Tunneling Ionization Research Articles

Quantum Chemical Analysis of the Molecular and Fragment Ion Formation of Butyrophenone by High-Electric Field Tunnel Ionization at Atmospheric Pressure.

The molecular ion M+· was observed when the liquid sample of butyrophenone was supplied using atmospheric pressure corona discharge (APCD). In contrast, the vapor supply resulted in the formation of the protonated molecule [M+H]+. The mass spectrum obtained with the liquid supply showed two distinctive fragment ions at m/z 105 and 120, resulting from α-cleavage and McLafferty rearrangement (McLR), respectively. The APCD spectrum showed peaks of M+· and the characteristic two fragment ions that were the same as the field ionization mass spectra of butyrophenone as reported by Chait et al. and Beckey et al. The formation of the molecular and fragment ions strongly indicated that high-electric field tunnel ionization (HEFTI) occurs by the HEF strength exceeding 108 V/m at the tip of the corona needle in APCD. The charge and spin density distributions of the molecular and fragment ions were analyzed by quantum chemical calculations using time-dependent density functional theory (TDDFT) and natural bond orbital (NBO) analysis.

Inline UV pulse synthesizer

We demonstrated an inline synthesizer for generating ultrashort pulses in the ultraviolet (UV) range. The inline UV pulse synthesizer comprised three nonlinear crystals located in the propagation path of the fundamental driving laser pulse. Second-harmonic signals with central wavelengths of 420, 375, and 345 nm were generated in turn in the three BBO crystals, resulting in a synthesized UV pulse subsequent to the final nonlinear crystal. Its temporal amplitude and phase could be manipulated easily by changing the relative positions of the crystals, allowing for flexibility of the waveform. The minimum pulse duration of the synthesized UV pulse was 4.7 fs, which was close to the Fourier-transform-limited pulse duration. This ultrashort UV pulse with 19 μ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\upmu$$\\end{document}J energy can be utilized in various applications such as high harmonic generation and frustrated tunneling ionization.

Femtosecond laser-induced damage threshold incubation in SrTiO3 thin films

This study delved into the microfabrication process on SrTiO3 thin films using femtosecond laser pulses, focusing on characterizing ablation behavior and elucidating on incubation parameters. A combination of microscopy techniques and systematic analysis of laser-material interactions provided insights into the features and fundamental processes governing the laser-induced modification of SrTiO3 thin films. The cutting profile morphology indicated high-resolution material removal, with line widths ranging from 0.6 to 1.6 µm, depending on number of pulses and energy. The study revealed a low incubation parameter for SrTiO3 thin films, quantified as (0.03 ± 0.01), indicating that a considerable number of pulses is required to cause damage to the material. Additionally, threshold energies for damage were determined to be 17.9 nJ for 20,000 pulses and 35.2 nJ for a single pulse. AFM analysis showed that the depth of the micromachined lines increased from approximately 80 nm to 315 nm with higher pulse energies, confirming substantial material removal. The Keldysh parameter provides insights into ionization mechanisms under femtosecond-laser irradiation, highlighting the dominance of tunneling ionization. Using higher pulse energies, the center of the microstructures exhibited significantly reduced Raman signals, correlating with substantial material removal, which was confirmed by atomic force microscopy. EDS analyses indicated that the elemental composition of the irradiated regions closely resembled the stoichiometric composition of SrTiO3, while the center of the microstructures showed significant oxygen levels but lacked titanium and strontium, consistent with the findings from AFM and Raman microscopy.

Multiphoton Resonance Meets Tunneling Ionization: High-Efficient Photoexcitation in Strong-Field-Dressed Ions.

Tunneling ionization, a fascinating quantum phenomenon, has played the key role in the development of attosecond physics. Upon absorption of a few tens of photons, tunneling ionization creates ions in different excited states and even enables the formation of population inversion between ionic states. However, the underlying physics is still being debated. Here, we demonstrate a significant enhancement in the efficiency of multiphoton excitation when ionization of neutral molecules and resonant excitation of ions coexist in strong laser fields. It facilitates the dramatic increase in population inversion and lasing radiation in N_{2}^{+} around 1000nm pump wavelength. Utilizing the ionization-coupling theory, we discover that the synergistic interplay between tunneling ionization and multiphoton excitation enables the ionic coherence to be maximized by phase locking of the periodically created ionic dipoles and consistently maintain an optimal phase for the follow-up photoexcitation. This Letter provides new insights into the photoexcitation mechanism of ions in strong laser fields and opens up a route for optimizing ionic lasing radiations.

Extraction of Molecular-Frame Electron-Ion Differential Scattering Cross Sections Based on Elliptical Laser-Induced Electron Diffraction.

We extracted the molecular-frame elastic differential cross sections (MFDCSs) for electrons scattering from N_{2}^{+} based on elliptical laser-induced electron diffraction (ELIED), wherein the structural evolution is initialized by the same tunneling ionization and probed by incident angle-resolved laser-induced electron diffraction imaging. To establish ELIED, an intuitive interpretation of the ellipticity-dependent rescattering electron momentum distributions was first provided by analyzing the transverse momentum distribution. It was shown that the incident angle of the laser-induced returning electrons could be tuned within 20° by varying the ellipticity and handedness of the driving laser pulses. Accordingly, the incident angle-resolved DCSs of returning electrons for spherically symmetric targets (Xe^{+} and Ar^{+}) were successfully extracted as a proof-of-principle for ELIED. The MFDCSs for N_{2}^{+} were experimentally obtained at incident angles of 4° and 7°, which were well reproduced by the simulations. The ELIED approach is the only successful method so far for obtaining incident angle-resolved ionic MFDCS, which provides a new sensitive observable for the transient structure retrieval of N_{2}^{+}. Our results suggest that the ELIED has the potential to extract the structural tomographic information of polyatomic molecules with femtosecond and subangstrom spatiotemporal resolutions that can enable the visualization of the nuclear motions in complex chemical reactions as well as chiral recognition.

Characterizing strong-field tunneling ionization with a phase-dependent THz polarization spectrum

The terahertz radiation emitted by asymmetrically ionized wavepackets in two-color strong-field tunneling ionization is essential for detecting the system's associated electron dynamics and structural properties. We propose to characterize and control tunneling ionization using a phase-dependent terahertz polarization (PTP) spectrum, analyzed through a combination of the classical trajectory Monte Carlo method, an analytical model based on the virial theorem, and the rigorous solution of the time-dependent Schrödinger equation as a benchmark. Our results demonstrate that the PTP spectrum offers a high-precision measure of the Coulomb effect through the relative phase of the two-color laser. Comparisons of PTP results calculated using different methods suggest how the electron can be manipulated by controlling the relative phase and laser intensity. In particular, the PTP spectrum can be used to calibrate the relative phase and provides a convenient and robust reconstruction of the time-averaging of tunneling positions with high precision using the analytical model. These insights reveal that the PTP spectrum as a whole can be a new and useful tool for the all-optical characterization of ultrafast atomic and molecular ionization.

Laser Machining at High ∼PW/cm2 Intensity and High Throughput

Laser machining by ultra-short (sub-ps) pulses at high intensity offers high precision, high throughput in terms of area or volume per unit time, and flexibility to adapt processing protocols to different materials on the same workpiece. Here, we consider the challenge of optimization for high throughput: how to use the maximum available laser power and larger focal spots for larger ablation volumes by implementing a fast scan. This implies the use of high-intensity pulses approaching ∼PW/cm2 at the threshold where tunneling ionization starts to contribute to overall ionization. A custom laser micromachining setup was developed and built to enable high speed, large-area processing, and easy system reconfiguration for different tasks. The main components include the laser, stages, scanners, control system, and software. Machining of metals such as Cu, Al, or stainless steel and fused silica surfaces at high fluence and high exposure doses at high scan speeds up to 3 m/s were tested for the fluence scaling of ablation volume, which was found to be linear. The largest material removal rate was 10 mm3/min for Cu and 20 mm3/min for Al at the maximum power 80 W (25 J/cm2 per pulse). Modified surfaces are color-classified for their appearance, which is dependent on surface roughness and chemical modification. Such color-coding can be used as a feedback parameter for industrial process control.

Ionizing terahertz waves with 260 MV/cm from scalable optical rectification.

Terahertz (THz) waves, known as non-ionizing radiation owing to their low photon energies, can actually ionize atoms and molecules when a sufficiently large number of THz photons are concentrated in time and space. Here, we demonstrate the generation of ionizing, multicycle, 15-THz waves emitted from large-area lithium niobate crystals via phase-matched optical rectification of 150-terawatt laser pulses. A complete characterization of the generated THz waves in energy, pulse duration, and focal spot size shows that the field strength can reach up to 260 megavolts per centimeter. In particular, a single-shot THz interferometer is employed to measure the THz pulse duration and spectrum with complementary numerical simulations. Such intense THz pulses are irradiated onto various solid targets to demonstrate THz-induced tunneling ionization and plasma formation. This study also discusses the potential of nonperturbative THz-driven ionization in gases, which will open up new opportunities, including nonlinear and relativistic THz physics in plasma.

Relative strengths of sum and difference frequency generation in perturbative high harmonic wave mixing

High harmonic generation (HHG) modulated by a weak laser field allows the perturbative wave mixing process which involves sum and difference frequency generations (SFG and DFG). The relative strengths of SFG and DFG have been extensively discussed in the literature but are still ambiguous. Here we experimentally study the relative strengths between SFG and DFG channels by applying a frequency-offset second-harmonic perturbing laser field collinearly in a thin gaseous nonlinear medium. It shows that SFG is favored for low harmonic orders, but DFG dominates for high-energy photons, when only short trajectories of high harmonics are considered. A semi-classical model incorporating both modulations to the tunneling ionization and the electron propagation steps by the perturbing laser field for a train of attosecond pulses explains the experimental results.

Sub-cycle strong-field tunneling dynamics in solids

Tunneling ionization is a crucial process in the interaction between strong laser fields and matter which initiates numerous nonlinear phenomena including high-order harmonic generation, photoelectron holography, etc. Both adiabatic and nonadiabatic tunneling ionization are well understood in atomic systems. However, the tunneling dynamics in solids, especially nonadiabatic tunneling, has not yet been fully understood. Here, we study the sub-cycle resolved strong-field tunneling dynamics in solids via a complex saddle-point method. We compare the instantaneous momentum at the moment of tunneling and the tunneling distances over a range of Keldysh parameters. Our results demonstrate that for nonadiabatic tunneling, tunneling ionization away from Γ point is possible. When this happens the electron has a nonzero initial velocity when it emerges in the conduction band. Moreover, consistent with atomic tunneling, a reduced tunneling distance as compared to the quasi-static case is found. Our results provide remarkable insight into the basic physics governing the sub-cycle electron tunneling dynamics with significant implications for understanding subsequent strong-field nonlinear phenomena in solids.

Wigner versus Stark: Connecting quantum to classical in a tunnel ionization process

We present a framework designed to illustrate the dynamics of a quantum particle tunneling from a bound state into a continuum of states under the influence of an external field. We concentrate on the question of what is the best classical-level description of the escaping particle. A toy model is constructed and investigated through complementary numerical, analytical, and approximate solutions. Issues related to the location of the apparent exit from the “quantum tunnel” are addressed in the language of Wigner trajectories and discussed in relation to the other types of solutions.

Tunnelling of electrons via the neighboring atom

As compared to the intuitive process that the electron emits straight to the continuum from its parent ion, there is an alternative route that the electron may transfer to and be trapped by a neighboring ionic core before the eventual release. Here, we demonstrate that electron tunnelling via the neighboring atomic core is a pronounced process in light-induced tunnelling ionization of molecules by absorbing multiple near-infrared photons. We devised a site-resolved tunnelling experiment using an Ar-Kr+ ion as a prototype system to track the electron tunnelling dynamics from the Ar atom towards the neighboring Kr+ by monitoring its transverse momentum distribution, which is temporally captured into the resonant excited states of the Ar-Kr+ before its eventual releasing. The influence of the Coulomb potential of neighboring ionic cores promises new insights into the understanding and controlling of tunnelling dynamics in complex molecules or environment.

Envelope effect of Rydberg States Generation in Strong Laser Pulses

Rydberg atoms are important building blocks for quantum technologies, exploited to new applications in quantum computing, quantum communication and quantum sensing due to their unique tunable quantum properties.Besides the widely-used few-photon resonant excitation for the specific Rydberg state, multiple Rydberg states can be populated coherently and effciently through the frustrated tunneling ionization or the Coulomb potential recapture effect in strong laser field. The Rydberg states excitation in strong field provides an opportunity to realize the ultrafast quantum control on Rydberg atom and bridge the strong field physics and quantum information technology. <br>Using the Classical Trajectory Monte Carlo method and Qprop package to solve Time-Dependent increases with the parameter of the asymmetric laser envelope. Based on the Quantitative Rescattering theory, the calculated time-dependence of recapture rate is negatively related to the laser envelope and the residual laser interaction time, which is termed as envelope effect. Combined with the carrier-wave effect, an analytic formula is proposed to calculate the Rydberg states population:$Y(t) \propto W_0(t) \frac{t-\tau+c}{f(t)} \cos (\omega t+\phi)$ This results open the door to enhance the Rydberg states generation using the laser envelope control, benefiting the future quantum technology based on the Rydberg states generated in the strong laser field.(a) Laser electric fields with the same pulse duration τ = 10T<sub>0</sub> and different asymmetric parameters α. Black solid line, red dashed line and blue dashed-dotted line are for α = -0.6, 0, 0.6 respectively. (b) The yields of Rydberg states change with the asymmetric parameter under different laser pulse duration. Black solid line, red dashed line and blue dashed-dotted line are for τ = 1010T<sub>0</sub>, 1510T<sub>0</sub>, 2010T<sub>0</sub> respectively. Schrödinger Equation, we calculate the population of Rydberg states. Our results show that the population.

Time-resolved subcycle and intercycle interference influenced momentum shift in nonadiabatic tunnelling ionization

Momentum shift is an important sign of nonadiabatic tunnelling ionization process. To investigate the mechanism of momentum shift, we use the strong-field approximation theory to track the formation of ionization momentum spectra of hydrogen atom under the action of different laser pulses in the time domain. By observing the ionization momentum spectra of different structures over time, we find that the momentum shift is formed by the continuous interference and evolution of ionization signals. Meanwhile, we further analyze how subcycle and intercycle interference influence the formation of momentum shift. Before the duration is long enough for intercycle interference to emerge, momentum shift grows smoothly. Our findings reveal different intrinsic mechanisms for the formation of momentum shift in many-cycle and few-cycle laser pulses, showing that subcycle interference plays a dominant role in the former while intercycle interference is critical in the latter. This work lays the foundation for a deeper understanding of the nonadiabatic tunnelling process and makes the regulation of momentum shift possible.

Development of Method for Isotope Ratio by Resonant Pumping / Tunnel Ionization SNMS

Development of Method for Isotope Ratio by Resonant Pumping / Tunnel Ionization SNMS

Probing the electron motion in molecules using forward-scattering photoelectron holography.

Charge migration initiated by the coherent superposition of several electronic states is a basic process in intense laser-matter interactions. Observing this process on its intrinsic timescale is one of the central goals of attosecond science. Here, using forward-scattering photoelectron holography we theoretically demonstrate a scheme to probe the charge migration in molecules. In our scheme, by solving the time-dependent Schrödinger equation, the photoelectron momentum distributions (PEMDs) for strong-field tunneling ionization of the molecule are obtained. For a superposition state, it is shown that an intriguing shift of the holographic interference appears in the PEMDs, when the molecule is aligned perpendicularly to the linearly polarized laser field. With the quantum-orbit analysis, we demonstrate that this shift of the interference fringes is caused by the time evolution of the non-stationary superposition state. By analyzing the dependence of the shift on the final parallel momentum of the electrons, the relative phase and the expansion coefficient ratio of the two electronic states involved in the superposition state are determined accurately. Our study provides an efficient method for probing the charge migration in molecules. It will facilitate the application of the forward-scattering photoelectron holography to survey the electronic dynamics in more complex molecules.

The Role of Collision Ionization of K-Shell Ions in Nonequilibrium Plasmas Produced by the Action of Super Strong, Ultrashort PW-Class Laser Pulses on Micron-Scale Argon Clusters with Intensity up to 5 × 1021 W/cm2

The generation of highly charged ions in laser plasmas is usually associated with collisional ionization processes that occur in electron–ion collisions. An alternative ionization channel caused by tunnel ionization in an optical field is also capable of effectively producing highly charged ions with ionization potentials of several kiloelectronvolts when the laser intensity q > 1020 W/cm2. It is challenging to clearly distinguish the impacts of the optical field and collisional ionizations on the evolution of the charge state of a nonequilibrium plasma produced by the interaction of high-intensity, ultrashort PW-class laser pulses with dense matter. In the present work, it is shown that the answer to this question can be obtained in some cases by observing the X-ray spectral lines caused by the transition of an electron into the K-shell of highly charged ions. The time-dependent calculations of plasma kinetics show that this is possible, for example, if sufficiently small clusters targets with low-density background gas are irradiated. In the case of Ar plasma, the limit of the cluster radius was estimated to be R0 = 0.1 μm. The calculation results for argon ions were compared with the results of the experiment at the J-KAREN-P laser facility at QST-KPSI.

The Surprising Dynamics of the McLafferty Rearrangement.

We report femtosecond time-resolved measurements of the McLafferty rearrangement following the strong-field tunnel ionization of 2-pentanone, 4-methyl-2-pentanone, and 4,4-dimethyl-2-pentanone. The pump-probe-dependent yields of the McLafferty product ion are fit to a biexponential function with fast (∼100 fs) and slow (∼10 ps) time constants, the latter of which is faster for the latter two compounds. Following nearly instantaneous ionization, the fast time scale is associated with rotation of the molecule to a six-membered cyclic intermediate that facilitates transfer of the γ-hydrogen, while the ∼50-100 times longer time scale is associated with a π-bond rearrangement and bond cleavage between the α- and β-carbons to produce the enol cation. These experimental measurements are supported by ab initio molecular dynamics trajectories, which further confirm the time scale of this important stepwise reaction in mass spectrometry.

Analysis of the stability region of light bullets propagating in the tunnel ionization mode in dielectric

An analytical estimation of the parameters of light bullets formed in the region of anomalous group dispersion in dielectrics under conditions of tunneling photoionization has been carried out. A system of ordinary differential equations for the parameters of a laser pulse is obtained by the method of moments. A new analytical approximation is proposed for calculating the contribution of tunneling ionization. With the help of Lyapunov’s stability theory, a quasi-stationary solution of this system and conditions for a quasi-stable propagation regime are found.

Ionization rate in an elliptically polarized laser field with respect to momentum at the tunneling exit point for noble atoms

In this paper, we present a novel theoretical model analyzing tunneling ionization for noble atoms exposed to an elliptically polarized laser field. Employing a semiclassical ensemble approximation, the model assesses the impact of the dynamic Coulomb field and ionization potential. The integration of the Coulomb field effect notably aligns theoretical predictions with experimental data. The study underscores the pivotal role of ellipticity on the tunneling rate and affirms the model's applicability.