Attosecond ionization time delays in strong-field physics

Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laserbased pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards the full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.

Ionization Engineering of Hydrogels Enables Highly Efficient Salt‑Impeded Solar Evaporation and Night‑Time Electricity Harvesting

Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization.Hydrogels,as a tunable material platform from the molecular level to the macroscopic scale,have been considered the most promising candidate for solar evaporation.However,the simultaneous achievement of high evaporation efficiency and satisfactory tolerance to salt ions in brine remains a challenging scientific bottleneck,restricting the widespread application.Herein,we report ionization engineering,which endows polymer chains of hydrogels with electronegativity for impeding salt ions and activating water molecules,fundamentally overcoming the hydrogel salt-impeded challenge and dramatically expediting water evaporating in brine.The sodium dodecyl benzene sulfonate-modified carbon black is chosen as the solar absorbers.The hydrogel reaches a ground-breaking evaporation rate of 2.9 kg m−2 h−1 in 20 wt%brine with 95.6%efficiency under one sun irradiation,surpassing most of the reported literature.More notably,such a hydrogel-based evaporator enables extracting clean water from oversaturated salt solutions and maintains durability under different high-strength deformation or a 15-day continuous operation.Meantime,on the basis of the cation selectivity induced by the electronegativity,we first propose an all-day system that evaporates during the day and generates salinity-gradient electricity using waste-evaporated brine at night,anticipating pioneer a new opportunity for all-day resource-generating systems in fields of freshwater and electricity.

Excitation and ionization of OCS molecules in strong UV and NIR laser fields

Rydberg state excitation(RSE) is a highly non-linear physical phenomenon that is induced by the ionization of atoms or molecules in strong femtosecond laser fields. Here we observe that both parent and fragments(S, C, OC) of the triatomic molecule carbonyl sulfide(OCS) can survive strong 800 nm or 400 nm laser fields in high Rydberg states. The dependence of parent and fragment RSE yields on laser intensity and ellipticity is investigated in both laser fields, and the results are compared with those for strong-field ionization. Distinctly different tendencies for laser intensity and ellipticity are observed for fragment RSE compared with the corresponding ions. The mechanisms of RSE and strong-field ionization of OCS molecules in different laser fields are discussed based on the experimental results. Our study sheds some light on the strong-field excitation and ionization of molecules irradiated by femtosecond NIR and UV laser fields.

Ion acoustic solitary waves in an adiabatic dusty plasma:Roles of superthermal electrons,ion loss and ionization

We investigate propagation of dust ion acoustic solitary wave(DIASW)in a multicomponent dusty plasma with adiabatic ions,superthermal electrons,and stationary dust.The reductive perturbation method is employed to derive the damped Korteweg-de Vries(DKdV)equation which describes DIASW.The result reveals that the adiabaticity of ions significantly modifies the basic features of the DIASW.The ionization effect makes the solitary wave grow,while collisions reduce the growth rate and even lead to the damping.With the increases in ionization cross sectionΔσ/σ_(0),ion-to-electron density ratioδ_(ie)and superthermal electrons parameterκ,the effect of ionization on DIASW enhances.

Absolute partial and total ionization cross sections of carbon monoxide with electron collision from 350 eV to 8000 eV

The absolute partial and total cross sections for electron impact ionization of carbon monoxide are reported for electron energies from 350 eV to 8000 eV.The product ions(CO^(+),C^(+),O^(+),CO^(2+),C^(2+),and O^(2+))are measured by employing an ion imaging mass spectrometer and two ion-pair dissociation channels(C^(+)+O^(+)and C^(2+)+O^(+))are identified.The absolute cross sections for producing individual ions and their total,as well as for the ion-pair dissociation channels are obtained by normalizing the data of CO^(+)to that of Ar^(+)from CO-Ar mixture target with a fixed 1:1 ratio.The overall errors are evaluated by considering various kinds of uncertainties.A comprehensive comparison is made with the available data,which shows a good agreement with each other over the energy ranges that are overlapped.This work presents new cross-section data with electron energies above 1000 eV.

Internal collision double ionization of molecules driven by co-rotating two-color circularly polarized laser pulses

The double ionization process of molecules driven by co-rotating two-color circularly polarized fields is investigated with a three-dimensional classical ensemble model. Numerical results indicate that a considerable part of the sequential double ionization(DI) events of molecules occur through internal collision double ionization(ICD), and the ICD recollision mechanism is significantly different from that in non-sequential double ionization(NSDI). By analyzing the results of internuclear distances R = 5 a.u. and 2 a.u., these two recollision mechanisms are studied in depth. It is found that the dynamic behaviors of the recollision mechanisms of NSDI and ICD are similar. For NSDI, the motion range of electrons after the ionization is relatively large, and the electrons will return to the core after a period of time. In the ICD process,electrons will rotate around the parent ion before ionization, and the distance of the electron motion is relatively small. After a period of time, the electrons will come back to the core and collide with another electron. Furthermore, the molecular internuclear distance has a significant effect on the electron dynamic behavior of the two ionization mechanisms. This study will help to understand the multi-electron ionization process of complex systems.

Theoretical investigation of electron-impact ionization of W8+ion

The electron-impact single ionization cross section for W8+ion has been calculated using flexible atomic code,employing the level-to-level distorted-wave approximation.This calculations takes into account contributions form both direct ionization(DI)and excitation autoionization(EA).However,the theoretical predictions,based solely on the ground state,tends to underestimate the experimental values.This discrepancy can be mitigated by incorporation contributions from excited states.We extended the theoretical analysis,including the contributions from the long-lived metastable states with lifetimes exceeding 1.5×10-5 s.We employed two statistical models to predict the fraction of ground state ions in the parent ion beam.Assuming a 79%fraction of parent ions in ground configuration,the experiment measurements align with the predictions.Furthermore we derived the theoretical cross-section for the ground state as correlated plasma rate coefficients,and compared it with existing data.Despite the uncertainty in our calculations,our results are still acceptable.

Polarization control of above-threshold ionization spectrum in elliptically polarized two-color laser fields

We study the above-threshold ionization(ATI)process of atoms exposed to fundamental and high-frequency lasers with arbitrary ellipticity by applying the frequency-domain theory.It is found that the angular-resolved ATI spectrum is sensitive to ellipticities of two lasers and emitted angles of the photoelectron.Particularly for the photon energy of the highfrequency laser more than atomic ionization potential,the width of plateau tends to a constant with increasing ellipticity of fundamental field,the dip structure disappears with increasing ellipticity of the high-frequency field.With the help of the quantum channel analysis,it is shown that the angular distribution depends mainly on the ellipticity of high-frequency field in the case that its frequency is high.Moreover,one can see that the maximal and minimal energies in quantum numerical results are in good agreement with the classical prediction.Our investigation may provide theoretical support for experimental research on polarization control of ionization in elliptically polarized two-color laser fields.

Manipulating the electron dynamics in the non-sequential double ionization process of Ar atoms by an orthogonal two-color laser field

Electron dynamics during non-sequential double ionization(NSDI) is one of the most attractive areas of research in the field of laser–atom or laser–molecule interaction. Based on the classic two-dimensional model, we study the process of NSDI of argon atoms driven by a few-cycle orthogonal two-color laser field composed of 800 nm and 400 nm laser pulses. By changing the relative phase of the two laser pulses, a localized enhancement of NSDI yield is observed at 0.5πand 1.5π, which could be attributed to a rapid and substantial increase in the number of electrons returning to the parent ion within extremely short time intervals at these specific phases. Through the analysis of the electron–electron momentum correlations within different time windows of NSDI events and the angular distributions of emitted electrons in different channels, we observe a more pronounced electron–electron correlation phenomenon in the recollision-induced ionization(RII) channel. This is attributed to the shorter delay time in the RII channel.

Steering the energy sharing of electrons in nonsequential double ionization with orthogonally polarized two-color field

Using the semiclassical ensemble model,the dependence of relative amplitude for the recollision dynamics in nonsequential double ionization(NSDI)of neon atom driven by the orthogonally polarized two-color field(OTC)laser field is theoretically studied.And the dynamics in two typical collision pathways,recollision-impact-ionization(RII)and recollisionexcitation with subsequent ionization(RESI),is systematically explored.Our results reveal that the V-shaped structure in the correlated momentum distribution is mainly caused by the RII mechanism when the relative amplitude of the OTC laser field is zero,and the first ionized electrons will quickly skim through the nucleus and share few energy with the second electron.As the relative amplitude increases,the V-shaped structure gradually disappears and electrons are concentrated on the diagonal in the electron correlation spectrum,indicating that the energy sharing after electrons collision is symmetric for OTC laser fields with large relative amplitudes.Our studies show that changing the relative amplitude of the OTC laser field can efficiently control the electron–electron collisions and energy exchange efficiency in the NSDI process.

First Born Double Differential Cross-Section for Ionization of H (3d) by Incident Electron Impact

Double differential cross section (DDCS) of First-Born approximation is calcu-lated for the ionization of metastable 3d-state hydrogen atoms by electron impact energy at 150 eV and 250 eV. A multiple scattering theory is applied in the present study. The present results are compared with the other related the-oretical results for the ionization of hydrogen atoms from different metastable states and ground-state experimental results. The findings demonstrate a strong qualitative agreement with the existing results. The obtained results have an extensive scope for further study of such an ionization process.

Prediction models of the ionization coefficient and ionization cross-section based on multi-layer molecular parameters

Prediction models were proposed to estimate the reduced Townsend ionization coefficient and ionization cross-section.A shape function of the reduced Townsend ionization coefficient curves was derived from the ionization collision probability model.The function had three parameters:the first ionization potential energy,A_(α),and B_(α).A_(α)and B_(α)were related to the molecule symmetry and size.The polarization of molecules could characterize the molecule symmetry.The multi-layer molecular cross-section(MMCS)was proposed to describe the contributions of electrons and molecule radius on different molecule surfaces to collisions.A prediction model of the ionization cross-section was also proposed based on Aα.The molecule parameters were calculated by the Becke3–Lee–Yang–Parr(B3LYP)method and the 6–311G**basis set.We used available data of 30 and 23 gases,respectively,to build the prediction models of reduced Townsend ionization coefficients and ionization cross-sections.The relationships between the molecular parameters Aαand Bαand the ionization cross-section were built up via nonlinear fittings.The determination coefficients R^(2)of Aα,Bα,and the ionization cross-section were 0.877,0.887,and 0.838,respectively.The results showed that the accuracy of models was positively correlated with the molecule symmetry and reduced electric field.This was mainly related to the accuracy of the MMCS model in predicting Aα.The MMCS model needed to be improved to describe the collision direction selectivity caused by the molecule asymmetry.Under a high reduced electric field,that error of Aαhad less influence on the prediction results.However,the prediction results for single atoms with high symmetry were poor.This may be due to the absolute error of the model close to single atoms’reduced Townsend ionization coefficients.The models could provide the basis for gas insulation prediction and discharge calculations,especially for symmetric molecules under a high electric field.

GHz bursts in MHz burst(BiBurst) enabling high-speed femtosecond laser ablation of silicon due to prevention of air ionization

For the practical use of femtosecond laser ablation, inputs of higher laser intensity are preferred to attain high-throughput material removal. However, the use of higher laser intensities for increasing ablation rates can have detrimental effects on ablation quality due to excess heat generation and air ionization. This paper employs ablation using BiBurst femtosecond laser pulses, which consist of multiple bursts(2 and 5 bursts) at a repetition rate of 64 MHz, each containing multiple intra-pulses(2–20 pulses) at an ultrafast repetition rate of 4.88 GHz, to overcome these conflicting conditions. Ablation of silicon substrates using the BiBurst mode with 5 burst pulses and 20 intra-pulses successfully prevents air breakdown at packet energies higher than the pulse energy inducing the air ionization by the conventional femtosecond laser pulse irradiation(single-pulse mode). As a result, ablation speed can be enhanced by a factor of23 without deteriorating the ablation quality compared to that by the single-pulse mode ablation under the conditions where the air ionization is avoided.

Electron-impact ionization of W^(9+)and W^(10+)

Electron-impact single-ionization(EISI)cross sections for W^(q+)(q=9,10)ions have been calculated by using the level-to-level distorted-wave(LLDW)method with emphasis on the contribution of metastable states to the total ionization cross sections.Contributions from direct-ionization(DI)and excitation-autoionization(EA)processes are taken into account.The calculated cross sections include the contributions from both the ground configuration and the long-lived metastable states with lifetimes exceeding 10^(-6)s.Calculated cross sections are in good agreement with experimental measurements when the influence of metastable states on the total ionization cross section are well considered.

Modeling of magnetized collisional plasma sheath with nonextensive electron distribution and ionization source

The properties of an atmospheric-pressure collisional plasma sheath with nonextensively distributed electrons and hypothetical ionization source terms are studied in this work. The Bohm criterion for the magnetized plasma is extended in the presence of an ion–neutral collisional force and ionization source. The effects of electron nonextensive distribution, ionization frequency, ion–neutral collision, magnetic field angle and ion temperature on the Bohm criterion of the plasma sheath are numerically analyzed. The fluid equations are solved numerically in the plasma–wall transition region using a modified Bohm criterion as the boundary condition. The plasma sheath properties such as charged particle density, floating sheath potential and thickness are thoroughly investigated under different kinds of ion source terms, contributions of collisions, and magnetic fields. The results show that the effect of the ion source term on the properties of atmosphericpressure collisional plasma sheath is significant. As the ionization frequency increases, the Mach number of the Bohm criterion decreases and the range of possible values narrows. When the ion source is considered, the space charge density increases, the sheath potential drops more rapidly,and the sheath thickness becomes narrower. In addition, ion–neutral collision, magnetic field angle and ion temperature also significantly affect the sheath potential profile and sheath thickness.

Fragmentation dynamics of electron-impact double ionization of helium

We study the double ionization dynamics of a helium atom impacted by electrons with full-dimensional classical trajectory Monte Carlo simulation. The excess energy is chosen to cover a wide range of values from 5 e V to 1 ke V for comparative study. At the lowest excess energy, i.e., close to the double-ionization threshold, it is found that the projectile momentum is totally transferred to the recoil-ion while the residual energy is randomly partitioned among the three outgoing electrons, which are then most probably emitted with an equilateral triangle configuration. Our results agree well with experiments as compared with early quantum-mechanical calculation as well as classical simulation based on a two-dimensional Bohr's model. Furthermore, by mapping the final momentum vectors event by event into a Dalitz plot,we unambiguously demonstrate that the ergodicity has been reached and thus confirm a long-term scenario conceived by Wannier. The time scale for such few-body thermalization, from the initial nonequilibrium state to the final microcanonical distribution, is only about 100 attoseconds. Finally, we predict that, with the increase of the excess energy, the dominant emission configuration undergoes a transition from equilateral triangle to T-shape and finally to a co-linear mode. The associated signatures of such configuration transition in the electron–ion joint momentum spectrum and triple-electron angular distribution are also demonstrated.

Rapid authentication of different herbal medicines by heating online extraction electrospray ionization mass spectrometry

The rapid and accurate authentication of traditional Chinese medicines(TCMs)has always been a key scientific and technical problem in the field of pharmaceutical analysis.Herein,a novel heating online extraction electrospray ionization mass spectrometry(H-oEESI-MS)was developed for the rapid and direct analysis of extremely complex substances without the requirement for any sample pretreatment or pre-separation steps.The overall molecular profile and fragment structure features of various herbal medicines could be completely captured within 10–15 s,with minimal sample(<0.5 mg)and solvent consumption(<20μL for one sample).Furthermore,a rapid differentiation and authentication strategy for TCMs based on H-oEESI-MS was proposed,including metabolic profile characterization,characteristic marker screening and identification,and multivariate statistical analysis model validation.In an analysis of 52 batches of seven types of Aconitum medicinal materials,20 and 21 key compounds were screened out as the characteristic markers of raw and processed Aconitum herbal medicines,respectively,and the possible structures of all the characteristic markers were comprehensively identified based on Compound Discoverer databases.Finally,multivariate statistical analysis showed that all the different types of herbal medicines were well differentiated and identified(R^(2)X>0.87,R^(2)Y>0.91,and Q^(2)>0.72),which further verified the feasibility and reliability of this comprehensive strategy for the rapid authentication of different TCMs based on H-oEESI-MS.In summary,this rapid authentication strategy realized the ultra-high-throughput,low-cost,and standardized detection of various complex TCMs for the first time,thereby demonstrating wide applicability and value for the development of quality standards for TCMs.

High-throughput analysis of anthocyanins in horticultural crops using probe electrospray ionization tandem mass spectrometry (PESI/MS/MS)

Plant secondary metabolites exhibit various horticultural traits.Simple and rapid analysis methods for evaluating these metabolites are in demand in breeding and consumer markets dealing with horticultural crops.We applied probe electrospray ionization(PESI)to evaluate secondary metabolite levels in horticultural crops.PESI does not require pre-treatment and separation of samples,which makes it suitable for high-throughput analysis.In this study,we targeted anthocyanins,one of the primary pigments in horticultural crops.Eighty-one anthocyanins were detected in approximately 3 minutes in the selected reaction-monitoring mode.Tandem mass spectrometry(MS/MS)could adequately distinguish between the fragments of anthocyanins and flavonols.Probe sampling,an intuitive method of sticking a probe directly to the sample,could detect anthocyanins qualitatively on a micro-area scale,such as achenes and receptacles in strawberry fruit.Our results suggest that PESI/MS/MS can be a powerful tool to characterize the profile of anthocyanins and compare their content among cultivars.

Wavelength-and ellipticity-dependent photoelectron spectra from multiphoton ionization of atoms

We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schr ¨odinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the(2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.

Measuring^(222)Rn in aquatic environment via Pulsed Ionization Chamber Radon Detector

Radon(Rn)is a naturally occurring radioactive inert gas in nature,and^(222)Rn has been routinely used as a powerful tracer in various aquatic environmental research on timescales of hours to days,such as submarine groundwater discharge.Here we developed a new approach to measure^(222)Rn in discrete water samples with a wide range of^(222)Rn concentrations using a Pulsed Ionization Chamber(PIC)Radon Detector.The sensitivity of the new PIC system is evaluated at 6.06 counts per minute for 1 Bq/L when a 500 mL water sample volume is used.A robust logarithmic correlation between sample volumes,ranging from 250 mL to 5000 mL,and system sensitivity obtained in this study strongly suggests that this approach is suitable for measuring radon concentration levels in various natural waters.Compared to the currently available methods for measuring radon in grab samples,the PIC system is cheaper,easier to operate and does not require extra accessories(e.g.,drying tubes etc.)to maintain stable measurements throughout the counting procedure.