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Recollision processes are fundamental to strong-field physics and attoscience, thus models connecting recolliding trajectories to quantum amplitudes are a crucial part in furthering understanding of these processes. We report developments in the semiclassical path-integral-based Coulomb quantum-orbit strong-field approximation model for strong-field ionization by including an additional phase known as Maslov’s phase and implementing a new solution strategy via Monte-Carlo-style sampling of the initial momenta. In doing so, we obtain exceptional agreement with solutions to the time-dependent Schrödinger equation for hydrogen, helium, and argon. We provide an in-depth analysis of the resulting photoelectron momentum distributions for these targets, facilitated by the quantum-orbits arising from the solutions to the saddle-point equations. The analysis yields a new class of rescattered trajectories that includes the well-known laser-driven long and short trajectories, along with novel Coulomb-driven rescattered trajectories. By virtue of the precision of the model, it opens the door to detailed investigations of a plethora of strong-field phenomena such as photoelectron holography, laser-induced electron diffraction and high-order above threshold ionization.

Photoelectron momentum distributions from strong-field ionization of carbonyl sulfide with 800 nm central-wavelength laser pulses at various peak intensities from 4.6 to 13 × 1013 W cm−2 were recorded and analyzed regarding resonant Rydberg states and photoelectron orbital angular momentum. The evaluation of the differentials of the momentum distributions with respect to the peak intensity highly suppressed the impact of focal volume averaging and allowed for the unambiguous recognition of Freeman resonances. As a result, previously made assignments of photoelectron lines could be reassigned. An earlier reported empirical rule, which relates the initial state's orbital momentum and the minimum photon expense to ionize an ac Stark shifted atomic system to the observable dominant photoelectron orbital momentum, was confirmed for the molecular target.

The debate on tunnelling times have always been full of contradictions and the attoclock experiments that measure tunnelling delays in strong-field ionization are no exception. The current review presents the debate and discussions concerning the studies of tunnelling times based only on the attoclock technique. We review them with their implications and pitfalls identified due to lack of accurate strong field models that validate the observations in interpreting the measurements performed on noble gases. In order to provide a complete picture, the review begins with a background on some of the popular tunnelling time definitions, most of them conceived during the late 1980s debate, which are often cited in the attoclock literature. We then discuss various attoclock experiments on noble gas atoms and their interpretations in context of the tunneling time debate. The recently performed attoclock experiment and numerical modelling using atomic hydrogen are also presented as an attempt at resolving the controversy. We conclude with the current status of the debate.

Electrons in atoms and molecules can not respond immediately to the action of intense laser field. There is a time lag (about 100 attoseconds) between instants of the field maximum and the ionization-rate maximum. This lag characterizes the response time of the electronic wave function to a strong-field ionization event and has important effects on dynamics of the ionized electron. For polar molecules with a large permanent dipole, the direct measurement or calculation of the absolute time lag is difficult. Here, a calibrated attoclock procedure, which is related to a simple Coulomb-induced temporal correction to electron trajectories, is proposed to measure the relative time lag of two different ionization events. Using this procedure, the relative lag of polar molecules in two consecutive half laser cycles can be probed with high time resolution.

While field ionization (FI) and field desorption (FD) are established soft vacuum ionization methods in mass spectrometry (MS), the technique of atmospheric pressure field desorption (APFD) has only recently been added to the repertoire. Similar to FI and FD, APFD can yield both positive even-electron ions of highly polar or ionic compounds and positive molecular ions, M+•, e.g., of polycyclic aromatic compounds. Thus, a dedicated APFD source assembly has been constructed and demonstrated to allow for robust APFD operation. This device also enabled observation of the emitter during operation and allowed for resistive emitter heating, thereby speeding up the desorption of the analytes and expanding the range of analytes accessible to APFD. While initial work was done using a Fourier transform-ion cyclotron resonance (FT-ICR) mass spectrometer, the new APFD source offered the flexibility to also be used on a trapped ion mobility-quadrupole-time-of-flight (TIMS-Q-TOF) instrument, and thus, it would be possible to be mounted to any Bruker mass spectrometer featuring an atmospheric pressure (AP) interface. Operating an APFD source at a TIMS-Q-TOF instrument called for the exploration of the combined use of APFD and TIMS. Here, operation, basic properties, and capabilities of this new atmospheric pressure field desorption-trapped ion mobility-mass spectrometry (APFD-TIMS-MS) coupling are described. APFD-TIMS-MS is employed for the separation of individual components of oligomers and for the accurate determination of their collision cross section (CCS). This work describes the application of APFD-TIMS-MS on poly(ethylene glycol) forming [M + Na]+ ions by cationization and on an amine-terminated poly(propylene glycol) yielding [M + H]+ ions. Some compounds forming molecular ions, M+•, by field ionization such as [60]fullerene and a mixture of four polycyclic aromatic hydrocarbons (PAHs) are examined. In APFD-TIMS-MS, the limits of detection (LODs) of fluoranthene and benzo[a]pyrene M+• ions are determined as ≈100 pg and <1 pg, respectively. Finally, [60]fullerene is analyzed by negative-ion APFD-TIMS-MS where it yields a molecular anion, M−•.

Deep learning models have provided huge interpretation power for image-like data. Specifically, convolutional neural networks (CNNs) have demonstrated incredible acuity for tasks such as feature extraction or parameter estimation. Here we test CNNs on strong-field ionization photoelectron spectra, training on theoretical data sets to ‘invert’ experimental data. Pulse characterization is used as a ‘testing ground’, specifically we retrieve the laser intensity, where ‘traditional’ measurements typically lead to 20% uncertainty. We report on crucial data augmentation techniques required to successfully train on theoretical data and return consistent results from experiments, including accounting for detector saturation. The same procedure can be repeated to apply CNNs in a range of scenarios for strong-field ionization. Using a predictive uncertainty estimation, reliable laser intensity uncertainties of a few percent can be extracted, which are consistently lower than those given by traditional techniques. Using interpretability methods can reveal parts of the distribution that are most sensitive to laser intensity, which can be directly associated with holographic interferences. The CNNs employed provide an accurate and convenient ways to extract parameters, and represent a novel interpretational tool for strong-field ionization spectra.

We present an efficient numerical method to solve the time-dependent Schrödinger equation in the single-active electron picture for atoms interacting with intense optical laser fields. Our approach is based on a non-uniform radial grid with smoothly increasing steps for the electron distance from the residual ion. We study the accuracy and efficiency of the method, as well as its applicability to investigate strong-field ionization phenomena, the process of high-order harmonic generation, and the dynamics of highly excited Rydberg states.

We investigate the intensity- and species-dependent strong-field ionization of alkali metal atoms; sodium, potassium, rubidium and caesium; by intense, few-cycle laser pulses in the short-wave infrared (sw-IR) regime at 1800 nm. The low ionization potential, Ip, of these atoms allows us to scale the interaction and study the tunneling regime at sw-IR wavelengths using low intensities and pulse energies. Measurements of above-threshold ionization spectra in the alkali species exhibit distinct differences to rare gas spectra at 800 and 1800 nm. However, pairing the low ionization potential of these atoms with longer wavelengths results in the reemergence of some well-know features of nobel gas spectra in the visible, e.g., the plateau. Our focus lies on the comparison of high-energy rescattered electron yield among the different alkali species. The highly unfavorable plateau scaling known from rare gases at longer wavelengths is successfully circumvented by switching to low-Ip targets. In the investigated parameter range, we identify potassium as the most efficient rescatterer. In addition, this paves the way to a carrier-envelope phasemeter operating in the sw-IR/mid-wave IR regime, employing alkali metal atoms as a target.

Field ionization (FI), field desorption (FD), and liquid injection field desorption/ionization (LIFDI) provide soft positive ionization of gaseous (FI) or condensed phase analytes (FD and LIFDI). In contrast to the well-established positive-ion mode, negative-ion FI or FD have remained rare exceptions. LIFDI provides sample deposition under inert conditions, i.e., the exclusion of atmospheric oxygen and water. Thus, negative-ion LIFDI could potentially be applied to highly sensitive anionic compounds like catalytically active transition metal complexes. This work explores the potential of negative-ion mode using modern mass spectrometers in combination with an LIFDI source and presents first results of the application of negative-ion LIFDI-MS. Experiments were performed on two orthogonal-acceleration time-of-flight (oaTOF) instruments, a JEOL AccuTOF GCx and a Waters Micromass Q-TOF Premier equipped with LIFDI sources from Linden CMS. The examples presented include four ionic liquids (ILs), i.e., N-butyl-3-methylpyridinium dicyanamide, 1-butyl-3-methylimidazolium tricyanomethide, 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide, and trihexyl(tetradecyl)phosphonium tris(pentafluoroethyl)trifluorophosphate), 3-(trifluoromethyl)-phenol, dichloromethane, iodine, polyethylene glycol diacid, perfluorononanoic acid, anionic surfactants, a tetraphosphazene silanol-silanolate, and two bis(catecholato)silanes. Volatile samples were delivered as vapors via the sample transfer capillary of the LIFDI probe or via a reservoir inlet. Condensed phase samples were applied to the emitter as dilute solutions via the sample transfer capillary. The compounds either yielded ions corresponding to their intact anions, A−, or the [M–H]− species formed upon deprotonation. This study describes the instrumental setups and the operational parameters for robust operation along with a discussion of the negative-ion LIFDI spectra of a variety of compounds.

The validity of the adiabatic approximation in strong field ionization under typical experimental conditions has recently become a topic of great interest. Experimental results have been inconclusive, in part, due to the uncertainty in experimental calibration of intensity. Here we turn to the time-dependent Schrödinger equation, where all the laser parameters are known exactly. We find that the centre of the electron momentum distribution (typically used for calibration of elliptically and circularly polarized light) is sensitive to non-adiabatic effects, leading to intensity shifts in experimental data that can significantly affect the interpretation of results. On the other hand, the transverse momentum spread in the plane of polarization is relatively insensitive to such effects, even in the Keldysh parameter regime approaching γ 3 . This suggests the transverse momentum spread in the plane of polarization as a good alternative to the usual calibration method, particularly for experimental investigation of non-adiabatic effects using circularly polarized light.