Quantum interference of multi-orbital effects in high-harmonic spectra from aligned carbon dioxide and nitrous oxide

We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO_2 and N_2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of the aligned molecules, a minimum in the harmonic spectrum is observed, the position of which shifts to lower-order harmonics when decreasing the intensity or increasing the ellipticity of the driving laser.This indicates that the minimum originates from the dynamic interference of different channels, of which the tunneling ionization and recombination are contributed via different molecular orbitals.The results show that both the highest occupied molecular orbital(HOMO) and low-lying HOMO-2 in CO_2(or HOMO-1 in N_2O) contribute to the molecular HHG in both linearly and elliptically polarized strong laser fields.Our study would pave a way for understanding multi-electron dynamics from polyatomic molecules irradiated by strong laser fields.     

Ionic Angular Distributions Induced by Strong-Field Ionization of Tri-Atomic Molecules

Angular distributions of fragment ions from ionization of several tri-atomic molecules(CO_2, OCS, N_2O and NO_2) by strong 800-nm laser fields are investigated via a time-of-flight mass spectrometer. Anisotropic angular distributions of fragment ions, especially those of atomic ions, are observed for all of the molecules studied.These anisotropic angular distributions are mainly due to the geometric alignment of molecules in the strong field ionization. Distinct different patterns in ionic angular distributions for different molecules are observed. It is indicated that both molecular geometric structure and ionization channels have effects on the angular distributions of strong field ionization/fragmentation.     

A NEW EXPERIMENTAL METHOD IN THE STUDY OF IONIC RYDBERG STATES BY RESONANCE IONIZATION MASS SPECTROSCOPY

We report a new method for detecting highly excited ions. With a strong constant electric field ionization following the extracting of ions by a pulsed electric field in a time-of-flight mass spectrometer, the direct multi-photon ionization background can be eliminated in laser multi-step resonance ionization mass spectroscopy of ionic Rydberg states. A high detection efficiency call be obtained for law members of ionic Rydberg states by use of this method. We have applied the method in the study of the spectroscopy of ionic Rydberg states ia ytterbium.     

In-source spectroscopy on astatine and radium for resonant laser ionization

At on-line isotope separator facilities, rare isotopes of radioactive elements such as astatine, radium or polonium are demanded for fundamental research on nuclear structure. These elements are generally suitable for a resonance ionization laser ion source, but more data on the atomic structure is necessary to develop efficient laser ionization schemes. Due to the missing stable reference isotopes spectroscopic investigation of the atomic structure can only be performed during on-line operation. At the Isotope Separator and ACcelerator (ISAC) facility at TRIUMF, the elements astatine and radium were investigated by in-source laser spectroscopy to optimize the laser ionization efficiency. For astatine, laser spectroscopy was performed to search for high lying bound states as well as for auto-ionizing resonances. This led to the identification of four new high lying bound states of odd parity, while no auto-ionizing resonances were observed in the investigated region. Furthermore, the feasibility and the impact of laser ionization on the yield of radium isotopes was investigated using an activated target after proton irradiation.     

同位素分子对高次谐波产率的影响

利用含时波包加上傅里叶变换方法研究强激光场中不同同位素分子对高次谐波产率的影响。运用电子与核运动的相干量子力学方法得到了电离电子与正离子的碰撞几率。通过对三种同位素分子H2,D2和T2的碰撞几率分布的对比,发现在前三个光周期内电离电子会多次返回与正离子发生碰撞,但是对应不同同位素分子的碰撞几率的最大值都出现在第一个光周期中。在后两个光周期内三种分子的碰撞几率分布表明较重同位素分子T2对应的碰撞几率最大。通过对三种同位素分子电离率的计算发现同位素分子中较重分子的电离率较高,而电离率越大高次谐波产率越大。因此,在同等条件下,重同位素分子对应较高的高次谐波产率。     

Influence of the initial electronic state on minima of high-order harmonic spectrum radiated from hydrogen molecular ion

We theoretically investigate the high-order harmonic generation of the one-dimensional hydrogen molecular ion at fixed intermediate internuclear distance, driven by a multicycle laser field. Our results show that the initial electronic state of the hydrogen molecular ion affects the modulation of the high-order harmonic spectrum, especially the positions of the minima. Based on the two-state model, the underlying physical mechanism of the minimum is analyzed and discussed.Further analysis shows that the different positions of the minima in the different initial electronic states can be understood via the different interferences of the two phase-adiabatic states at the ionization times.     

Controlling high harmonic generation with molecular wave packets

We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.     

Experimental evidence of a dynamic Jahn-Teller effect in C60(+)

Detailed analysis of the highest occupied molecular orbital band shape in the photoelectron spectrum of gaseous C60 reveals a dynamic Jahn-Teller effect in the ground state of C60(+). The direct observation of three tunneling states asserts a D(3d) geometry for the isolated cation, originating from a strong vibronic coupling. These results show that the ionic motion plays an important role in the electron-phonon interaction.     

In-source laser spectroscopy developments at TRILIS—towards spectroscopy on actinium and scandium

Resonance Ionization Laser Ion Sources (RILIS) have become a versatile tool for production and study of exotic nuclides at Isotope Separator On-Line (ISOL) facilities such as ISAC at TRIUMF. The recent development and addition of a grating tuned spectroscopy laser to the TRIUMF RILIS solid state laser system allows for wide range spectral scans to investigate atomic structures on short lived isotopes, e.g., those from the element actinium, produced in uranium targets at ISAC. In addition, development of new and improved laser ionization schemes for rare isotope production at ISAC is ongoing. Here spectroscopic studies on bound states, Rydberg states and autoionizing (AI) resonances on scandium using the existing off-line capabilities are reported. These results allowed to identify a suitable ionization scheme for scandium via excitation into an autoionizing state at 58,104 cm^???1 which has subsequently been used for ionization of on-line produced exotic scandium isotopes.     

Pulse shape and molecular orientation determine the attosecond charge migration in Caffeine

The recent reduction of laser pulse duration down to the attosecond regime offers unprecedented opportunities to investigate ultrafast changes in the electron density before nuclear motion sets in. Here, we investigate the hole dynamics in the Caffeine molecule that is induced by an ionizing XUV pulse of 6 fs duration using the approximate time-dependent density functional theory method TD-DFTB. In order to account for ionization in a localized atomic orbital basis we apply a complex absorbing potential to model the continuum. Propagation of the time-dependent Kohn–Sham equations allows us to extract the time-dependent hole density taking the pulse shape explicitly into account. Results show that the sudden ionization picture, which is often used to motivate an uncorrelated initial state, fails for realistic pulses. We further find a strong dependence of the hole dynamics on the polarization of the laser field. Notwithstanding, we observe fs charge migration between two distant functional groups in Caffeine even after averaging over the molecular orientation.     

飞秒激光场中OCS分子的里德堡态激发

本文研究了800nm飞秒强激光场下OCS分子的里德堡态激发过程. 实验不仅观测到强激光场中的中性母体分子的里德堡态激发,而且观测到大量的中性里德堡态碎片. 我们测量了里德堡态激发产率随激光强度及椭偏率的变化,并与强场电离解离进行了比较. 分析表明,飞秒激光场下中性里德堡态碎片的产生与强场多次电离密切相关. 此外,我们还讨论了中性里德堡态碎片对激光椭偏率依赖的内在原因.     

Coulomb exploded directional double ionization of N_2O molecules in multicycle femtosecond laser pulses

We experimentally investigate Coulomb exploded directional double ionization of N_2O molecules in elliptically polarized femtosecond laser pulses.The denitrogenation and deoxygenation channels are accessed via various pathways.It leads to distinct asymmetries in directional breaking of the doubly ionized N_2O molecules versus the instantaneous laser field vector, which is revealed by tracing the sum-momentum spectra of the ionic fragments as a recoil of the ejected electrons.Our results demonstrate that the accessibility of the Coulomb exploded double ionization channels of N_2O molecules are ruled by the detailed potential energy curves, and the directional emission of the fragments are governed by the joint effects of the electron localization-assisted enhanced ionization of the stretched molecules and the profiles of the molecular orbitals.     

Satellite peaks in the high energy photoelectron spectra of some small first row molecules

The gas phase high energy photoelectron spectra of CH₄, NH₃, H₂O, N₂, O₂, CO and CO₂ have been recorded, and in all cases weak satellite peaks to high binding energy of the main ionization peak are observed. These peaks are assigned to transitions to ionic states in which valence electron excitation as well as core ionization has occurred. The intensity and position of these peaks, relative to the main ionization peak have been estimated from ab initio UHF calculations on the core hole states, which in general allow assignment of the satellite peaks in terms of orbital transitions of the core hole ion.     

Odd-isotope enrichment studies of Gd by double resonance laser-ionization for the production of burnable nuclear reactor poison

 Because of its large neutron capture cross-section, gadolinium (Gd) is widely used as burnable poison in nuclear reactors. Only two of its naturally occurring seven isotopes are strong neutron absorbers; hence, it would be desirable to enrich Gd in those isotopes. We demonstrate experimentally that significant enrichment can be achieved by two-step laser-ionization by relatively broad-band (bandwidth 1–2 GHz) lasers and by utilizing the isotope shifts only. Our results indicate that the content of the strong absorbers can be raised from the natural 30% to nearly 70%. We also compare the performance of this partially enriched Gd to natural Gd and to pure ¹⁵⁷Gd, the most strongly absorbing isotope, as burnable poison. Received: 3 April 1996/Revised version: 14 October 1996     

激光共振电离过程中铅同位素歧视效应研究

以速率方程为基础,通过数值模拟方法,对Pb的激光共振电离通道：“6s26p2 3P0—6s26p7s 3P0₁—电离”的激光诱导同位素歧视效应进行了研究,以探讨减小激光诱导歧视效应,准确测定Pb同位素比值的有效途径。通过考虑激光线型、原子吸收谱线线型、同位素位移及同位素超精细结构等因素的影响,对速率方程进行近似。在近似的速率方程基础上,以“1+1”激光共振电离过程为例,进而探讨激光峰值功率密度、带宽和中心波长对Pb的同位素歧视效应的影响。研究结果表明,利用最佳波长法,可基本消除同位素歧视效应的影响;提高激发光光强可使Pb同位素饱和电离,从而消除同位素歧视效应的影响;采用宽带激光激发,可减小同位素歧视效应的影响。     

Galena oxidation investigations on oxygen and sulphur isotopes

Batch experiments with the lead sulphide ore mineral galena were carried out in order to get information about the oxidation mechanisms and to contribute to the understanding of field data, especially those obtained from the mining-affected sites. Results indicate that oxygen and sulphur isotopes of dissolved sulphate may be useful tools for the investigation of galena oxidation mechanisms. However, some methodological modifications are necessary to obtain sufficient sulphate yields, which are a prerequisite for the reduction of the analytical uncertainty. Surface and hydrochemical investigations indicated that galena was dissolved non-oxidatively during the experiment at initial pH 2, whereas the oxidative dissolution of galena dominated in experiments at initial pH 6 and 8. No isotope results could be obtained from the experiment at initial pH 2 due to the low sulphate production. The oxidative dissolution of galena resulted in somewhat higher sulphate yields. Thus, the oxygen isotope composition of sulphate produced from galena oxidation could be determined for the first time. Oxygen in sulphate derived largely from water molecules; but minor amounts of molecular oxygen could be also observed. Both molecular oxygen and ferric iron may act as oxidants of galena. A variety of intermediate reactions allow for a variable oxygen isotope composition of sulphate. Sulphur isotopes of sulphate showed an enrichment of (32)S in sulphate (relative to galena), which increases with increasing pH. Sulphur isotope enrichment processes may be associated with the formation of anglesite.     

Resonance ionization mass spectroscopy for nuclear research and trace analysis

Resonance ionization mass spectroscopy (RIMS) has been applied, firstly, to a study of the nuclear properties of short-lived Au isotopes at the on-line isotope separator ISOLDE at CERN and, secondly, to a trace-analysis experiment of Pu.     

用于核物理研究的精密激光谱技术的发展和展望

原子核基本性质（自旋、质量、寿命、磁矩、电四极矩和电荷半径等）与原子核的内在结构密切相关,是检验和发展原子核理论模型的重要依据。实验上可以通过多学科交叉的精密激光谱技术测量原子核外电子的超精细结构和同位素移位,来模型独立地提取原子核的自旋、磁矩、电四极矩和电荷均方根半径等多个核物理参量。这些基本性质的系统测量可以用于探索不稳定原子核中展现出来的新奇的物理现象与规律。近年来,为了测量产额更低的丰中子核的基本性质,激光谱技术不断更新和发展,以实现高分辨、高效率测量。本文详细介绍了激光谱测量的基本原理以及由此发展起来的用于不稳定原子核结构研究的各类互补的激光谱学技术,如共线激光谱（高分辨率低灵敏度）、在源激光谱（高灵敏度低分辨率）、共线共振电离谱（高分辨率高灵敏度）等激光谱技术,以及在不同核区的测量优势和局限。最后结合我国正在发展和规划中的新一代放射性核束装置,讨论精密激光谱技术在国内的发展以及在核物理研究中的应用。     

Novel Experimental Method in the Study of Double Rydberg States by Laser Resonance Excitation

1.IntroductionSequentia1multisteplaserexcitationhasbeenextensivelyusedtostudydoublyexcit-edstatesofa1ka1ine-earthatoms.Mostoftheinvestig8tionsconcernedthedoublyexcitedstatesinwhichoneofthetwovalenceelectronsishighlyexcitedandtheotherisweaklyexcited[1].Inthecasewhenbothvalenceelectronarehighlyexcited(doubleRydbergstates),onlyafewresultswereobtainedduetothelimitutioninexPerimentaltech-nique['j.ThelimitationarosefromvariousaSpectS.First,duringthesequentiallaserex-citationofdoubleRydbergstatesw…