dissociation of CO2^2＋ and CO2^＋ in intense femtosecond laser fields （45 fs, about 5 × 10^15 W/cm^2） are studied at a laser wavelength of 800nm based on the time-of-flight mass spectra of CO^＋ fragment ions. The experimental results show that structural deformation occurs in the charge state of CO2^2＋ and the CO^＋ maintains linear geometrical structure.     

Electron Scattering by C4H10 and C6H6 in the Energy Range 100--1000eV

We investigate the applicability of the independent atom model （IAM） to elastic electron scattering from complex polyatomic molecules, namely C4H10 and C6H6, in the energy range 100-1000eV. The cross sections of the elastic electron scattering are calculated by employing the IAM together with the relativistic partial waves. The incorporation of both the modified absorption potential and the extended structural factor in the IAM makes the elastic differential cross sections and momentum transfer cross sections have a good agreement with the available experimental data. The present simple model seems to be insensitive to the complexity of the target molecules so that the proposed procedure can be quite useful for calculation of electron scattering from bio-molecules.     

Fast decay of high vibronic S1 states in gas-phase benzene

Lifetimes of different vibronic levels at high excess energies in the S₁ state of isolated benzene molecules are measured using for the first time a two-photon ionization pump–probe technique with UV femtosecond pulses. For the 6¹1³ state (3290 cm^-1 excess energy) at the onset of the ‘channel three’ a biexponential decay is found with a fast (τ_f=20 ps) and a slow (τ_s>500 ps) component. The values are in line with previous sub-Doppler high-resolution measurements of this band in our laboratory. We explain the measured faster decay (τ_f=900 fs, τ_s=100 ps) of the 7¹ state at a lower excess energy of 3077 cm^-1 by a simultaneous excitation of the adjacent 6¹ ₀1³ ₀16¹ ₁ hot band leading to a vibronic state of higher excess energy and faster decay. The vibronic levels 6¹1⁴ and 7¹1¹ at a higher excess energy of ≳4000 cm^-1 show a biexponential decay of τ_f=550 fs, τ_s=30 ps and τ_f≲300 fs, τ_s=20 ps, respectively. The experimental results point to dynamic processes within the vibronic level manifold of the S₁ state and a fast nonradiative electronic relaxation process. Received: 3 November 1999 / Published online: 5 July 2000     

Infrared-laser-pulse control of bond- and state-selective excitation, dissociation and space quantization: application to a three-dimensional model of HONO2 in the ground electronic state

Selective control over the vibrational excitation and space quantization of the dissociation fragments by optimally designed linearly polarized and shaped infrared (IR) laser pulses of the picosecond (ps) and subpicosecond duration is demonstrated by means of quantum-dynamical simulations within the Schr?dinger wave-function formalism for a three-dimensional (3-D) model of HONO₂ in the ground electronic state, wherein the OH and the ON single-bond stretches are explicitly treated, together with the bending angle between them, on the basis of the ab initio defined 3-D potential-energy surface and dipole function. The high-lying zeroth-order vibrational states of the OH bond are prepared selectively both below and above the dissociation threshold of the ON single bond, and demonstrate a quasi-periodic oscillatory behaviour, manifesting intramolecular vibrational energy redistribution (IVR) on the picosecond timescale. Selective breakage of the ON single bond in HONO₂ with more than 97% probability is demonstrated, along with control of the space quantization of the dissociation fragments: the OH fragments rotating clockwise, OH(c), and anticlockwise, OH(a), are prepared selectively, with the OH(a)/OH(c) branching ratio being as high as 10.975. The results obtained show that optimally designed strong and short IR-laser pulses can compete against IVR and manipulate vibrational excitation and dissociation of polyatomic molecules. Received: 3 November 1999 / Published online: 13 July 2000     

An Efficient Pulsed CH3OH Terahertz Laser Pumped by a TEA CO2 Laser

An efficient pulsed CH3OH terahertz （THz） laser pumped by a TEA CO2 laser is investigated experimentally. To improve photon conversion efficiency and THz laser energy, two cavity configurations of the TEA CO2 laser, which is external and semi-external, are evaluated. The pump intensities are about 4.7 MW/cm2 and 1.2 MW/cm2, respectively. Higher pump intensity and more stable single lines are obtained in the external cavity. For the 3.8 J pump energy of the 9P（16） transition in the external cavity, the maximum terahertz output energy with 570.5 μm wavelength at 160 Pa is 431 μJ. With a 6 J energy pulse in terms of a semi-external cavity, a 353 μJ terahertz emission （570.5 μm） is produced. The corresponding photon conversion efficiencies are 1.36% and 0.705%, increasing by a factor of about 2.     

A Theoretical Study of Super-Excited States of F2

In the framework of quantum defect theory, we study super-excited states of F2 molecules which can dissociate into F^＋ （^3P2,1,0） and F^-（^1 So） ion-pair. Based on our calculation, we present a vibrational resolved assignment of the high precision photofragment yield spectra for F^- from the F2 ion-pair production.     

Absence of Charge-Resonance-Enhanced Ionization in Attosecond Pulse Photoionization： Numerical Result on One-Dimensional H2^＋

We present a numerical result of photoionization rate for the one-dimensional molecular hydrogen ion model exposed to intense light of 1 × 10^16-2×10^16 W/cm^2, 55-as pulse duration, and 800nm wavelength. In contrast to the previous calculation result of charge-resonance-enhanced ionization for lower intensity and much longer pulse, our result exhibits an ionization saturation. The numerical results are interpreted in the field-dressed potential picture as over-the-barrier liberation of electrons. This extremely short pulsewidth and relatively high field phenomenon requests experimental demonstration.     

Double-Exponentially Decayed Photoionization in CREI Effect： Numerical Experiment on 3D H2^＋

On the platform of the 3D H2^＋ system, we perform a numerical simulation of its photoionization rate under excitation of weak to intense laser intensities with varying pulse durations and wavelengths. A novel method is proposed for calculating the photoionization rate： a double exponential decay of ionization probability is best suited for fitting this rate. Confirmation of the well-documented charge-resonance-enhanced ionization （CREI） effect at medium laser intensity and finding of ionization saturation at high light intensity corroborate the robustness of the suggested double-exponential decay process. Surveying the spatial and temporal variations of electron wavefunctions uncovers a mechanism for the double-exponentially decayed photoionization probability as onset of electron ionization along extra degree of freedom. Henceforth, the new method makes clear the origins of peak features in photoionization rate versus internuclear separation. It is believed that this multi-exponentially decayed ionization mechanism is applicable to systems with more degrees of motion.     

Theoretical Investigation of Femtosecond-Resolved Photoelectron Spectra of the Li2 Molecule

The time-dependent quantum wave packet method is used to investigate the dynamics for the Li2 molecule, and the time-resolved photoelectron spectra （TRPES） of the Li2 molecule are calculated. At the short delay time, the particular phenomenon of TRPES with four peaks is qualitatively interpreted in a dressed state picture by analyzing wave packet motion on light-induced potential （LIP）. The significant difference in the electronic structure of E1∑g^＋ between the inner and outer turning points has an impact on the TRPES. The control for the first excited state A1∑u^＋ of the initial wave packet is discussed.     

Theoretical Investigation of Femtosecond-Resolved Photoelectron Spectrum of Na2 Molecules

Effect of laser fields on Na2 interaction potentials is studied by calculating the time-resolved photoelectron spectrum （TRPES） with the time-dependent wave-packet method. It is shown that the photoelectron spectrum at different delay times reflects the population in different electronic states. We inspect the periodicity of vibrational motion in neutral states, and map the vibrational wave-packet propagation in corresponding internuclear coordinate.     

Excellent Passivation of p-Type Si Surface by Sol-Gel Al2O3 Films

Al2O3 films with a thickness of about lOOnm synthesized by spin coating and thermally treated are applied for field-induced surface passivation of p-type crystalline silicon. The level of surface passivation is determined by techniques based on photoconductance. An effective surface recombination velocity below lOOcm/s is obtained on 10Ωcm p-type c-Si wafers （Cz Si）. A high density of negative fixed charges in the order of 10^12 cm^-2 is detected in the Al2O3 films and its impact on the level of surface passivation is demonstrated experimentally. Furthermore, a comparison between the surface passivation achieved for thermal SiO2 and plasma enhanced chemical vapor deposition SiNx ：H films on the same c-Si is presented. The high negative fixed charge density explains the excellent passivation of p-type c-S/by Al2O3.     

大气CO2反演的地表反射率影响分析与比值反演方法

近红外波段空基大气CO₂反演是一个病态问题,地表特征的不确定性是其重要的影响因素之一。针对大气CO₂高精度反演的需求,研究了地表反射率两大不确定性因素对大气CO₂反演的影响程度,提出了比值光谱法对这种影响进行校正。比值光谱法中CO₂无吸收通道(off-line)的选择至关重要,通过比较和分析多种off-line通道的选择方法,发现多通道多点平均法因多数据平均可降低随机误差的优势,获得的off-line通道对应的反演精度最高,而且离散程度也小。比值光谱法结合多通道多点平均法选取出的off-line通道对地表反射率的不确定性影响有明显的校正效果,有利于大气CO₂反演精度的提高。     

Guiding of 60keV O6+ Ions through Nanocapillaries in an Uncoated Al2O3 Membrane

We measure the transmission of O^6＋ ions with a higher energy of 60 keV （in turn a higher value of Ep/q） through capillaries in an uncoated AI2 03 membrane, and obtain agreements with previously reported results in general angular distribution of the transmitted ions and the transmission profile width variation with capillary tilt angle. The transmission fractions as a function of the tilt angle can be fitted to the semi-empirical Gaussian-like function well. Due to using uncoated capillary membrane, our ψc is larger than that using gold-coated one, in spite of our larger value of Ep/q, which suggests a larger equilibrium charge Q∞ in our experiment.     

Autler-Townes Splitting in Photoelectron Spectrum of Three-Level Li2 Molecule in Ultrashort Pulse Laser Fields

The Autler-Townes （AT） splitting in femtosecond photoelectron spectrum of three-level Li2 molecules is theoretically investigated using time-dependent quantum wave packet method. With proper femtosecond laser pulses, three peaks of the AT splitting can be observed in the photoelectron spectrum. The AT splitting stems from rapid Rabi oscillation caused by intense ultrashort laser pluses. The effects of laser parameters on the molecular ionization dynamics are also discussed.     

A Kilowatt Radio-Frequency Excited Diffusively Cooled All-Metal Slab Waveguide CO2 Laser

A new type of rf excited diffusively cooled all-metal slab waveguide CO2 laser is presented, in which the waveguide channel is constructed by two copper side walls and two copper electrodes, and the discharge is confined in the slab waveguide channel in terms of the voltage division structure. From this type of structure, over 1 kW laser power is obtained with an efficieney of more than 13%.     

Generation of Intense THz Pulsed Lasers Pumped Strongly by CO2 Pulsed Lasers

A theoretical method dealing with two intense laser fields interacting with a three-level molecular system is proposed. A discussion is presented on the properties of the solutions for time-independent and time-dependent absorption coefficients and gain coefficient on resonance for strong laser fields, based on analytic evaluation of the rate equations for a homogeneously broadened, three-level molecular system. The pump intensity range can be estimated according to the analytic expression of pump saturation intensity. The effects of pulse width, gas pressure and path length on the energy absorbed from pump light are studied theoretically. The results can be applied to the analysis of pulsed, optically pumped terahertz lasers.     

Rotational and Vibrational State Distributions of CsH and Relative Reactivity in Reactions of Cs（6^2D,7^2D） with H2

By using a pump-probe technique, the nascent rotational and vibrational state distributions of CsH are obtained in the Cs（6^2 D,7^2 D） plus H2 reaction. The nascent CsH molecules are found to populate the lowest two vibrational （v″ = 0 and 1） levels of the ground electronic state. By comparing the spectral intensities of the CsH action spectra with those of pertinent Cs atomic fluorescence excitation spectra, the relative reactivity with 1-12 is in an order of6^2D3/2 〉 6^2D5/2 〉 7^2D3/2 〉 7^2D5/2. The rotational temperatures are found to be slightly below the cell temperature. The relative fractions （〈fV〉, 〈fR〉, 〈fT〉） of average energy disposal are derived as （0.2,0.12,0.68）, （0.2,0.12,0.68）, （0.07,0.04,0.89） and （0.07,0.04,0.89） for the 6^2D3/2, 6^2D5/2, 7^2D3/2 and 7^2D5/2, respectively. The major available energy is released as translation. These results support that the reaction mechanism of Cs（6^2 D,7^2 D） plus 112 is primarily a eollinear abstraction and not an insertion.     

高气压CO2激光器宽带输出频谱特性的理论研究

从理论上研究了高气压CO2激光器的宽带输出频谱特性.结果表明，在20个大气压下，CO2激光器有宽带输出，带宽高达5.0 cm－1（相当于150 GHz），从971 cm－1~976 cm－1，峰值在10R(16)线处，10R(14)线和10R(18)线差不多对称地分布其两侧.很小的增益差异（4.6%）造成了很大的能量输出差异（100多倍）.比较了谐振腔内有无色散元件时的输出频谱，理论证明了谐振腔内无任何色散元件时的宽带输出频谱是光滑连续的，而频率依赖的反馈引起了输出频谱很强的精细结构.理论计算结果与实验测量结果符合较好.     

Average Energy Loss Measured in Single and Double Electron Capture Collisions of He^2＋ on Ar at Low Velocities ＊

Employing the recoil ion momentum spectroscopy we investigate the collision between He^2＋ and argon atoms. By measuring the recoil longitudinal momentum the energy losses of projectile are deduced for capture reaction channels. It is found that in most cases for single- and double-electron capture, the inner electron in the target atom is removed, the recoil ion is in singly or multiply excited states （hollow ion is formed）, which indicates that electron correlation plays an important role in the process. The captured electrons prefer the ground states of the projectile. It is experimentally demonstrated that the average energy losses are directly related to charge transfer and electronic configuration