The dissociation pathways of N2+ in intense femtosecond laser fields

Using a neutral N2 beam as target,this paper studies the dissociation of N2+ in intense femtosecond laser fields(45 fs,～1×10 16 W/cm 2) at the laser wavelength of 800 nm based on the time-of-flight mass spectra of N + fragment ions.The angular distributions of N+ and the laser power dependence of N + yielded from different dissociation pathways show that the dissociation mechanisms mainly proceed through the couplings between the metastable states(A,B and C) and the upper excited states of N2+.A coupling model of light-dressed potential energy curves of N+2 is used to interpret the kinetic energy release of N+.     

Spin polarization effect of Ni2 molecule

The density functional theory （DFT） method （b3p86） of Gaussian 03 is used to optimize the structure of the Ni2 molecule. The result shows that the ground state for the Ni2 molecule is a 5-multiple state, symbolizing a spin polarization effect existing in the Ni2 molecule, a transition metal molecule, but no spin pollution is found because the wavefunction of the ground state does not mingle with wavefunctions of higher-energy states. So the ground state for Ni2 molecule, which is a 5-multiple state, is indicative of spin polarization effect of the Ni2 molecule, that is, there exist 4 parallel spin electrons in Ni2 molecule. The number of non-conjugated electrons is greatest. These electrons occupy different spatial orbitals so that the energy of the Ni2 molecule is minimized. It can be concluded that the effect of parallel spin in the Ni2 molecule is larger than that of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell-Sorbie potential functions with the parameters of the ground state and other states of the Ni2 molecule are derived. The dissociation energy De for the ground state of the Ni2 molecule is 1.835 eV, equilibrium bond length Re is 0.2243 nm, vibration frequency we is 262.35 cm^-1. Its force constants f2, f3 and f4 are 1.1901 aJ.nm^-2, -5.8723 aJ.nm^-3, and 21.2505 aJ.nm^-4 respectively. The other spectroscopic data for the ground state of the Ni2 molecule ωeχe, Be and αe are 1.6315cm 2, 0.1141 cm^-1, and 8.0145× 10^-4 cm^-1 respectively.     

Spin polarization effect for Tc2 molecule

Density functional method (DFT) (B3p86) of Gaussian98 has been used to optimize the structure of the Tc_2 molecule. The result shows that the ground state for Tc_2 molecule is an 11-multiple state and its electronic configuration is {}^{11}Σ_g^-, which shows the spin polarization effect of Tc_2 molecule of a transition metal element for the first time. Meanwhile, we have not found any spin pollution because the wavefunction of the ground state does not mingle with wavefunctions of higher energy states. So, that the ground state for Tc_2 molecule is an 11-multiple state is indicative of the spin polarization effect of Tc_2 molecule of a transition metal element: that is, there exist 10 parallel spin electrons. The non-conjugated electron is greatest in number. These electrons occupy different spacious tracks, so that the energy of Tc_2 molecule is minimized. It can be concluded that the effect of parallel spin of the Tc_2 molecule is larger than the effect of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell--Sorbie potential functions with the parameters for the ground state {}^{11}Σ_g^- and other states of Tc_2 molecule are derived. Dissociation energy D_e for the ground state of T_{c2} molecule is 2.266eV, equilibrium bond length R_e is 0.2841nm, vibration frequency ω_e is 178.52cm^{-1}. Its force constants f_2, f_3, and f_4 are 0.9200aJ·nm^{-2}, --3.5700aJ·nm^{-3}, 11.2748aJ·nm^{-4} respectively. The other spectroscopic data for the ground state of Tc_2 molecule ω_eχ_e, B_e, α_e are 0.5523cm^{-1}, 0.0426cm^{-1}, 1.6331×10^{-4}cm^{-1} respectively.     

Spin polarization effect for Os2 molecule

Density functional Theory （DFT） （B3p86） of Gaussian03 has been used to optimize the structure of Os2 molecule. The result shows that the ground state for Os2 molecule is 9-multiple state and its electronic configuration is ^9∑^＋g, which shows spin polarization effect of Os2 molecule of transition metal elements for the first time. Meanwhile, we have not found any spin pollution because the wavefunction of the ground state does not mingle with wavefunctions with higher energy states. So, the fact that the ground state for Os2 molecule is a 9-multiple state is indicative of spin polarization effect of Os2 molecule of transition metal elements. That is, there exist 8 parallel spin electrons. The non-conjugated electron is greatest in number. These electrons occupy different spacious tracks, so that the energy of Os2 molecule is minimized. It can be concluded that the effect of parallel spin of Os2 molecule is larger than the effect of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell-Sorbie potential functions with the parameters for the ground state ^9∑^＋g and other states of Os2 molecule are derived. Dissociation energy De for the ground state of Os2 molecule is 3.3971eV, equilibrium bond length Re is 0.2403nm, vibration frequency ωe is 235.32cm^-1. Its force constants f2, f3, and f4 are 3.1032×10^2aJ·nm^-2, -14.3425×10^3aJ·nm^-3 and 50.5792×10^4aJ·nm^-4 respectively. The other spectroscopic data for the ground state of Os2 molecule ωexe, Be and ae are 0.4277cm^- 1, 0.0307cm^- 1 and 0.6491 × 10^-4cm^-1 respectively.     

Spin polarization effect for Mn2 molecule

The density functional theory method （DFT） （b3p86） of Gaussian 03 has been used to optimize the structure of the Mn2 molecule. The result shows that the ground state of the Mn2 molecule is an 11-multiple state, indicating a spin polarization effect in the Mn2 molecule, a transition metal element molecule. Meanwhile, we have not found any spin pollution because the wavefunction of the ground state does not mingle with wavefunctions of higher-energy states. So the ground state for Mn2 molecule being of an 11-multiple state is the indicative of spin polarization effect of the Mn2 molecule among those in the transition metal elements： that is, there are 10 parallel spin electrons in a Mn2 molecule. The number of non-conjugated electrons is the greatest. These electrons occupy different spacious orbitals so that the energy of the Mn2 molecule is minimized. It can be concluded that the effect of parallel spin in the Mn2 molecule is larger than the effect of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell-Sorbie potential functions with the parameters for the ground state and other states of the Mn2 molecule are derived. The dissociation energy De for the ground state of the Mn2 molecule is 1.4477 eV, equilibrium bond length Re is 0.2506 nm, vibration frequency ωe is 211.51 cm^-1. Its force constants f2, f3, and f4 are 0.7240 aJ·nm-2, -3.35574 aJ·nm^-3, 11.4813 aJ·nm^-4 respectively. The other spectroscopic data for the ground state of the Mn2 molecule ωeχe, Be, αe are 1.5301 cm^-1, 0.0978 cm^-1, 7.7825×10^-4 cm^-1 respectively.     

Spin polarization effect for Fe2 molecule

This paper uses the density functional theory （DFT）（B3p86） of Gaussian03 to optimize the structure of Fe2 molecule. The result shows that the ground state for Fe2 molecule is a 9-multiple state, which shows spin polarization effect of Fe2 molecule of transition metal elements for the first time. Meanwhile, we have not found any spin pollution because the wavefunction of the ground state does not mingle with wavefunctions with higher energy states. So, that the ground state for Fe2 molecule is a 9-multiple state is indicative of the spin polarization effect of Fe2 molecule of transition metal elements. That is, there exist 8 parallel spin electrons. The non-conjugated electron is greatest in number. These electrons occupy different spacious tracks, so that the energy of the Fe2 molecule is minimized. It can be concluded that the effect of parallel spin of the Fe2 molecule is laFger than the effect of the conjugated molecule, which is obviously related to the effect of electron d delocalization. In addition, the Murrell Sorbie potential functions with the parameters for the ground state and other states of Fe2 molecule are derived. Dissociation energy De for the ground state of Fe2 molecule is 2.8586ev, equilibrium bond length Re is 0.2124nm, vibration frequency we is 336.38 cm^-1. Its force constants f2, f3, and f4 are 1.8615aJ.nm^-2, -8.6704aJ.nm^-3, 29.1676aj.nm^-4 respectively. The other spectroscopic data for the ground state of Fe2 molecule weXe, Be, αe are 1.5461 cm^-1, 0.1339cm^-1, 7.3428× 10^-4 cm^-1 respectively.     

Far-infrared hydrazine laser pumped by an N2O laser

We have used an N₂O laser to optically pump N₂H₄ molecules in a far-infrared cavity and observed 17 new laser lines in the wavelength range 93.0 to 374.2 μm, the 136.8 μm line pumped by 10P(16) being a doublet. We measured the frequencies of the laser lines by heterodyne mixing of the far-infrared radiation with radiation from two frequency-stabilized CO₂ lasers.     

等离激元钼掺杂二氧化钛半导体的光催化固氮反应机理研究

近年来光催化固氮引起了广泛的关注,其代表了将N₂有效转化为NH₃的“绿色工业”的可持续发展路线,如何有效合理地设计这方面的光催化剂仍然是本领域地一个挑战. 本文提出了一种策略,即在高浓度掺杂的TiOsub>2中利用等离激元热电子来激活惰性Nsub>2分子. 成功合成的Mo掺杂TiOsub>2催化剂在常温常压条件下显示出高达134 μmol·g^-1·h^-1的NH₃催化效率,这与传统的等离激元贵金属所实现的催化效率相当. 通过超快光谱技术,发现该体系中的等离激元热电子激活了N₂分子,从而提高了TiO₂的催化活性. 本文为基于等离激元半导体的光催化固氮反应开辟了一条新的途径.     

Far infrared laser frequencies of CH3OD and N2H4

The frequencies of 26 laser lines with wavelengths between 57 and 534 m have been measured in the optically pumped laser gases CH₃OD and N₂H₄. A pair of stabilized cw 12_{CO 2} lasers was used as a frequency standard for the heterodyne frequency measurements. Seven of the 26 lines are new.     

The improvement of Al2O3/AlGaN/GaN MISHEMT performance by N2 plasma pretreatment

This paper discusses the effect of N 2 plasma treatment before dielectric deposition on the electrical performance of a Al2O3 /AlGaN/GaN metal-insulator-semiconductor high electron mobility transistor(MISHEMT),with Al2O3 deposited by atomic layer deposition.The results indicated that the gate leakage was decreased two orders of magnitude after the Al2O3 /AlGaN interface was pretreated by N 2 plasma.Furthermore,effects of N 2 plasma pretreatment on the electrical properties of the AlGaN/Al2O3 interface were investigated by x-ray photoelectron spectroscopy measurements and the interface quality between Al2O3 and AlGaN film was improved.     

Interference of dissociating wave packets in the I2 molecule driven by femtosecond laser pulses

The interference between two dissociating wave packets of the I2 molecule driven by femtosecond laser pulses is theoretically studied by using the time-dependent quantum wave packet method.Both the internuclear distanceand velocity-dependent density functions are calculated and discussed.It is demonstrated that the interference pattern is determined by the phase difference and the delay time between two pump pulses.With two identical pulses with a delay time of 305 fs and a FWHM of 20 fs,more interference fringes can be observed,while with two pump pulses with a delay time of 80 fs and a FWHM of 20 fs,only a few interference fringes can be observed.     

N2价轨道的精细电子动量谱学研究

在高分辨率（ΔE=08?eV,Δp≈01a.u.）高效率的第三代电子动量谱仪上获得了N₂价轨道的电离能谱和动量谱.通过对伴线结构的电子动量谱学（EMS）研究,得到了不同伴线结构的电子动量谱,另一方面也得到了伴线结构的强度.由伴线的电子动量分布形状判断出其跃迁的主要来源,并由实验测量的伴线结构强度确定了谱因子（极强度）的大小,通过对谱因子实验值与理论计算结果的比较检验了各种理论模型的精确度. 关键词： 氮分子 价轨道 电子动量谱 电子关联效应     

Optically pumped submillimeter laser lines from CD2Cl2 using a large tunability CW CO2 laser

Twenty-five new laser lines have been obtained in the wavelength region from 155 to 830 μm by optically pumping the CD₂Cl₂ (deuterated dichloromethane) molecule with a CW CO₂ laser having a tunability range of 300 MHz. The wavelength, polarization relative to that of CO₂ pumping radiation, and offset relative to the CO₂ center frequency were determined for all of the new lines and some other already known laser emissions. For all of them we give also the relative intensity and the optimum pressure of operation. Permanent address: Depto de Física e Química da FEIS — UNESP 15.378-000 Ilha Solteira-SP, Brazil     

CS2团簇增强的激光多价电离现象的质谱研究

利用脉宽为25ns的脉冲Nd: YAG 532 nm的激光，在8×10¹⁰W/cm²的强度下，用飞行时间质谱对CS₂的激光电离过程进行了研究.观察到了较强的C²⁺和S²⁺高价离子信号，这些高价离子C²⁺，S²⁺的最可几平动能高达144 eV，112 eV.不同进样方式，激光延迟以及束源压力的实验结果表明，这些高价离子可能来源于CS₂团簇的库仑爆炸过程.多光子电离引发，逆韧致吸收加热-电子碰撞电离模型可能是高价离子产生的机理. 关键词： 2')" href="#">CS₂ 团簇 高价离子 激光电离     

CO2 laser assisted removal of UO2 and ThO2 particulates from metal surface

Pulsed laser assisted removal of uranium dioxide and thorium dioxide particulates from stainless steel surface have been studied using a TEA CO₂ laser. Decontamination efficiency is measured as a function of laser fluence and number of pulses. Threshold fluence for the removal of UO₂ particulates has been found to be lower than that required for the removal ThO₂ particulates. Usage of a ZnSe substrate, that is transparent to the laser wavelength used here, enabled us to decouple the cleaning effect arising out of absorption in the particulates from that in the substrate and has contributed towards understanding the mechanism responsible for cleaning. The experimental observations are also corroborated by simple theoretical calculations.     

Optical pumping by CO2 and N2O lasers: New cw FIR emissions in vinyl cyanide

A systematical study of optical pumping by CO₂ and N₂O lasers using a FIR metallic waveguide has been undertaken in vinyl cyanide. 97 new FIR laser lines are reported in the wavelength range 400 m–1,5 mm.Unité associée au CNRS (UA 836).     

Optically pumped submillimeter laser lines from CH2F2 and CD2Cl2 using a12C18O2 CW laser

Thirty-nine new submillimetre laser lines in CH₂F₂ and twelve in CD₂Cl₂ have been obtained in a Fabry-Perot FIR resonator by optically pumping with a CW¹²C¹⁸O₂ laser. The wavelength range obtained for CH₂F₂ is 126m to 1091m and for CD₂Cl₂ 212m to 774m. The wavelength measurements are accurate to within 5.10^–3. The relative polarisations of the pump laser and the FIR laser output were also determined. Tentative assignments of the IR and FIR transitions were made using existing microwave data.     

合成氨钌催化剂的晶体和形貌敏感性

哈伯-博施法合成氨反应是高温高压的耗能过程,因此降低该过程的能量消耗及开发温和条件下合成氨反应催化剂具有重要意义. 金属钌是合成氨反应中最有前途的催化剂之一,一直备受广泛关注. 确定金属钌催化剂的结构敏感性并提高其比质量活性是多相催化中亟待解决的重要问题. 氮气(N₂)活化是合成氨反应中的关键步骤. 本文通过第一性原理理论计算和微观动力学模拟方法系统研究了具有六方密排和面心立方晶体结构的钌催化剂上N₂活化过程和N₂解离反应速率. 理论计算研究表明,在六方密排Ru形貌中,{2130}晶面具有最高的N₂解离活性,其次是{0001}台阶面,它们比六方密排Ru其他表面上N₂解离反应速率高3个数量级以上;在面心立方Ru形貌中,{211}和{311}表面上N₂解离活性最高. 这些结果都表明台阶面/台阶位对氮气活化至关重要. 虽然六方密排Ru {2130}晶面具有最低的N₂解离能垒,然而由于面心立方Ru上可以暴露更高密度的活性位点,使得面心立方Ru比六方密排Ru具有更高的N₂转化速率. 本研究深入理解了N₂解离过程中,金属Ru 催化剂形貌和晶相结构敏感性,这为设计和优化高活性的合成氨Ru催化剂提供了理论基础.     

New experimental measurements and theoretical analysis of the collision-induced absorption in N2-H2 pairs

We present new experimental data on the collision-induced fundamental absorption in N₂-H₂ mixtures at room temperature and at low enough pressures so that the binary contribution is dominant. Previous measurements have been made at pressures where the ternary and possibly higher absorption coefficients are significant, and this makes it difficult to obtain accurate values for the binary absorption enhancement coefficient. To obtain the enhancement spectrum from the measurements of the mixture, it is necessary to subtract out both the spectra of pure H₂ and N₂, along with some CO₂ impurities thus increasing the experimental uncertainty. Nevertheless, we obtain a value for the integrated intensity of 1.15×10⁻⁴ cm⁻² amagat⁻² that is in good agreement with the previous value of 1.38×10⁻⁴. We also discuss how one can scale this result to high temperatures for application to brown dwarf or methane dwarf atmospheres.     

New NH2H4 far-infrared laser lines and their frequencies

We report 25 new far-infrared laser lines and 26 heterodyne frequency measurements in hydrazine. The frequencies range from 1.0 to 5.5 THz with most of the frequencies between 2.5 and 4.0 THz. The lines were generated in a high frequency, far-infrared Fabry-Perot laser cavity pumped by a CO₂ laser. The cavity has a high Q for wavelengths below 150 µm and uses variable coupling to optimize the power for each line.This work has been financed by the Brazilian Government - Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq), and by the United States Government - NASA grant W-18, 623.Contribution of NIST, not subject to U.S. copyright.