High harmonic spectra contributed by HOMO-1 orbital of aligned CO_2 molecules

Li, Jiawei; Liu, Peng; Ye, Hua; Song, Liwei; Zhao, Shitong; Lu, Hui; Li, Ruxin; Xu, Zhizhan

doi:10.1364/oe.21.007599

Cited by 14 publications

(19 citation statements)

References 38 publications

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“…24 Analysis of HHG spectra of CO 2 + reveal contributions from ionization from lower lying orbitals. 16,22 Calculations by other groups also show that the σ u orbital contributes to ionization along the molecular axis and the π u orbital contributes to ionization perpendicular to the axis, 9,25,28 and that at higher intensities these contributions can become larger than from the π g orbital. 28 The angular dependence of the ionization of formaldehyde (Figure 4a−c) has a richer three-dimensional structure since it lacks the cylindrical symmetry of linear molecules in this study.…”

Section: The Journal Of Physical Chemistry Lettersmentioning

confidence: 95%

“…7,8 Molecular ADK theory has a sharp maximum at 25°, 7 but more careful application of MO-ADK 19 and more elaborate theories have broader maxima in the 30−45°range. 9,17,20,25,28 At higher E max , there is a large increase in the ionization rate along the molecular axis. This is indicative of ionization to the B 2 Σ u state of CO 2 + and the Dyson orbital corresponds to the σ u orbital involving the oxygen lone pairs, Figure 3f.…”

Section: The Journal Of Physical Chemistry Lettersmentioning

confidence: 99%

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Angle-Dependent Ionization of Small Molecules by Time-Dependent Configuration Interaction and an Absorbing Potential

Krause

Schlegel

2015

J. Phys. Chem. Lett.

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The angle-dependence of strong field ionization of O2, N2, CO2, and CH2O has been studied theoretically using a time-dependent configuration interaction approach with a complex absorbing potential (TDCIS-CAP). Calculation of the ionization yields as a function of the direction of polarization of the laser pulse produces three-dimensional surfaces of the angle-dependent ionization probability. These three-dimensional shapes and their variation with laser intensity can be interpreted in terms of ionization from the highest occupied molecular orbital (HOMO) and lower lying orbitals, and the Dyson orbitals for the ground and excited states of the cations.

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Section: The Journal Of Physical Chemistry Lettersmentioning

confidence: 95%

Section: The Journal Of Physical Chemistry Lettersmentioning

confidence: 99%

Angle-Dependent Ionization of Small Molecules by Time-Dependent Configuration Interaction and an Absorbing Potential

Krause

Schlegel

2015

J. Phys. Chem. Lett.

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“…The interference effect between the harmonics generated from different MOs was found to be responsible for the interference minimum shifting with the laser intensity [6]. Generally, the harmonics generated from lower-lying MOs are observed in the special directions [8] or beyond the cutoff of the HOMO spectra [6]. Hence, tomographic reconstruction of the lower-lying MOs by those harmonics is difficult.…”

Section: Introductionmentioning

confidence: 99%

Intensity-dependent multiorbital effect in high-order harmonics generated from aligned O2molecules

Zhang

et al. 2013

Phys. Rev. A

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High-order harmonics generated from multiple orbitals of aligned O 2 molecules are studied theoretically and we focus on the effect of two-center interference during photoexcitation. We find that the contribution of the harmonics generated from different molecular orbitals to the total harmonics varies distinctively with the laser intensity. The total harmonic spectra are dominated by the harmonics generated from a 1π g valence shell at lower intensities, but are dominated by those generated from a 1π u valence shell at higher intensities. This change is a sequence of the structure-induced two-center interference during photoexcitation of harmonic generation. This study indicates that by properly choosing the intensity of driving laser pulses, one can extract the orbital information of both the 1π g and the 1π u valence shells by the generated harmonics. This provides a potential way to tomographically reconstruct the low-lying 1π u valence shell.

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“…However, HHG spectra can also have contributions from direct ionization of lower lying orbitals if the intensity is high enough. [12][13][14][15][16][17] Earlier work also showed that an intense laser pulse can cause nonresonant multiphoton ionization of inner-valence electrons. 18,19 A qualitative description of the angular dependence of ionization for simple molecules can be obtained from Dyson orbitals.…”

Section: Introductionmentioning

confidence: 99%

Angle-dependent strong-field ionization of triple bonded systems calculated by time-dependent configuration interaction with an absorbing potential

Liao

Schlegel

2016

Can. J. Chem.

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The angle dependence of strong field ionization has been studied for a set of molecules containing triple bonds: HCCH, HCN, HCC–CN, H2N–CCH, H2N–CN, and H2N–CC–CN. Time-dependent configuration interaction (TDCI) with a complex absorbing potential was used to model strong field ionization by a linearly polarized seven-cycle 800 nm cosine squared pulse. The ionization yields have been calculated as a function of the laser intensity and polarization direction and plotted as three-dimensional surfaces. At low field strengths, the angular dependence can be understood in terms of ionization from the highest occupied orbitals. At higher laser intensities, ionization occurs from lower lying orbitals as well as from the highest occupied orbitals, as indicated by changes in the angular dependence of the ionization yield and by variations in the population analysis of the TDCI wavefunction with the intensity of the laser field. The ionization yield for directions parallel to the molecular axis increases more rapidly than perpendicular to the axis as the conjugation length is increased. NH2 substitution substantially increases the ionization yield along the molecular axis but has only a small effect for perpendicular directions.

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High harmonic spectra contributed by HOMO-1 orbital of aligned CO_2 molecules

Cited by 14 publications

References 38 publications

Angle-Dependent Ionization of Small Molecules by Time-Dependent Configuration Interaction and an Absorbing Potential

Angle-Dependent Ionization of Small Molecules by Time-Dependent Configuration Interaction and an Absorbing Potential

Intensity-dependent multiorbital effect in high-order harmonics generated from aligned O2molecules

Angle-dependent strong-field ionization of triple bonded systems calculated by time-dependent configuration interaction with an absorbing potential

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