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The momentum distribution of photoelectrons in H 2 + molecules subjected to an attosecond pulse is theoretically investigated. To better understand the laser-molecule interaction, we develop an in-line photoelectron holography approach that is analogous to optical holography. This approach is specifically suitable for extracting the amplitude and phase of the forward-scattered electron wave packet in a dissociating molecule with atomic precision. We also extend this approach to imaging the transient scattering cross-section of a molecule dressed by a near infrared laser field. This attosecond photoelectron holography sheds light on structural microscopy of dissociating molecules with high spatial-temporal resolution.

We experimentally study two-body Coulomb explosions of CO2, O2, and CH3Cl molecules in intense femtosecond laser pulses. We observe an obvious variation in the ionic angular distribution of the fragments with respect to the kinetic energy releases (KERs). Using a classical model based on ab initio potential energy curves, we find that the dependence of the ionic angular distribution on the KER is relevant to the fact that the accurate potential energy deviates significantly from the value determined by applying the Coulomb interaction approximation at a relatively small internuclear distance of the molecule. We show that the KER-dependent ionic angular distribution provides an effective way to determine the critical internuclear distance at which the Coulomb interaction approximation holds or breaks down without relying on the knowledge of the accurate potential energy curves., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

Light-induced deprotonation of molecules is an important process in photochemical reactions. Here, we theoretically investigate the tunneling deprotonation of H2+ and its asymmetric isotopologues driven by circularly polarized THz laser pulses. The quasi-static picture shows that the field-dressed potential barrier is significantly lowered for the deprotonation channel when the mass asymmetry of the diatomic molecule increases. Our numerical simulations demonstrate that when the mass symmetry breaks, the tunneling deprotonation is significantly enhanced and the proton tunneling becomes the dominant dissociation channel in the THz driving fields. In addition, the simulated nuclear momentum distributions show that the emission of the proton is directed by the effective vector potential for the deprotonation channel and, meanwhile, the angular distribution of the emitting proton is affected by the alignment and rotation of the molecule induced by the rotating field., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

With the development of intelligent aquaculture, the aquaculture industry is gradually switching from traditional crude farming to an intelligent industrial model. Current aquaculture management mainly relies on manual observation, which cannot comprehensively perceive fish living conditions and water quality monitoring. Based on the current situation, this paper proposes a data-driven intelligent management scheme for digital industrial aquaculture based on multi-object deep neural network (Mo-DIA). Mo-IDA mainly includes two aspects of fish state management and environmental state management. In fish state management, the double hidden layer BP neural network is used to build a multi-objective prediction model, which can effectively predict the fish weight, oxygen consumption and feeding amount. In environmental state management, a multi-objective prediction model based on LSTM neural network was constructed using the temporal correlation of water quality data series collection to predict eight water quality attributes. Finally, extensive experiments were conducted on real datasets and the evaluation results well demonstrated the effectiveness and accuracy of the Mo-IDA proposed in this paper.

New insights are proposed into enhancing detection of uranyl ions (UO 2 2+ ) by electropolymerization brilliant cresyl blue-modified glassy carbon electrode (PBCB/GCE). The mercury-free PBCB/GCE sensor was applied to determine UO 2 2+ in water samples by differential pulse adsorptive stripping voltammetry (DPAdSV). The unique combination of the PBCB/GCE and DPAdSV significantly improves sensitivity due to the polymer of high electroactive area and fast electron transfer rate. The DPAdSV current using a 3 mm diameter PBCB/GCE was proportional to the UO 2 2+  concentration in the range 2.0-90.0 μg·L -1 (- 0.113 V vs. SCE) with a detection limit of 0.650 μg·L -1 , RSD = 3.1% (n = 10), and 4.5% reproducibility. In addition, the sensitivity for UO 2 2+ determination was further improved at using an 1 mm diameter PBCB/GCE, which enhances the efficiency of UO 2 2+ deposition due to its higher current density. The 1 mm diameter PBCB/GCE based on DPAdSV technique could be used to determine uranyl ions in the concentration range 0.20-2.0 μg·L -1 (- 0.113 V vs. SCE) with a detection limit of 0.067 μg·L -1 , RSD = 5.7 % (n = 10) and 5.4% reproducibility. Hence, the PBCB/GCE is a suitable candidate to substitute the mercury electrode. Graphical abstract., (© 2022. The Author(s), under exclusive licence to Springer-Verlag GmbH Austria, part of Springer Nature.)

Tunneling is one of the most fundamental and ubiquitous processes in the quantum world. The question of how long a particle takes to tunnel through a potential barrier has sparked a long-standing debate since the early days of quantum mechanics. Here, we propose and demonstrate a novel scheme to accurately determine the tunneling time of an electron. In this scheme, a weak laser field is used to streak the tunneling current produced by a strong elliptically polarized laser field in an attoclock configuration, allowing us to retrieve the tunneling ionization time relative to the field maximum with a precision of a few attoseconds. This overcomes the difficulties in previous attoclock measurements wherein the Coulomb effect on the photoelectron momentum distribution has to be removed with theoretical models and it requires accurate information of the driving laser fields. We demonstrate that the tunneling time of an electron from an atom is close to zero within our experimental accuracy. Our study represents a straightforward approach toward attosecond time-resolved imaging of electron motion in atoms and molecules., (© 2022. The Author(s).)

With a three-dimensional classical ensemble method, we theoretically investigated the correlated electron dynamics in nonsequential double ionization (NSDI) driven by the spatially inhomogeneous fields. Our results show that NSDI in the spatially inhomogeneous fields is more efficient than that in the spatially homogeneous fields at the low laser intensities, while at the high intensities NSDI is suppressed as compared to the homogeneous fields. More interestingly, our results show that the electron pairs from NSDI exhibit a much stronger angular correlation in the spatially inhomogeneous fields, especially at the higher laser intensities. The correlated electron momentum distribution shows that in the inhomogeneous fields the electron pairs favor to achieve the same final momentum, and the distributions dominantly are clustered in the more compact regions. It is shown that the electron's momentum is focused by the inhomogeneous fields. The underlying dynamics is revealed by back-tracing the classical trajectories.

Laser-induced tunneling ionization is one of the fundamental light-matter interaction processes. An accurate description of the tunnel-ionized electron wave packet is central to understanding and controlling subsequent electron dynamics. Because of the anisotropic molecular structure, tunneling ionization of molecules involves considerable challenges in accurately describing the tunneling electron wave packet. Up to now, some basic properties of the tunneling electron from molecules still remain unexplored. Here, we demonstrate that the tunneling electron from a molecule is not always emitted from the geometric center of the molecule along the tunnel direction. Rather, the photoemission position depends on the molecular orientation. Using a photoelectron holographic technique, we determine the photoemission position for a nitrogen molecule relative to the molecular geometric center to be 95±21  pm when the molecular axis is oriented along the tunnel direction. Our Letter poses, and answers experimentally, a fundamental question as to where the molecular photoionization actually begins, which has significant implications for time-resolved probing of valence electron dynamics in molecules.

By numerically solving the time-dependent Schrödinger equation, we theoretically study strong-field tunneling ionization of Ar atom in the parallel two-color field which consists of a strong fundamental pulse and a much weaker second harmonic component. Based on the quantum orbits concept, we analyzed the photoelectron momentum distributions with the phase-of-the-phase spectroscopy, and the relative contributions of the two parts of the photoelectrons produced during the rising and falling edges of the adjacent quarters of the laser cycle are identified successfully. Our results show that the relative contributions of these two parts depend on both of the transverse and longitude momenta. By comparing the results from model atoms with Coulomb potential and short-range potential, the role of the long-range Coulomb interaction on the relative contributions of these two parts of electrons is revealed. Additionally, we show that the effects of Coulomb interaction on ionization time are vital for identifying their relative contributions.

This study conducted the first life cycle analysis for citrus residue (CR) management systems in China. The results indicated conventional waste treatment systems were not suitable for CR management in China. Although feed system seems to be a favourable option, the uncertainty analysis suggested valorisation system could achieved better performance in global warming, eutrophication and human toxicity. The environmental impacts of valorisation systems were more sensitive to energy consumption. For silage and single cell protein (SCP) system, the environmental impacts could be significantly reduced by improving the energy use efficiency or using more renewable energy. In comparison, although the environmental impacts of biorefinery system were less favourable than SCP and silage systems. The multiple extraction unit had less impact than reported values in other studies. Further research in biorefinery system can focus on increasing the energy efficiency of pre-treatment or reuse of extraction chemicals., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Up to now, to directly image the onset of Jahn-Teller symmetry breaking remains unreached. Here we employ ultrafast ion-coincidence Coulomb explosion imaging with sub-10 fs resolution and unambiguously image the ultrafast dynamics of Jahn-Teller deformations of [Formula: see text] cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C 3v to C 2v geometries takes a characteristic time of 20 ± 7 fs for this system. Classical and quantum molecular dynamics simulations agree well with the measurement, and reveal dynamics for the build-up of the C 2v structure involving complex revival process of multiple vibrational pathways of the [Formula: see text] cation., (© 2021. The Author(s).)

By solving the three-dimensional time-dependent Schrödinger equation, we investigate the angular distributions of the low-energy electrons when an intense high-frequency laser pulse is applied to the hydrogen atom. Our numerical results show that the angular distributions of the low-energy electrons which generated by the nonadiabatic transitions sensitively depend on the laser intensity. The angular distributions evolve from a two-lobe to a four-lobe structure as the laser intensity increases. By analyzing nonadiabatic process in the Kramers-Henneberger frame, we illustrate that this phenomenon is attributed to the intensity-dependent adiabatic evolution of the ground state wavefunction. When the laser intensity further increases, the pathway of nonadiabatic transition from the ground state to the excited state and then to the continuum states is non-negligible, which results in the ring-like structure in the photoelectron momentum distribution. The angular distributions of the low-energy electrons provide a way to monitor the evolution of the electron wavefunction in the intense high frequency laser fields.

We theoretically study the interference of photoelectrons released from atomic p ± orbitals in co-rotating and counter-rotating circularly polarized two-color laser pulses consisting of a strong 400-nm field and a weak 800-nm field. We find that in co-rotating fields the interference fringes in the photoelectron momentum distributions are nearly the same for p ± orbitals, while in counter-rotating fields the interference fringes for p + and p - orbitals oscillate out of phase with respect to the electron emission angle. The simulations based on the strong-field approximation show a good agreement with the numerical solutions of the time-dependent Schrödinger equation. We find that different phase distributions of the electron wave packets emitted from p + and p - orbitals can be easily revealed by the counter-rotating circularly polarized two-color laser fields. We further show that the photoelectron interference patterns in the circularly polarized two-color laser fields record the time differences of the electron wave packets released within an optical cycle.

By numerically solving the time-dependent Schrödinger equation, we theoretically investigate the dynamics of the low-energy photoelectrons ionized by a single attosecond pulse in the presence of an infrared laser field. The obtained photoelectron momentum distributions exhibit complicated interference structures. With the semiclassical model, the originations for the different types of the interference structures are unambiguously identified. Moreover, by changing the time delay between the attosecond pulse and the infrared laser field, these interferences could be selectively enhanced or suppressed. This enables us to extract information about the ionization dynamics encoded in the interference structures. As an example, we show that the phase of the electron wave-packets ionized by the linearly and circularly polarized attosecond pulses can be extracted from the interference structures of the direct and the near-forward rescattering electrons.

Strong-field photoelectron holography (SFPH), originating from the interference of the direct electron and the rescattering electron in tunneling ionization, is a significant tool for probing structure and electronic dynamics in molecules. We theoretically study SFPH by counter rotating two-color circularly (CRTC) polarized laser pulses. Different from the case of the linearly polarized laser field, where the holographic structure in the photoelectron momentum distribution (PEMD) is clustered around the laser polarization direction, in the CRTC laser fields, the tunneling ionized electrons could recollide with the parent ion from different angles and thus the photoelectron hologram appears in the whole plane of laser polarization. This property enables structural information delivered by the electrons scattering the molecule from different angles to be recorded in the two-dimensional photoelectron hologram. Moreover, the electrons tunneling at different laser cycles are streaked to different angles in the two-dimensional polarization plane. This property enables us to probe the sub-cycle electronic dynamics in molecules over a long time window with the multiple-cycle CRTC laser pulses.

We theoretically investigated frustrated tunneling ionization (FTI) in the interaction of atoms with elliptically polarized laser pulses by a semiclassical ensemble model. Our results show that the yield of frustrated tunneling ionization events exhibits an anomalous behavior which maximizes at the nonzero ellipticity. By tracing back the initial tunneling coordinates, we show that this anomalous behavior is due to the fact that the initial transverse velocity at tunneling of the FTI events is nonzero in the linear laser pulses and it moves across zero as the ellipticity increases. The FTI yield maximizes at the ellipticity when the initial transverse momentum for being trapped is zero. Moreover, the angular momentum distribution of the FTI events and its ellipticity dependence are also explored. The anomalous behavior revealed in our work is very similar to the previously observed ellipticity dependence of the near- and below-threshold harmonics, and thus our work may uncover the mechanism of the below-threshold harmonics which is still a controversial issue.

Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectron holographic fringes generated by a strong 800-nm pulse. The fringe shift offers direct experimental access to the intermediate canonical momentum of the rescattering electron, allowing us to reconstruct the momentum offset at the tunnel exit with high accuracy. Our result unambiguously proves the existence of nonzero initial longitudinal momentum at the tunnel exit and provides fundamental insights into the nonquasistatic nature of the strong-field tunneling.

Using the classical ensemble method, we have investigated the alignment dependence of the correlated electron dynamics in strong-field nonsequential double ionization (NSDI) of diatomic molecules driven by linearly polarized laser pulses. Our numerical results show that the correlated electron pairs are more likely to emit into the same hemisphere (side-by-side emission) for the parallel aligned molecules at the small internuclear distance, in agreement with previous experimental results. Surprisingly, as the internuclear distance increases, this side-by-side emission is more prevalent for the perpendicularly aligned molecules. Back analyzing of the classical trajectories shows that a considerable part of the NSDI events for the parallel aligned molecules at the large internuclear distances occur through an internal collision, not the well-known recollision. In the internal collision induced NSDI, the first electron tunnels through the inner barrier from the up-field core, moves directly towards the other core, and kicks out the second electron. For this type of NSDI events, the electron pairs are more likely to emit into the opposite hemispheres and thus the correlated electron momentum spectrum exhibits a more dominant back-to-back behavior in the parallel aligned molecules.

Quantitative identification of tunneling ionization (TI) and multiphoton ionization (MPI) with Keldysh parameter γ in intermediate regime is of great importance to better understand various ionization-triggered strong-field phenomena. We theoretically demonstrate that the numerical observable ionization delay time is a more reliable indicator for characterizing the transition from TI to MPI under different laser parameters. Using non-linear iterative curve fitting algorithm (NICFA), the detected time-dependent probability current of ionized electrons can be decoupled into weighted TI and MPI portions. This enables us to confirm that the observed plateau-like structure in ionization delay time picture at the intermediate γ originates from the competition between TI and MPI processes. A hybrid quantum and classical approach (HQCA) is developed to evaluate the weights of TI and MPI electrons in good agreement with NICFA result. Moreover, the well separated TI and MPI electrons using HQCA are further propagated classically for mapping their final momentum, which well reproduces the experimental or ab-initio numerical calculated signatures of ionized electron momentum distribution in a rather broad γ regime.

The nonadiabaticity of quantum tunneling through an evolving barrier is relevant to resolving laser-driven dynamics of atoms and molecules at an attosecond timescale. Here, we propose and demonstrate a novel scheme to detect the nonadiabatic behavior of tunnel ionization studied in an attoclock configuration, without counting on the laser intensity calibration or the modeling of the Coulomb effect. In our scheme, the degree of nonadiabaticity for tunneling scenarios in elliptically polarized laser fields can be steered continuously simply with the pulse ellipticity, while the critical instantaneous vector potentials remain identical. We observe the characteristic feature of the measured photoelectron momentum distributions, which matches the distinctive prediction of nonadiabatic theories. In particular, our experiments demonstrate that the nonadiabatic initial transverse momentum at the tunnel exit is approximately proportional to the instantaneous effective Keldysh parameters in the tunneling regime, as predicted theoretically by Ohmi, Tolstikhin, and Morishita [Phys. Rev. A 92, 043402 (2015)PLRAAN1050-294710.1103/PhysRevA.92.043402]. Our study clarifies a long-standing controversy over the validation of the adiabatic approximation and will substantially advance studies of laser-induced ultrafast dynamics in experiments.

With the semiclassical ensemble model, we systematically investigate the correlated electron dynamics in strong-field nonsequential double ionization (NSDI) by the counter-rotating circularly polarized two-color (CPTC) laser pulses. Our results show that the angular distributions of the electrons in NSDI sensitively depend on the intensity ratio of the CPTC laser fields. At the small ratio, the electron pairs emit with a relative angle of about 120°, and this angle shifts to 40° as the ratio increases and finally it exhibits a wide range distribution as the intensity ratio further increases. Back analysis of the NSDI trajectories shows that this behavior results from the relative-intensity-dependence of the release time of the electron pairs in the CPTC laser fields. The release times of the electron pairs are directly mapped to the angular distribution. Our results indicate that the emission times of the correlated electrons in NSDI can be controlled with the CPTC laser fields.

Laser-induced electron tunneling ionization from atoms and molecules plays as the trigger for a broad class of interesting strong-field phenomena in attosecond community. Understanding the time of electron tunneling ionization is vital to achieving the ultimate accuracy in attosecond metrology. We propose a novel attosecond photoelectron interferometer, which is based on the interference of the direct and near-forward rescattering electron wave packets, to determine the time information characterizing the tunneling process. Adding a weak perturbation in orthogonal to the strong fundamental field, the phases of the direct and the near-forward rescattering electron wave packets are modified, leading to the shift of the interferogram in the photoelectron momentum distributions. By analyzing the response of the interferogram to the perturbation, the real part of the ionization time, which denotes the instant when the electron exits the potential barrier, and the associated rescattering time are precisely retrieved. Moreover, the imaginary part of the ionization time, which has been interpreted as a quantity related to electron motion under the potential barrier, is also unambiguously determined.

Electron correlation is ubiquitous across diverse physical systems from atoms and molecules to condensed matter. Observing and controlling dynamical electron correlation in photoinduced processes paves the way to the coherent control of chemical reactionsand photobiological processes. Here, we experimentally investigate dynamics of electron correlation in double ionization of neon irradiated by intense elliptically polarized laser pulses. We find a characteristic, ellipticity-dependent, correlated electron emission along the minor axis of the elliptically polarized light. This observation is well reproduced by a semi-classical ensemble model simulation. By tracing back the corresponding electron trajectories, we find that the dynamical energy sharing during the electron emission process is modified by the ellipticity of the laser light. Thus, our work provides evidence for a possible ultrafast control of the energy sharing between the correlated electrons by varying the light ellipticity.

Accurate determination of laser intensity is of fundamental importance to study various phenomena in intense laser-atom/molecule interactions. We theoretically demonstrate a scheme to measure laser intensity by examining the holographic structure originating from the interference between the direct and near-forward rescattering electrons in strong-field tunneling ionization. By adding a weak second-harmonic field with polarization orthogonal to the strong fundamental driving field, the interference pattern oscillates with the changing relative phases of the two-color fields. Interestingly, the amplitude of this oscillation in the photoelectron momentum spectrum depends on the parallel momentum. With the quantum-orbit analysis, we show that the amplitude of the oscillation minimizes when the time difference between the recollision and ionization of near-forward rescattering electron is half cycle of the fundamental driving field. This enables us to measure accurately the laser intensity by seeking the minimum of the oscillation amplitude. Moreover, we show that this minimum can be determined without scanning the relative phases, instead, by just monitoring the interference patterns for two relative phases. This facilitates the application of our scheme in experiment.

We report on the scaling of the photoelectron holography with the laser ellipticity in strong-field atomic ionization. We find that the spacing of the holographic fringe gradually decreases with increasing of the ellipticity. In terms of the strong-field approximation, the scaling of the fringe spacing with the laser ellipticity is explained by the effect of the initial transverse momenta at the tunnel exit. With increasing of the laser ellipticity, a ridge structure arising from forward scattering electrons is observed in the low-energy region of the electron momentum distribution. An analytic formula is obtained that demarcates the phase diagram for the observation of the holographic pattern and ridge structure in elliptically polarized laser fields.

We measure the recoil-ion momentum distributions from nonsequential double ionization of Ne by two-color laser pulses consisting of a strong 800-nm field and a weak 400-nm field with parallel polarizations. The ion momentum spectra show pronounced asymmetries in the emission direction, which depend sensitively on the relative phase of the two-color components. Moreover, the peak of the doubly charged ion momentum distribution shifts gradually with the relative phase. The shifted range is much larger than the maximal vector potential of the 400-nm laser field. Those features are well recaptured by a semiclassical model. Through analyzing the correlated electron dynamics, we found that the energy sharing between the two electrons is extremely unequal at the instant of recollison. We further show that the shift of the ion momentum corresponds to the change of the recollision time in the two-color laser field. By tuning the relative phase of the two-color components, the recollision time is controlled with attosecond precision.

Watching the valence electron move in molecules on its intrinsic timescale has been one of the central goals of attosecond science and it requires measurements with subatomic spatial and attosecond temporal resolutions. The time-resolved photoelectron holography in strong-field tunneling ionization holds the promise to access this realm. However, it remains to be a challenging task hitherto. Here we reveal how the information of valence electron motion is encoded in the hologram of the photoelectron momentum distribution (PEMD) and develop a novel approach of retrieval. As a demonstration, applying it to the PEMDs obtained by solving the time-dependent Schrödinger equation for the prototypical molecule H_{2}^{+}, the attosecond charge migration is directly visualized with picometer spatial and attosecond temporal resolutions. Our method represents a general approach for monitoring attosecond charge migration in more complex polyatomic and biological molecules, which is one of the central tasks in the newly emerging attosecond chemistry.

Due to its strong ultraviolet absorption, low background interference in the small molecular range, and salt tolerance capacity, N-phenyl-2-naphthylamine (PNA) was developed as a novel matrix in the present study for analysis and imaging of small molecules by matrix-assisted laser desorption/ionization mass spectrometry time-of-fight (MALDI-TOF MS). The newly developed matrix displayed good performance in analysis of a wide range of small-molecule metabolites including free fatty acids, amino acids, peptides, antioxidants, and phospholipids. In addition, PNA-assisted LDI MS imaging of small molecules in brain tissue of rats subjected to middle cerebral artery occlusion (MCAO) revealed unique distributions and changes of 89 small-molecule metabolites including amino acids, antioxidants, free fatty acids, phospholipids, and sphingolipids in brain tissue 24 h postsurgery. Fifty-nine of the altered metabolites were identified, and all the changed metabolites were subject to relative quantitation and statistical analysis. The newly developed matrix has great potential application in the field of biomedical research.

Using the classical ensemble model, we systematically investigate strong-field nonsequential double ionization (NSDI) of Mg by intense elliptically polarized laser pulses with different wavelengths. Different from the noble atoms, NSDI occurs for Mg driven by elliptically and circularly polarized laser fields. Our results show that in elliptically and circularly polarized laser fields, the NSDI yield is sharply suppressed as the wavelength increases. Interestingly, the correlated behavior in the electron momentum spectra depends sensitively on the wavelengths. The corresponding electron dynamics is revealed by back tracing the classical trajectory.

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajectories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H_{2} and D_{2} are used simultaneously to retrieve the nuclear dynamics on the attosecond and ångström scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.

We study the carrier-envelope phase (CEP) dependent photoelectron energy spectra from above-threshold ionization by numerically solving the time-dependent Schrödinger equation of hydrogen atom in a few-cycle laser field at intensities in the range of (2-10) × 10 13 W/cm 2 . Depending on the electron energy and the laser intensity, the yield of the photoelectron reveals clear oscillations with respect to the CEP. At high laser intensities (larger than ~3 × 10 13 W/cm 2 ), the yield of the high-energy photoelectrons (larger than 2U p , with U p being the ponderomotive potential) shows two kinds of oscillations with the CEP for different electron energies. There is a clear phase jump for those two kinds of oscillations. In contrast, at low laser intensities (smaller than ~3 × 10 13 W/cm 2 ), the phase of the oscillation for the high-energy photoelectron yield with the CEP is nearly independent on the electron energy, which will reduce the sensitivity of the retrieval of single-shot CEP using the method reported by T. Wittmann et al. [Nat. Phys. 5, 357 (2009)] at low laser intensities. We further show that the low-energy photoelectrons display distinct CEP-dependent intercycle interference fringes, providing an alternative approach to retrieve the CEP with high sensitivity in a few-cycle laser field with low intensity.

Recent experiments on strong-field sequential double ionization (SDI) have reported several observations which are regarded as evidence of electron correlation, querying the validity of the standard independent electron approximation for SDI. Here we theoretically study SDI with a classical ensemble model. The experimental results are well reproduced with this model. Back tracing of the ionization process shows that these results are ascribed to the subcycle ionization dynamics of the two electrons, not the evidences of the electron correlation in SDI. Thus, the previously reported observations are not enough to claim the breakdown of the independent electron approximation in SDI.

The partition of the photon energy into the subsystems of molecules determines many photon-induced chemical and physical dynamics in laser-molecule interactions. The electron-nuclear energy sharing from multiphoton ionization of molecules has been used to uncover the correlated dynamics of the electron and fragments. However, most previous studies focus on symmetric molecules. Here we study the electron-nuclear energy sharing in strong-field photoionization of HeH 2+ by solving the one-dimensional time-dependent Schrödinger equation (TDSE). Compared with symmetric molecules, the joint electron-nuclear energy spectrum (JES) of HeH 2+ reveals an anomalous energy shift at certain nuclear energies, while it disappears at higher and lower nuclear energies. Through tracing the time evolution of the wavepacket of bound states, we identify that this energy shift originates from the joint effect of the Stark shift, associated with the permanent dipole, and the Autler-Townes effect due to the coupling of the 2pσ and 2sσ states in strong fields. The energy shift in the JES appears at certain nuclear distances only when both Stark effect and Autler-Townes effect play important roles. We further demonstrate that the electron-nuclei energy sharing can be controlled by varying laser intensity for asymmetric molecules, providing alternative approaches to manipulate photochemical reactions for more complex molecules.

Using semiclassical models with implementing interference effects, we study the low-energy photoelectron intra-half-cycle interferences among nonscattering trajectories and multiple forward scattering trajectories of atoms ionized by a strong mid-infrared laser field. Tracing back to the initial tunneling coordinates, we find that up to three kinds of forward scattering trajectories have substantial contributions to the low-energy photoelectrons. Those multiple forward scattering trajectories depend sensitively on the initial transverse momentum at the tunnel exit and they lead to sign reversal of the transverse momentum of the electrons. We show that the interference of the nonscattering trajectory and the triple-scattered trajectory has the largest contribution to the low-energy structure in mid-infrared laser fields. It is also shown that the long-range Coulomb potential has a significant effect on the low-energy photoelectron interference patterns.

Backscattering photoelectron hologram (BPH) originating from direct and backward-rescattering electrons encodes important structural information and ultrafast dynamics of the underlying processes. However, the BPH is usually overshadowed by other interference structures in the photoelectrons momentum spectra, preventing a direct extraction of information using BPH. Here we theoretically demonstrate disentanglement of the BPH from other types of interference with the orthogonal two-color field, where a weak orthogonal component is used to streak the BPH. By carefully adjusting the relative phase of the two-color field, the BPH is effectively separated from other interferences in the photoelectron momentum spectra and thus the BPH is unambiguously identified. This takes a significant step to time-resolved imaging of the attosecond dynamics with strong-field photoelectron holography.

The combination of thin layer chromatography (TLC) and mass spectrometry (MS) has been studied for decades, but for most cases MS detection is done after TLC separation is finished. Here, an online simultaneous TLC-MS analysis system, liquid thin layer chromatography-mass spectrometry (LTLC-MS), is developed which successfully synchronize TLC separation process and MS detection process like GC-MS and HPLC-MS do. And there's no need to use specially designed TLC, just regular TLC plates are enough. LTLC-MS method is composed of a newly developed ambient ionization method, glow discharge-matrix assisted infrared desorption ionization (GD-MAIRDI), and forced-flow TLC (FFTLC) technique, which guarantees the MS detection process does not disturb the TLC separation process throughout the whole analysis. The whole LTLC-MS analysis only need two steps and less than 15min. Mixtures as well as the two main components of a pain relief pills have been successfully analyzed by LTLC-MS. This proof of concept study opens up new possibilities of combining TLC with MS, and will further broaden the application abilities of TLC., (Copyright © 2016 Elsevier B.V. All rights reserved.)

We revisit the concept of near-forward rescattering strong-field photoelectron holography introduced by Y. Huismans et al. [Science 331, 61 (2011)]. The recently developed adiabatic theory is used to show how the phase of the scattering amplitude for near-forward rescattering of an ionized electron by the parent ion is encoded in and can be read out from the corresponding interference pattern in photoelectron momentum distributions (PEMDs) produced in the ionization of atoms and molecules by intense laser pulses. A procedure to extract the phase is proposed. Its application to PEMDs obtained by solving the time-dependent Schrödinger equation for a model atom yields results in good agreement with scattering calculations. This establishes a novel general approach to extracting structural information from strong-field observables capable of providing time-resolved imaging of ultrafast processes.

With the classical ensemble model, we have investigated the pulse-duration dependence of nonsequential double ionization (NSDI) over a wide range of laser intensity. The correlated electron momentum distributions are distinctly different for the few-cycle and multiple cycle pulses, which agree well with the previous experiments. Based on this agreement, we analyzed the underlying process for the pulse-duration dependence of the electron correlation by tracing the classical trajectories. Counterintuitively, our analysis shows that the recollision-induced excited states of NSDI could resist ionization in the strong laser field for a time much longer than one optical cycle even at very high intensities. For the multiple-cycle pulses, NSDI events with such a long time delay have significant contribution to the total NSDI yields, which is responsible for the pulse-duration dependence of the observed correlated patterns in the electron momentum distributions.

Using a fully classical model, we have studied sequential double ionization (SDI) of argon driven by elliptically polarized laser pulses at intensities well in the over-barrier ionization region. The results show that ion momentum distributions evolve from the two-band structure to the four-band, six-band structure and finally to the previously obtained four-band structure as the pulse duration increases. Our analysis shows that the evolution of these band structures originates from the pulse-duration-dependent multiple ionization bursts of the second electron. These band structures unambiguously indicate the subcycle electron emission in SDI.

Molecular ions are generated in induced electrospray ionization, and they can be transported to grounded ambient surfaces in the form of charged microdroplets. Efficient amide bonds formation between amines and carboxylic acids were observed inside charged droplets during transfer to the surface. Biomolecules derivatized using this method were self-assembled on a bare gold surface via Au-S bonds under the charged microdroplet environment. Cyclic voltammetric analysis of the self-assembled molecular film showed accelerated protein derivatization with cysteine, which allowed the covalent immobilization of the protein to the gold surface. Cytochrome C-functionalized electrodes prepared using the induced dual nanoelectrospray process showed bioactivity toward aqueous solutions of hydrogen peroxide below 50 μM. In effect, we have developed a method that allows derivatization of biomolecules and their immobilization at ambient surfaces in a single experimental step.

Better sensitivity and interface of ambient sampling/ionization mass spectrometry remain a challenge. Herein, a novel, plasma-based, ambient sampling/ionization/transmission (PASIT) integrated source in a pin-to-funnel configuration was developed for the sensitive analysis of complex samples. With the funnel sleeve directly affected by direct-current discharge plasma, PASIT combines the ability to sample/ionize analyte molecules and then efficiently collect/transport charged mass species under atmospheric pressure and consequently shows an improved sensitivity. The integrated source enhances the signal intensity by more than 2 orders of magnitude compared with the previous pin-to-plate plasma source without significant background addition. A surface limit of detection (LOD) of 130 fmol mm-(2) (S/N = 3) has been achieved for clenbuterol on filter paper with an argon carrier gas. Demonstrated applications include the direct determination of active ingredients from drugs and symbolic compounds from natural plants and cholesterol from mouse brain tissue sections.

Double ionization of neon with orthogonally polarized two-color (OTC) laser fields is investigated using coincidence momentum imaging. We show that the two-electron emission dynamics in nonsequential double ionization can be controlled by tuning the subcycle shape of the electric field of the OTC pulses. We demonstrate experimentally switching from correlated to anticorrelated two-electron emission, and control over the directionality of the two-electron emission. Simulations based on a semiclassical trajectory model qualitatively explain the experimental results by a subcycle dependence of the electron recollision time on the OTC field shape.

The multielectron dynamics in nonsequential triple ionization (NSTI) of neon atoms driven by mid-infrared (MIR) laser pulses is investigated with the three-dimensional classical ensemble model. In consistent with the experimental result, our numerical result shows that in the MIR regime, the triply charged ion longitudinal momentum spectrum exhibits a pronounced double-hump structure at low laser intensity. Back analysis reveals that as the intensity increases, the responsible triple ionization channels transform from direct (e, 3e) channel to the various mixed channels. This transformation of the NSTI channels leads to the results that the shape of ion momentum spectra becomes narrow and the distinct maxima shift towards low momenta with the increase of the laser intensity. By tracing the triply ionized trajectories, the various ionization channels at different laser intensities are clearly identified and these results provide an insight into the complex dynamics of the correlated three electrons in NSTI.

Accurate mass information is of great importance in the determination of unknown compounds. An effective and easy-to-control internal mass calibration method will dramatically benefit accurate mass measurement. Here we reported a simple induced dual-nanospray internal calibration device which has the following three advantages: (1) the two sprayers are in the same alternating current field; thus both reference ions and sample ions can be simultaneously generated and recorded. (2) It is very simple and can be easily assembled. Just two metal tubes, two nanosprayers, and an alternating current power supply are included. (3)With the low-flow-rate character and the versatility of nanoESI, this calibration method is capable of calibrating various samples, even untreated complex samples such as urine and other biological samples with small sample volumes. The calibration errors are around 1 ppm in positive ion mode and 3 ppm in negative ion mode with good repeatability. This new internal calibration method opens up new possibilities in the determination of unknown compounds, and it has great potential for the broad applications in biological and chemical analysis.

Using the classical ensemble method, we have investigated double ionization (DI) of diatomic molecules driven by circularly polarized laser pulses with different internuclear distances (R). The results show that the DI mechanism changes from sequential double ionization (SDI) to nonsequential double ionization (NSDI) as the internuclear distance increases. In SDI range, the structure of the electron momentum distribution changes seriously as R increases, which indicates the sensitive dependence of the release times of the two electrons on R. For NSDI, because of the circular polarization, the ionization of the second electron is not through the well-known recollision process but through a process where the first electron ionizes over the inner potential barrier of the molecule, moves directly towards the other nucleus, and kicks out the second electron.

Chinese liquors are often a very important part of social event in China. Driven by high profit, some illegal traders often use inferior liquors instead of the products with high quality to cheat the customer. Therefore, it is highly required to authenticate Chinese liquors. In this paper a novel method based on ambient glow discharge ionization mass spectrometry has been developed to differentiate Chinese liquors. Volatile components from liquor samples were ionized by the plasma generated by glow discharge and then detected by a commercial linear ion trap mass spectrometer. Consequently, the fingerprint mass spectra of several Chinese liquors were obtained. Combined with principal component analysis, this new method was successfully applied to differentiate different brands of Chinese liquors without any sample pretreatment. Compared with conventional methods, this novel method has the advantages of easy operation, high speed, and high efficiency, which make it a potential tool in the fields of food safety, atmosphere chemistry.

With the three-dimensional classical ensemble model, we investigate the correlated electron emission in nonsequential double ionization (NSDI) of argon atoms by few-cycle laser pulses. Our calculations well reproduce the experimentally observed cross-shaped structure in the correlated two-electron momentum spectrum [ Nature Commun. 3, 813 (2012)]. By tracing these NSDI trajectories, we find that besides the process of recollision-induced excitation with subsequent ionization just before the next field maximum, the recollision ionization also significantly contributes to the cross-shaped structure.

With the development of material science and the practical needs of the polymer industry, rapid characterization of synthetic polymers using mass spectrometry is of sustainable interest. Herein a new method for characterizing synthetic polymers using thermal-assisted atmospheric pressure glow discharge mass spectrometry (TA-APGD-MS) is established. After illustration of the mechanism of ion formation, typical polymer samples such as polystyrene (PS), polyoxymethylene (POM) and poly (butanediol succinate) (PBS) were directly characterized at the molecular level using TA-APGD-MS. The thermal degradation products of synthetic polymers including monomer units and/or other fragments were rapidly detected by tandem mass spectrometry, providing rich information about the chemical composition for the structural characterization of homo- and co-polymers. The result suggests that TA-APGD-MS allows direct and rapid analysis of both synthetic homo-polymers and co-polymers under ambient conditions without any sample pretreatment. This method features high throughput, high sensitivity and rich information, showing promising applications in polymer science.

We theoretically investigated sequential double ionization (SDI) of Ar by the nearly circularly polarized laser pulses with a fully correlated classical ensemble model. The ion momentum distributions of our numerical results at various laser intensities and pulse durations agree well with the experimental results. The experimentally observed multi-electron effects embodied in the joint momentum spectrum of the two electrons is also reproduced by our correlated classical calculations. Interestingly, our calculations show that the angular distribution of the first photoelectron from the trajectories which eventually suffer SDI differs from the distribution of the photoelectrons from above-threshold ionization trajectories. This observation provides additional evidence of multi-electron effects in strong field SDI.

The electron dynamics in strong field nonsequential double ionization (NSDI) of nitrogen molecules by mid-infrared (MIR) laser pulses is investigated with the three-dimensional classical ensemble model. The numerical results show that in the MIR regime, the correlated behavior of the two electrons from NSDI is independent on the molecular alignment, contrary to the case in the near-infrared (NIR) regime where the electron correlations exhibit a strong alignment dependence. In consistent with the experimental results, our numerical results show that the longitudinal momentum spectrum of the doubly charged ion evolves from a wide single-hump structure at NIR regime into a double-hump structure when wavelength enters the MIR regime. This double-hump structure becomes more pronounced as the wavelength further increases. The responsible microscopic electron dynamics of NSDI at the MIR regime is explored by back analysis of the classical trajectories.