Tunneling Ionization Research Articles

Direct Visualization of Valence Electron Motion Using Strong-Field Photoelectron Holography.

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.

Matrix and element dependences of useful yield in Si and SiO2 matrices using laser-ionization sputtered neutral mass spectrometry

The element and/or material dependence of the useful yield in laser-ionization sputtered neutral mass spectrometry (SNMS) using a high-photon-flux laser was investigated. Useful yields obtained from Si, B, As, and O in Si and SiO2 matrices using both secondary ion mass spectrometry (SIMS) and SNMS were compared, and the possibility of the accurate analysis of impurities in multilayers was investigated in terms of tunnel ionization. The behavior of atoms released from the surface by ion bombardment was calculated, and it was considered that the flying speed of sputtered atoms depends on the mass and that this causes the elemental difference in the fractions of laser-irradiated atoms. In the case of SNMS, excluding O, whose ionization probability is considered to be much lower than for the other elements, the useful yields of Si, B, and As are within 1 order of magnitude in both the Si and SiO2 matrices, and the difference between the matrices for each element is within a factor of two. These differences are much smaller than in the result of SIMS. It was confirmed that the distribution of B in a SiO2/Si stacked layer can be analyzed more accurately by SNMS than by SIMS. SNMS with a high-photon-density laser is considered to be effective for the analysis of more than one element in multilayers.

Bound and continuum energy distributions of nuclear fragments resulting from tunneling ionization of molecules

Bound and continuum energy distributions of nuclear fragments resulting from tunneling ionization of molecules

Wiggler magnetic field assisted third harmonic generation in expanding clusters

A simple theoretical model is constructed to study the wiggler magnetic field assisted third harmonic generation of intense short pulse laser in a cluster in its expanding phase. The ponderomotive force of laser causes density perturbations in cluster electron density which couples with wiggler magnetic field to produce a nonlinear current that generates transverse third harmonic. An intense short pulse laser propagating through a gas embedded with atomic clusters, converts it into hot plasma balls via tunnel ionization. Initially, the electron plasma frequency inside the clusters ωpe > (with ω1 being the frequency of the laser). As the cluster expands under Coulomb force and hydrodynamic pressure, ωpe decreases to . At this time, there is resonant enhancement in the efficiency of the third harmonic generation. The efficiency of third harmonic generation is enhanced due to cluster plasmon resonance and by phase matching due to wiggler magnetic field. The effect of cluster size on the expansion rate is studied to observe that the clusters of different radii would expand differently. The impact of laser intensity and wiggler magnetic field on the efficiency of third harmonic generation is also explored.

Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

Structural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses. Here we use transform limited femtosecond pulses to distinguish the isomers using two methods. First, we probe doubly charged parent ions with circularly polarized light. We show that the yield of doubly charged ortho-xylene decreases while para-xylene increases over a range of laser intensities when the laser polarization is changed from linear to circular. Second, we probe high harmonic generation from randomly oriented isomer molecules subjected to an intense laser field. We show that the yield of high-order harmonics varies with the positioning of the methyl group in xylene isomers (ortho-, para- and meta-) and is due to differences in the strength of tunnel ionization and the overlap between the angular peaks of ionization and photo-recombination.

Disentangling Long Trajectory Contributions in Two-Colour High Harmonic Generation

This work investigates High Harmonic Generation (HHG) in gas targets, induced by intense two-colour driving fields. We compared classical trajectory Monte Carlo simulations based on a semiclassical model of strong field tunnel ionisation of helium to experimental HHG spectra, and investigated the relative contribution of long trajectories to low harmonic orders. This phenomenon can be found even when the experimental setup is chosen to suppress long trajectories and favour phase matching for short trajectories.

Robust generation of Fourier-synthesized laser fields and their estimation of the optical phase by using quantum control of molecular tunneling ionization

Intense (5.0 × 1012 W cm−2) nanosecond Fourier-synthesized laser fields consisting of fundamental, second-, third-, and fourth-harmonic light generated by an interferometer-free Fourier-synthesized laser field generator induce orientation-selective ionization based on directionally asymmetric molecular tunneling ionization (TI). The laser field generator ensures adjustment-free operation, high stability, and high reproducibility. Phase-sensitive, orientation-selective molecular TI provides a simple way to estimate the relative phase differences between the fundamental light and each harmonic by data-fitting analysis. This application of Fourier-synthesized laser fields will facilitate not only lightwave engineering but also the control of matter.

Tunneling exit characteristics from classical backpropagation of an ionized electron wave packet

We investigate tunneling ionization of a single active electron with a strong and short laser pulse, circularly polarized. With the recently proposed backpropagation method, we can compare different criteria for the tunnel exit as well as popular approximations in strong-field physics on the same footing. Thereby, we trace back discrepancies in the literature regarding the tunneling time to inconsistent tunneling exit criteria. The main source of error is the use of a static ionization potential, which is, however, time dependent for a short laser pulse. A vanishing velocity in the instantaneous field direction as tunneling exit criterion offers a consistent alternative, since it does not require the knowledge of the instantaneous binding energy. Finally, we propose a mapping technique that links observables from attoclock experiments to the intrinsic tunneling exit time.

Three-dimensional femtosecond laser processing for lab-on-a-chip applications

AbstractThe extremely high peak intensity associated with ultrashort pulse width of femtosecond laser allows us to induce nonlinear interaction such as multiphoton absorption and tunneling ionization with materials that are transparent to the laser wavelength. More importantly, focusing the femtosecond laser beam inside the transparent materials confines the nonlinear interaction only within the focal volume, enabling three-dimensional (3D) micro- and nanofabrication. This 3D capability offers three different schemes, which involve undeformative, subtractive, and additive processing. The undeformative processing preforms internal refractive index modification to construct optical microcomponents including optical waveguides. Subtractive processing can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. Additive processing represented by two-photon polymerization enables the fabrication of 3D polymer micro- and nanostructures for photonic and microfluidic devices. These different schemes can be integrated to realize more functional microdevices including lab-on-a-chip devices, which are miniaturized laboratories that can perform reaction, detection, analysis, separation, and synthesis of biochemical materials with high efficiency, high speed, high sensitivity, low reagent consumption, and low waste production. This review paper describes the principles and applications of femtosecond laser 3D micro- and nanofabrication for lab-on-a-chip applications. A hybrid technique that promises to enhance functionality of lab-on-a-chip devices is also introduced.

Publisher's Note: Two-photon vibrational excitation of air by long-wave infrared laser pulses [Phys. Rev. A 94 , 023816 (2016)

Received 11 January 2018DOI:https://doi.org/10.1103/PhysRevA.97.019904©2018 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasMultiphoton or tunneling ionization & excitationNonlinear opticsStrong field excitationUltrafast phenomenaUltrashort pulsesAtomic, Molecular & Optical

Strongly coupled stimulated Brillouin amplification in pump-ionizing plasma

Laser amplification based on strongly coupled stimulated Brillouin scattering in plasma is investigated. The pump and seed are at the same wavelength of 800 nm and the same duration of 3.5 ps, but with a different intensity. The plasma is produced by the front part of the pump via tunnel ionization from hydrogen. The hydrogen is fully ionized to eliminate small-scale density fluctuations in the plasma, so the transmission level of the seed is enhanced to 22%, and a relative amplification factor of 6 is obtained.

A single-electron picture based on the multiconfiguration time-dependent Hartree–Fock method: application to the anisotropic ionization and subsequent high-harmonic generation of the CO molecule

The mechanisms of anisotropic near-IR tunnel ionization and high-order harmonic generation (HHG) in a CO molecule are theoretically investigated by using the multiconfiguration time-dependent Hartree–Fock (MCTDHF) method developed for the simulation of multielectron dynamics of molecules. The multielectron dynamics obtained by numerically solving the equations of motion (EOMs) in the MCTDHF method is converted to a single orbital picture in the natural orbital representation where the first-order reduced density matrix is diagonalized. The ionization through each natural orbital is examined and the process of HHG is classified into different optical paths designated by a combinations of initial, intermediate and final natural orbitals. The EOMs for natural spin-orbitals are also derived within the framework of the MCTDHF, which maintains the first-order reduced density matrix to be a diagonal one throughout the time propagation of a many-electron wave function. The orbital dependent, time-dependent effective potentials that govern the dynamics of respective time-dependent natural orbitals are deduced from the derived EOMs, of which the temporal variation can be used to interpret the motion of the electron density associated with each natural spin-orbital. The roles of the orbital shape, multiorbital ionization, linear Stark effect and multielectron interaction in the ionization and HHG of a CO molecule are revealed by the effective potentials obtained. When the laser electric field points to the nucleus O from C, tunnel ionization from the C atom side is enhanced; a hump structure originating from multielectron interaction is then formed on the top of the field-induced distorted barrier of the HOMO effective potential. This hump formation, responsible for the directional anisotropy of tunnel ionization, restrains the influence of the linear Stark effect on the energy shifts of bound states.

Dynamics of tunneling ionization using Bohmian mechanics

Recent attoclock experiments and theoretical studies regarding the strong-field ionization of atoms by few-cycle infrared pulses revealed new features that have attracted much attention. Here we investigate tunneling ionization and the dynamics of the electron probability using Bohmian Mechanics. We consider a one-dimensional problem to illustrate the underlying mechanisms of the ionization process. It is revealed that in the major part of the below-the-barrier ionization regime, in an intense and short infrared pulse, the electron does not tunnel \through" the entire barrier, but rather already starts from the classically forbidden region. Moreover, we highlight the correspondence between the probability of locating the electron at a particular initial position and its asymptotic momentum. Bohmian Mechanics also provides a natural definition of mean tunneling time and exit position, taking account of the time dependence of the barrier. Finally, we find that the electron can exit the barrier with significant kinetic energy, thereby corroborating the results of a recent study [Camus et al., Phys. Rev. Lett. 119 (2017) 023201].

Angular momentum distribution in strong-field frustrated tunneling ionization

Using the classical-trajectory Monte Carlo model, we have theoretically studied the angular momentum distribution of frustrated tunneling ionization (FTI) of atoms in strong laser fields. Our results show that the angular momentum distribution of the FTI events exhibits a double-hump structure. With this classical model, we back traced the tunneling coordinates, i.e., the tunneling time and initial transverse momentum at tunneling ionization. It is shown that for the events tunneling ionized at the rising edge of the electric field, the final angular momentum exhibits a strong dependence on the initial transverse momentum at tunneling. While for the events ionized at the falling edge, there is a relatively harder recollision between the returning electron and the parent ion, leading to the angular momentum losing the correlation with the initial transverse momentum. Our study suggests that the angular momentum of the FTI events could be manipulated by controlling the initial coordinates of the tunneling ionization.

Quasiclassical theory of tunnel ionization of an atom by parallel electric and magnetic fields

Quasiclassical theory of tunnel ionization of an atom by parallel electric and magnetic fields

High harmonic generation at the tunneling ionization of atoms by intense laser radiation near the classical cut-off

The yield of spontaneous photons at the tunneling ionization of atoms by intense low-frequency laser radiation near the classical cut-off is estimated analytically by using the three-step model. The Bell-shaped dependence in the universal photon spectrum is explained qualitatively.

Carrier-envelope phase-dependent ionization of Xe in intense, ultrafast (two-cycle) laser fields

We report an experimental study that shows the dependence of the tunnel ionization of Xe by two-cycle, intense, near infrared light on the carrier-envelope-phase (CEP) of incident laser pulses. At low values of the optical field (E), the ionization yield is found to be maximum for cos-like pulses; the CEP dependence of the ion yield becomes stronger for higher charge states. At higher E-values, the CEP dependence either washes out or flips. A simple phenomenological model is used to confirm that our results fall within the ambit of the current understanding of ionization dynamics in strong, ultrashort optical fields. In the observed tunnel ionization of Xe, CEP effects appear to persist for longer, eight-cycle, pulses. Electron rescattering is observed to play a relatively unimportant role in the observed CEP dependence. These results provide fresh perspectives in the ionization mechanisms of multielectron systems in the few-cycle regime.

Quantum theory of strong-field frustrated tunneling

We show how the strong-field approximation, widely used for description of multiphoton and tunneling ionization, can be extended to analyse the excitation of bound states in intense low-frequency laser pulses. The proposed theory is based on the formalism of quantum trajectories and fills the gap between the numerical solution of the time-dependent Schrödinger equation and classical simulations. In particular, it allows identifying non-adiabatic and interference effects in strong-field excitation of Rydberg states.

Laser-induced deformation of triatomic molecules: Influence on tunnel ionization

We consider a type of light-dressing effect in molecules which is due to laser-induced deformation of molecules. We derive general formulas which describe the change of the equilibrium bond lengths, bending angles, and vibration frequencies for a polyatomic molecule. Up to the second-order terms in the field strength, the normal coordinates of the molecule are not changed. Explicit expressions for the change of the geometric parameters and vibration frequencies are found for a nonlinear triatomic molecule of the ${A}_{2}B$ type. These results are applied to calculation of the tunnel-ionization rates for ${\mathrm{H}}_{2}\mathrm{O}$, ${\mathrm{H}}_{2}{\mathrm{O}}^{+}$, and ${\mathrm{SO}}_{2}$ molecules, both in ac and dc fields. The main influence of the laser-induced deformation on the tunnel ionization is due to the changes in Franck-Condon factors, which are determined by overlap of the nuclei wave function of the molecule and its residual ion. In a laser field with an intensity of $\ensuremath{\sim}{10}^{14}\phantom{\rule{0.28em}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$, the contribution of the laser-dressing effect to the ionization rate is within 5% for ${\mathrm{H}}_{2}\mathrm{O}$ and ${\mathrm{H}}_{2}{\mathrm{O}}^{+}$, while accounting for this effect changes the ionization rate of the ${\mathrm{SO}}_{2}$ molecule by up to 20 times depending on the molecule's orientation with respect to the electric-field vector. Such a large difference is due to the electronic structures of these molecules.

The electron tunneling from fullerene molecule in a weak electric field

We derive equations describing the electron tunneling ionization of the molecular orbitals without symmetry. The modified method of smooth matching the asymptotic wave functions with molecule’s wave functions is suggested, to use the results of numerical calculations of the molecules in the GAUSSIAN. The spatial distribution of the current is considered for tunneling ionization the fullerene C60. We obtained the ionization probability of individual orbitals and spatial distribution of the electron currents at different values of the field, a distance to the screen and orientation of the fullerene.