Anti-Stokes-enhanced tunnelling ionization of polar molecules

Kornev, A. S.; Zon, B. A.

doi:10.1088/1054-660x/24/11/115302

Cited by 11 publications

(22 citation statements)

References 72 publications

(194 reference statements)

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“…Alternatively, based on the MO-ADK model, Zon et al proposed an anti-stokes-enhanced tunneling ionization (ASETI) method to investigate the effect of vibrational motion on the strong field ionization of molecules. [27][28][29] In their method, the Dyson orbital wavefunctions including nuclear motion are used as the molecular wavefunctions, and the ionization rate of molecules in the TI regime is described by the combination of the Frank-Condon factors between the neutral and ionic electronic states and the ADK ionization rate, which is dependent on the ionization potential. [27][28][29] According to this ASETI model, we can qualitatively understand the experimental observation in Fig.…”

Section: Discussionmentioning

confidence: 99%

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

Zuo¹,

Lv²,

Liang³

et al. 2018

Chinese Phys. B

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By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide (CS 2 ) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 10 12 W/cm 2 -1.5 × 10 14 W/cm 2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS 2 molecules. The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS 2 , as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank-Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strongfield ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.

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Section: Discussionmentioning

confidence: 99%

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

Zuo¹,

Lv²,

Liang³

et al. 2018

Chinese Phys. B

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“…According to our calculations, the initial population ratio in the X 2 Σ + and A 2 Π states of CO + is about 100:1. The ionization probability of removing one electron from HOMO (σ symmetry) of CO is maximal when the molecular axis is parallel to the laser field, while removing one electron from HOMO-1(π symmetry) of CO the ionization probability is maximal when the molecule axis perpendicular to the polarization of the laser field [13,14]. For the dissociation process, we numerically solved the time dependent Schrödinger equation (for details of the model please see Ref [7].).…”

Section: Numerical Simulations and Discussionmentioning

confidence: 99%

“…For the single ionization of a molecule, as described by the strong-field approximation [8] or molecular orbital Ammosov-Delone-Krainov theories [9,10], and numerically simulated by solving the timedependent Schrödinger equation [11,12], electrons are favored to be freed by the laser field pointing along the maximal density distributions of the ionizing orbital, i.e. selective ionization of molecule with a given spatial orientation correlated to the orbital profile [13,14]. Although most of the models are based on the single-active-electron approximation by assuming tunneling ionization from the highest occupied molecular orbital (HOMO) [12], for a molecule with multiple electrons, e.g.…”

Section: Introductionmentioning

confidence: 99%

Orientation-dependent strong-field dissociative single ionization of CO

Song

et al. 2017

Opt. Express

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The dissociative ionization of CO in orthogonally polarized femtosecond laser pulses are studied in a pump-probe scheme. The ionization of CO by the pump pulse and the dissociation of the created CO⁺ by the probe pulse can be fully disentangled by identifying the photoelectron momentum distributions. Different from the dissociative ionization by a single pulse in which the CO molecule mostly breaks along the field polarization, in this pump-probe strategy, the CO⁺ ion created from ionization by the pump pulse is favored to dissociate when it orients orthogonal to the polarization direction of the probe pulse. It is attributed to the laser-coupling of various electronic states of the molecular ion in the dissociation process, supported by the numerical simulation of a modeled time-dependent Schrödinger equation.

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“…The x2dhf program was also used by Grabo and Gross for optimized effective potential calculations within the KLI approximation, 596,597 by Karasiev and coworkers for density functional development, [598][599][600][601][602][603][604][605][606] by Halkier and Coriani for computing molecular electric quadrupole moments, 607 Roy and Thakkar who studied MacLaurin expansions of the electron momentum density for 78 diatomic molecules, 608 Weigend, Furche, and Ahlrichs for studying total energy and atomization energy basis set errors in quadruple-ζ basis sets, 609 Shahbazian and Zahedi who studied basis set convergence patterns, 610 Pruneda, Artacho, and Kuzmin for the calculation of range parameters, [611][612][613] Madsen and Madsen for modeling high-harmonic generation, 614 Williams et al who reported numerical HF energies for transition metal diatomics, 615 Madsen and coworkers who calculated structure factors for tunneling, [616][617][618][619] Kornev and Zon who studied anti-Stokes-enhanced tunneling ionization of polar molecules, 620 and Endo and coworkers who studied laser tunneling ionization of NO. 621 Based on the results of Laaksonen et al, Kolb and coworkers developed a FEM program for HF and density functional calculations employing triangular basis functions, again in the (µ, ν) coordinate system.…”

Section: Diatomic Moleculesmentioning

confidence: 99%

A review on non‐relativistic, fully numerical electronic structure calculations on atoms and diatomic molecules

Lehtola

2019

Int J of Quantum Chemistry

102

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The need for accurate calculations on atoms and diatomic molecules is motivated by the opportunities and challenges of such studies. The most commonly used approach for all-electron electronic structure calculations in general-the linear combination of atomic orbitals (LCAO) method-is discussed in combination with Gaussian, Slater a.k.a. exponential, and numerical radial functions. Even though LCAO calculations have major benefits, their shortcomings motivate the need for fully numerical approaches based on, for example, finite differences, finite elements, or the discrete variable representation, which are also briefly introduced. Applications of fully numerical approaches for general molecules are briefly reviewed, and their challenges are discussed. It is pointed out that the high level of symmetry present in atoms and diatomic molecules can be exploited to fashion more efficient fully numerical approaches for these special cases, after which it is possible to routinely perform allelectron Hartree-Fock and density functional calculations directly at the basis set limit on such systems. Applications of fully numerical approaches to calculations on atoms as well as diatomic molecules are reviewed. Finally, a summary and outlook is given.atomic calculations, density functional theory, diatomic calculations, fully numerical electronic structure theory, Hartree-Fock | INTRODUCTIONThanks to decades of development in approximate density functionals and numerical algorithms, density functional theory [1,2] (DFT) is now one of the cornerstones of computational chemistry and solid-state physics. [3][4][5] Since atoms are the basic building block of molecules, a number of popular density functionals [6][7][8][9][10] have been parametrized using ab initio data on noble gas atoms; these functionals have been used in turn as the starting point for the development of other functionals. A comparison of the results of density-functional calculations to accurate ab initio data on atoms has, however, recently sparked controversy on the accuracy of a number of recently published, commonly used density functionals. [11][12][13][14][15][16][17][18][19][20][21] This underlines that there is still room for improvement in DFT even for the relatively simple case of atomic studies.The development and characterization of new density functionals require the ability to perform accurate atomic calculations. Because atoms are the simplest chemical systems, atomic calculations may seem simple; however, they are in fact sometimes surprisingly challenging. For instance, a long-standing discrepancy between the theoretical and experimental electron affinity and ionization potential of gold has been resolved only very recently with high-level ab initio calculations. [22] Atomic calculations can also be used to formulate efficient starting guesses for molecular electronic structure calculations via either the atomic density [23,24] or the atomic potential as discussed in Ref. [25].

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Anti-Stokes-enhanced tunnelling ionization of polar molecules

Cited by 11 publications

References 72 publications

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

Orientation-dependent strong-field dissociative single ionization of CO

A review on non‐relativistic, fully numerical electronic structure calculations on atoms and diatomic molecules

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