Observation of a molecular frame (e, 2e) cross section: an (e, 2e + M) triple coincidence study on H(2)

We report the first experimental results showing transition-specific anisotropy of molecular frame (e, 2e) cross sections. Vector correlations between the two outgoing electrons and the fragment ion have been measured for specific ionization-excitation processes of H2. The results enable us to obtain molecular frame (e, 2e) cross sections for transitions to the 2ssigma(g) and 2psigma(u) excited states of H(2)(+), thereby making stereodynamics of the electron-molecule collisions directly visible.     

Dissociation energies of molecular hydrogen and the hydrogen molecular ion

We have obtained improved values for the dissociation energies of molecular hydrogen and its ion by using a high-resolution pulse-amplified laser to probe the second dissociation limit. The onset of the vibrational continuum is observed by state-selective detection of the atomic products of dissociation, and several auxiliary measurements link the results to the ground state. The dissociation energies are accurate to 0.010-0.026 cm(-1), improving previous measurements by a factor of 3-7. Agreement with ab initio calculations is good for H2, D2, and their ions, but not for HD and HD+.     

Controlling HD+ and H+2 dissociation with the carrier-envelope phase difference of an intense ultrashort laser pulse

Carrier-envelope phase difference effects in the dissociation of the HD+ molecular ion in the field of an intense, linearly polarized, ultrashort laser pulse are studied in the framework of the time-dependent Schr?dinger equation. We consider a reduced-dimensionality model in which the nuclei are free to vibrate along the field polarization and the electrons move in two dimensions. The laser has a central wavelength of 790 nm and a pulse length of 10 fs with intensities in the range 6x10(14) to 9x10(14) W/cm(2). We find that the angular distribution of dissociation to p+D and H+d can be controlled by varying the phase difference, generating differences between the dissociation channels of more than a factor of 2. Moreover, the asymmetry is nearly as large for H+2 dissociation.     

The characteristics of O＋HD （v = 0, j = 0） reaction dynamics

The analytical potential energy function of HDO is constructed at first using the many-body expansion method.The reaction dynamics of O+HD(v = 0,j = 0) in five product channels are all studied by quasi-classical trajectory(QCT) method.The results show that the long-lived complex compound HDO is the dominant product at low collision energy.With increasing collision energy,O+HD → OH+D and O+HD → OD+H exchange reactions will occur with remarkable characteristics,such as near threshold energies,different reaction probabilities,and different reaction cross sections,implying the isotopic effect between H and D.With further increasing collision energy(e.g.,up to 502.08 kJ/mol),O+HD → O+H+D will occur and induce the complete dissociation into single O,H,and D atoms.     

HOD分子在?1B1态的光解动力学： 产物OH/OD的分支比以及OD键解离能

利用H(D)原子里德堡态时间飞渡谱技术研究了HOD超声射流分子束在124 nm附近的?态光解动力学．实验测量了HOD分子在?态的转动分辨的吸收谱,并得到了五个转动峰下H+OD以及D+OH通道的产物总的平动能谱．通过对产物平动能谱的分析,得到了?态解离产物OH和OD的分支比,并与Β态和?态相应解离产物的分支比做了对比．实验结果确定了HOD分子OD键的解离能为41751.3±5 cm^-1.     

Discussion on the dissociation of fast HD^＋2 ions traversing thin foils

the discussion is on the following experimental results:The energy distribution of the H^ and D^ fragments resulting from the dissociation of HD^ 2 molecular ions at energy 1.4977 MeV has been measured using the Coulomb explosion techoique,The spectra were used to determing the binding energy of HD^ 2 and its structure,There existed differenoes between the spectral structures for proton and for deuteron.     

Discussion on the dissociation of fast HD+2 ions traversing thin foils

the discussion is on the following experimental results: The energy distribution of the H+ and D+ fragments resulting from the dissociation of HD+2 molecular ions at energy 1.497 7 MeV has been measured using the Coulomb explosion technique. The spectra were used to determine the binding energy of HD+2 and its structure. There existed differences between the spectral structures for proton and for deuteron.     

Coincident fragment detection in strong field photoionization and dissociation of H2

Electron-ion momentum spectroscopy is used to investigate the correlated electronic and nuclear motion in fragmentation of H2 in 4 x 10(14) W/cm(2), 25 fs laser pulses at 795 nm. Reaction channel dependent photoelectron spectra indicate that besides the main, stepwise H2 ionization H2(+) dissociation mechanism resulting in the products H(1s) + H(+) + e(-) a second new mechanism has to be assumed. The momentum distribution of H(+) ions in the dissociation channels H(1s) + H(+) + e(-) and 2H(+) + 2e(-) is found to be independent of the kinetic energy of the photoelectrons.     

Br_2分子在360—610 nm的光解离动力学研究

利用包含转动自由度在内的含时薛定谔方程研究了Br_2分子在波长范围为360—610 nm的光解离动力学.通过计算得到了Br_2分子在四个特征波长处的切片解离影像,并经过分析得到了与切片解离影像相对应的动能分布;计算了Br_2分子在波长范围为360—610 nm内总的动能分布,以及从A,B和C三个电子态解离的碎片各自所对应的动能分布;计算了A,B和C三个电子态各自的解离概率以及碎片产物的分支比Γ(Br~*/(Br+Br~*))随波长的变化.     

强场中初始振动态对H2+解离过程的影响

本文通过数值求解非玻恩-奥本海默近似下的一维含时薛定谔方程模拟了强场中初始振动态对H_2~+解离过程的影响.结果表明:不同初始振动态H_2~+的对应的核动能谱结构不同.低振动态时解离过程主要由阈上解离通道贡献,振动态提高时会增加一个键的软化通道.     

Above threshold dissociation of vibrationally cold HD+ molecules

The experimental study of molecular dissociation of H2+ by intense laser pulses is complicated by the fact that the ions are initially produced in a wide range of vibrational states, each of which responds differently to the laser field. An electrostatic storage device has been used to radiatively cool HD+ ions enabling the observation of above threshold dissociation from the ground vibrational state by 40 fs laser pulses at 800 nm. At the highest intensities used, dissociation through the absorption of at least four photons is found to be the dominant process.     

Anomalous quasielastic electron scattering from single H2, D2, and HD molecules at large momentum transfer: indications of nuclear spin effects

Quasielectron electron scattering from gaseous H2, D2, a 50:50 mixture of H2 and D2, and HD is investigated with 2.25 keV impact energy and a momentum transfer variant Planck's over 2piq of 19.7 a.u. The energy transfer is less than the dissociation energy. The spectral positions of the H and D recoil peaks agree with Rutherford scattering theory. Surprisingly, in the spectrum of the 50:50 H2-D2 mixture, the integrated intensity of the H peak is 31%+/-4% lower (as compared to that of D) than predicted by Rutherford scattering, despite equal screening of nuclear charges by the electrons. In contrast, the ratio of scattering intensities from H and D in HD agrees with the predictions of Rutherford scattering. Comparison is made with neutron Compton scattering results from the same systems, but at higher energy transfers causing bond breaking. Possible theoretical explanations are outlined.     

H2+和HD+分子体系高次谐波发射效率的理论研究

本文通过求解一维含时薛定谔方程, 比较研究了H2+和HD+分子离子体系的高次谐波发射效率. 数值计算结果表明, 在相同激光条件下, 不对称分子体系能产生更高强度的谐波谱. 此外, 借助时频分布, 电离几率和电子-核波包密度概率分布图, 对计算结果做出了合理的解释.     

Three-body dissociation dynamics of the low-lying Rydberg states of H3 and D3

The dynamics of the three-body dissociative charge exchange of fast (12 keV) H+3 and D+3 with Cs have been studied using multiparticle translational spectroscopy. The observed partitioning of product momenta was found to be state-specific and yields insights into the nuclear motion during dissociation for the three lowest-lying 2s 2A'1, 2p 2A'2, and 3p 2E' metastable Rydberg states of H3 and the 2s 2A'1 and 2p 2A'2 states for D3. These results provide direct empirical information on the nonadiabatic couplings that govern the three-body dissociation of the lowest-lying Rydberg states of H3 and D3.     

Enhancing high-order above-threshold dissociation of H2+ beams with few-cycle laser pulses

High-order (three-photon or more) above-threshold dissociation (ATD) of H(2)(+) has generally not been observed using 800 nm light. We demonstrate a strong enhancement of its probability using intense 7 fs laser pulses interacting with beams of H(2)(+), HD(+), and D(2)(+) ions. The mechanism invokes a dynamic control of the dissociation pathway. These measurements are supported by theory that additionally reveals, for the first time, an unexpectedly large contribution to ATD from highly excited electronic states.     

Charge transfer and elastic scattering in very slow H(+)+D(1s) half collisions

Charge transfer and elastic scattering probabilities were measured for half collisions between very slow protons and atomic deuterium. Collision energies down to a few meV, lower by more than an order of magnitude and with better energy resolution than previous measurements, were studied using the dissociation of the HD+ electronic ground state. The collision energy is determined a posteriori from the measured momentum vector of the dissociating charged fragments. The experimental results are in good agreement with our coupled channel calculations.     

Quantum dynamics studies on the non-adiabatic effects of H + LiD reaction

After the Big Bang, chemical reactions of hydrogen with LiH and its isotopic variants played an important role in the late stage of recombination. Moreover, these reactions have attracted the attention of experts in the field of molecular dynamics because of its simple structure. Electronically non-adiabatic effects play a key role in many chemical reactions, while the related studies in LiH₂ reactive system and its isotopic variants are not enough, so the microscopic mechanism of this system has not been fully explored. In this work, the microscopic mechanism of H + LiD reaction are performed by comparing both the adiabatic and non-adiabatic results to study the non-adiabatic effects. The reactivity of R1 (H + LiD → Li + HD) channel is inhibited, while that of R2 (H + LiD → D + LiH) channel is enhanced when the non-adiabatic couplings are considered. For R1 channel, a direct stripping process dominates this channel and the main reaction mechanism is not influenced by the non-adiabatic effects. For R2 channel, at relatively low collision energy, the dominance changes from a rebound process to the complex-forming mechanism when the non-adiabatic effects are considered, whereas the rebound collision approach still dominates the reaction at relatively high collision energy in both calculations. The presented results provide a basis for further detailed study on this importantly astrophysical reaction system.     

丁酮分子的多光子电离-离解机理

研究了丁酮分子经(n0,3d)共振的多光子电离-离解机理(MPID).多光子电离-飞行时间质谱测得的主要离子产物是C2H3O+和CH3CH+2,C2H3O+的强度为CH3CH+2的2～5倍,还有少量C2H+2,C2H+3和CH+3离子,未见到母体离子.主要离子产物的分质量多光了电离谱结构相似,而各离子产物的光强指数不同.实验结果说明丁酮分子的多光子电离-离解机理符合母体离子阶梯模型,文中用梯开关模型对主要产物离子的产生机理进行了解释.     

HD^＋核间距及基态势能曲线的排列通道量子力学计算

依据排列通道量子力学（ＡＣＱＭ）的基本原理，对分子离子ＨＤ＾＋的核间距和基态势能曲线以及离解能Ｄｅ做了量论计算，得到了ＨＤ＾＋的核间距为２．０７２５ａｏ，并求得ＨＤ＾＋按两种方式离解时的势能曲线，认为多数ＨＤ＾＋应按Ｈ＾＋＋Ｄ的方式离解。通过比较计算，文章认为ＨＤ＾＋比Ｈ２＾＋更容易激发和离解，也更不稳定。同时文章对用ＡＣＱＭ解决非对称的同位素微团簇的一般方法做了简明阐述。     

分子高次谐波产生过程中同位素效应的理论研究

本文通过求解非玻恩-奥本海默近似条件下的一维含时薛定谔方程比较研究了H2+和HD+分子离子体系高次谐波谱的特征.数值计算结果表明,对于H2+体系干涉最小值对激光强度和分子初始振动态都很敏感,与此不同,HD+体系的干涉最小值的变化只依赖于初始振动态的选取.此外,借助于时频分布和电离几率,计算结果得到了合理的解释.