Excitation dynamics of Rydberg states in C<Subscript>60</Subscript>

The electron and nuclear dynamics of C₆₀ fullerenes irradiated with femtosecond laser pulses are investigated with photoelectron and photoion spectroscopy. The focus of this work is the detailed exploration of the population mechanism of Rydberg levels within the excitation process of neutral C₆₀. The effect of excitation wavelength, intensity, chirp, and polarization on the kinetic energy distribution of photoelectrons in single-pulse experiments gives first insight into the underlying processes. In combination with time-resolved two-color pump-probe spectroscopy depending on either pump, or probe pulse intensity, a more complete picture of the interaction can be drawn. The results point towards a very interesting but nevertheless complex behavior including four steps: (i) non-adiabatic multielectron excitation of the HOMO (h_u) → LUMO+1 (t_1g) transition; (ii) thermalization within the hot electron cloud on a time scale below 100 fs, followed by a coupling of energy to vibrational modes of the molecule via doorway state(s); (iii) population of electronically excited Rydberg states by multiphoton absorption, and (iv) single photon ionization from the excited Rydberg states. This excitation process results in a characteristic sequence of photoelectron lines in the photoemission spectra. The comparison of the experimental results with recent theoretical work gives convincing evidence that non-adiabatic multielectron dynamics (NMED) plays a key role for the understanding of the response of C₆₀ to short-pulse laser radiation.     

Interaction of dielectrics with femtosecond laser pulses: application of kinetic approach and multiple rate equation

We calculate the transient free-electron density in laser-irradiated dielectrics with two different approaches, both considering the energy distribution of excited electrons. The kinetic approach solves a system of complete Boltzmann collision integrals describing different excitation and relaxation processes in detail. The multiple rate equation (MRE) is an approximative way to keep track of the energy distribution of excited electrons with reduced numerical effort. Both methods are applied to trace dielectric breakdown, considering the changing optical parameters during irradiation with a high-intensity laser pulse. In the MRE approach we include also fast recombination, leading to a delay of the increase of the electronic density and to a decrease of the maximum number of free electrons.     

高频激光脉宽对原子光电子发射谱的影响

采用广义含时伪谱方法数值求解原子在激光脉冲作用下的动量空间含时薛定谔方程,研究了高频激光脉宽对原子光电子发射谱的影响.数值模拟表明,随着激光脉冲宽度的增加,光电子谱干涉结构的振荡幅值逐渐减小,其最大峰值的强度和位置取决于产生有效电离的最大即时强度.通过分析光电子谱的变化规律能进一步加深对高频强场电离产生的动力学干涉效应的理解.     

Excitation and ionization of positronium by 50–100 fs laser pulses

The interaction between Ps and a strong laser pulse of short duration is studied. Substantial population is deposited in excited states under few photon excitation. The possible usefulness as a source of excited Ps to spectroscopy and the formation of antihydrogen is discussed. Finally, photoelectron energy spectra are calculated. This revised version was published online in August 2006 with corrections to the Cover Date.     

Characterization of attosecond XUV pulses from photoelectron spectra of atoms

A method to characterize attosecond extreme ultra violet (XUV) pulses from photoelectron spectra of atoms is presented. A pump pulse prepares a coherent superposition of two atomic bound states, from which photoionization takes place after variable time delays by the attosecond XUV pulse. Information on the spectral phase of the attosecond XUV pulse is extracted from the analysis of photoelectron spectra as a function of photoelectron energy and time delay. Together with information on the spectral intensity obtained from a separate optical measurement, a temporal shape of the attosecond XUV pulse can be precisely reconstructed. After the theoretical formulation of the problem, we present numerical examples for H atom and show that, depending on the choice of energy separation of two bound states, a different accuracy is reached to characterize attosecond XUV pulses.     

Predicting intense-field photoionization of atoms and molecules from their linear photoabsorption spectra in the ionization continuum

We report a new approach to intense-field photoionization that is based on the ad hoc assumption that m photons of energy arriving within a typical electronic response time are effectively equivalent to a single photon of energy . The heuristic model contains no adjustable parameters and unifies apparent multiphoton and field aspects. Moreover, nonsequential, suppressed and above-threshold ionization phenomena become readily understandable. Predicted ionization intensities are in satisfactory agreement with available experimental data ranging from C₆H₆ to Ne^{3 +} , from femtosecond to nanosecond laser pulses, and from ultraviolet to infrared laser radiation.Received: 20 January 2004, Published online: 17 August 2004PACS: 32.80.Rm Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 32.80.Wr Other multiphoton processes - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

利用强场多光子电离技术实现对多原子分子离子振动量子态的光学操控

利用飞秒光电子影像技术研究了碘甲烷分子在飞秒强激光场作用下的多光子电离动力学,在实验上实现了运用飞秒强场多光子电离技术对多原子分子离子的振动量子态进行光学操控.提高了飞秒激光的强度,从1.6×1013W/cm2提高到2.5×1013W/cm2.在增大的激光强度范围内,发现了新的能量组分,并对此进行归属.通过采集光电离的光电子影像可以得到强场电离后光电子的动能分布和角度分布两方面的信息,前期的研究主要侧重于讨论光电子动能随光强的变化,重点讨论了光电子角度分布随光强的变化,通过观察光电子角度分布的变化趋势对振动量子态调控机理进一步认识.     

Excitation transfer between components of molecular layers of cyanine compounds

Using the example of layers of symmetric polymethine dyes, we have studied the optical excitation energy transfer processes between nanocomponents of a molecular layer. The fluorescence yields and life-times of excited states of monomeric stereoisomers have been estimated, and the stereoisomerization yields have been determined. We show that the excitation transfer yield between the S ₁ states of monomeric stereoisomers (tens of percent) is considerably higher than the fluorescence yield (several percent) and depends on the structure of terminal groups of the molecule.     

Phase-dependent electron-ion recombination in a microwave field

Using picosecond laser photoionization of Li in a microwave field we have observed phase-dependent reccombination of the photoelectrons with their parent Li+ ions. Recombination occurs at phases of the microwave field such that energy is removed from the photoelectron in the first microwave cycle after excitation, and there are two maxima in the recombination in each microwave cycle. These observations are consistent with observations made using an attosecond pulse train phase locked to an infrared pulse and with the "simpleman's" model, modified to account for the fact that the photoelectrons are produced in a Coulomb potential.     

Threshold laws in delayed emission: an experimental approach

Delayed emission is a common decay process for very excited complex systems where the excitation energy is, to a large extent, statistically distributed over all accessible degrees of freedom. A rich variety of delayed decay processes is found in complex molecules and clusters such as thermionic emission, evaporation of heavy fragments or blackbody radiation. In this article, we present the general threshold laws that govern the kinetic energy spectrum of matter particles (electrons or fragments) ejected from spherically symmetric species in such processes, and we illustrate these laws by experimental results obtained in photoelectron and photoion spectroscopy. Deviations from simple laws for non spherical species are also evidenced.     

Two-color laser desorption of nanostructured MgO thin films

Neutral magnesium atom emission from nanostructured MgO thin films is induced using two-color nanosecond laser excitation. We find that combined vis/UV excitation, for single-color pulse energies below the desorption threshold, induces neutral Mg-atom emission with hyperthermal kinetic energies in the range of 0.1-0.2 eV. The observed metal atom emission is consistent with a mechanism involving rapid electron transfer to three-coordinated Mg surface sites. The two-color Mg-atom signal is significant only for parallel laser polarizations and temporally overlapped laser pulses indicating that intermediate excited states are short-lived compared to the 5 ns laser pulse duration.     

高等植物外周捕光天线LHCⅡ中的超快光动力学过程

利用飞秒抽运探测技术及时间分辨荧光(TRPL)等光谱技术对高等植物LHCⅡ中的超快光动力学过程进行了研究。在其时间分辨荧光光谱中表现出了明显的各向异性特性。实验上观察了LHCⅡ中色素间的能量传递过程,由飞秒动力学发现,单体内Chlb到邻近的Chla之间的能量传递在200～300fs的时间尺度,Chla激子带间的能量弛豫发生在几百飞秒,不同单体Chla分子间能量分布过程在几个皮秒。而时间分辨荧光和飞秒动力学过程中上百皮秒的慢过程归属于不同聚集体间的能量平衡过程或分子构象变化。     

Luminescence kinetics of an Y0.8Yb0.2F3:Tm3+ solid solution crystal

Upconversion luminescence kinetics of Tm³⁺ doped Y_0.8Yb_0.2F₃ solid solution crystal was studied for various values of pulse excitation parameters: pulse duration, wavelength and excitation power. Analysis of obtained results allowed a conclusion about the presence of transient processes. The transient processes found in upconversion luminescence kinetics are characterized by duration commensurate with lifetime of the excited energy levels of the activator ions. Upon completion of these processes a stable equilibrium state is established between the processes of population and spontaneous decay of the excited energy levels of Tm³⁺ ions. Conditions under which the equilibrium state can be maintained have been considered.     

Theory of energy- and time-resolved two-photon photoemission from metal surfaces – influence of pulse duration and excitation condition

The theory of energy- and time-resolved two-photon photoemission (2PPE) spectra of metal surfaces is presented using density matrix formulation for a three-level system consisting of an initial occupied, intermediate unoccupied and final photoelectron states. A perturbation expansion method is employed to calculate the energy-resolved 2PPE spectrum for continuous light beams. We have obtained analytical expressions of the 2PPE spectrum corresponding to a step-by-step one-photon process through the intermediate state and a direct two-photon-ionization process via virtual transition. It is demonstrated that the intermediate state can also be populated via the nonresonant virtual process. This indicates an absolute importance of “pure dephasing” associated with the transition between the initial and intermediate states. Evolution of the 2PPE spectrum as a function of the pump photon energy is calculated to demonstrate the conditions under which the intrinsic linewidth (total dephasing time) can be deduced from the lineshape analysis. It is also found that the intensity ratio of the two peaks due to the initial and the intermediate states in 2PPE spectrum can be used to estimate the pure dephasing time. Transient behavior of the excited-state population following pulse excitation is calculated with a focus on how the ultrafast relaxation times of the excited states such as image-potential states of metal surfaces are deduced from the transient 2PPE response observed with a pulse laser with much longer duration. The time-resolved 2PPE spectra are calculated for varying detuning from the resonant excitation from the initial state to the intermediate state. Transient responses of the 2PPE signal due to direct ionization and step-by-step processes are also calculated to demonstrate that the nonresonant former process has an influence on the analysis of the cross-correlation trace of the intermediate state, by which the population relaxation time is estimated. Attempts are also made to apply the present theory to a recent time-resolved 2PPE study of the relaxation dynamics of the image-potential states as well as hot electrons in Cu(100) and Ag(100) surfaces. Received: 23 May 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

超短脉冲谐波辐射过程中的量子路径分析

本文数值计算了脉宽为半个光学周期的超短脉冲在不同载波包络相位下的谐波波谱,通过比较谐波波谱截止频率与电子通过主要路径可获得的最大动能的差异,研究了超短脉冲谐波辐射过程中的量子路径。结果显示,超短脉冲谐波辐射过程中电子获得动能的量子路径偏离主要量子路径,而且该偏离效应受载波包络相位的影响。     

超短脉冲谐波辐射过程中的量子路径分析

本文数值计算了脉宽为半个光学周期的超短脉冲在不同载波包络相位下的谐波波谱,通过比较谐波波谱截止频率与电子通过主要路径可获得的最大动能的差异,研究了超短脉冲谐波辐射过程中的量子路径。结果显示,超短脉冲谐波辐射过程中电子获得动能的量子路径偏离主要量子路径,而且该偏离效应受载波包络相位的影响。     

Dynamics of ultrashort pulsed laser radiation induced non-thermal ablation of graphite

We report on the dependence of a laser radiation induced ablation process of graphite on the applied pulse duration of ultrashort pulsed laser radiation smaller than 4 ps. The emerging so-called non-thermal ablation process of graphite has been confirmed to be capable to physically separate ultrathin graphitic layers from the surface of pristine graphite bulk crystal. This allows the deposition of ablated graphitic flakes on a substrate in the vicinity of the target. The observed ablation threshold determined at different pulse durations shows a modulation, which we ascribe to lattice motions along the c axis that are theoretically predicted to induce the non-thermal ablation process. In a simple approach, the ablation threshold can be described as a function of the energy penetration depth and the absorption of the applied ultrashort pulsed laser radiation. Based on the analysis of the pulse duration dependence of those two determining factors and the assumption of an invariant ablation process, we are able to reproduce the pulse duration dependence of the ablation threshold. Furthermore, the observed pulse duration dependences confirm the assumption of a fast material specific response of graphite target subsequent to optical excitation within the first 2 ps.     

Spectral dependent kinetics of the EHD luminescence in As-doped Ge

Following pulsed laser excitation of As-doped Ge with impurity concentrations between 10¹⁵-10¹⁷cm^-3, we observe the electron-hole drop (EHD) and excitonic luminescence decay. The spectrum resolved no-phonon (NP) EHD luminescence kinetics are found to depend on its spectral position. “Plateaus” on the kinetic curves for the high energy side of NP-spectrum are observed at high excitation. The data suggest this luminescence is due to the states which are in dynamical equilibrium during some time after excitation pulse.     

Ultrafast and nanosecond laser-induced desorption of positive ions from lithium fluoride single crystals

We compare desorption of positive ions from lithium fluoride single crystals following pulsed laser excitation using either femtosecond (180 fs, 265 nm) or nanosecond (3 ns, 266 nm) sources. Following optical excitation, desorbed ions are mass analyzed using standard time-of-flight techniques. Several important differences between nanosecond and femtosecond excitation are revealed. Femtosecond excitation produces higher kinetic energy Li⁺ than does nanosecond excitation (10 eV vs. 5 eV) while nanosecond excitation yields significant quantities of impurity ions Na⁺ and K⁺, in addition to efficient Li⁺ emission. The Li⁺ desorption threshold is similar for both laser sources. This similarity is a surprising result, as sub-bandgap nanosecond pulses are only likely to excite defect states efficiently (via linear excitation), while the ultrahigh peak-power femtosecond pulses could in principle induce multiphoton and avalanche excitation. Femtosecond excitation results in much less complicated time-of-flight spectra, as predominantly Li⁺ is detected with some H⁺ also observed. We have measured the Li⁺ yield as a function of time delay between two sub-threshold femtosecond laser pulses. We find that the majority of the Li⁺ yield decays rapidly, largely within the fs pulse duration. However, a weak but measurable decay component of approximately 2 ps is indicated.     

Atomic and molecular ions in intense ultra-fast laser fields

The interaction of a 60 fs 790 nm laser pulse with beams of Ar⁺, C⁺, H₂ ⁺, HD⁺ and D₂ ⁺ are discussed. Intensities up to 10¹⁶ Wcm^-2 are employed. An experimental z-scanning technique is used to resolve the intensity dependent processes in the confocal volume.Received: 6 January 2003, Published online: 15 July 2003PACS: 32.80.Fb Photoionization of atoms and ions - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift