Numerical Bound State Electron Dynamics of Carbon Dioxide in the Strong-Field Regime

Smith, Stanley M.; Romanov, Dmitri; Li, Xiaosong; Sonk, Jason A.; Schlegel, H. Bernhard; Levis, Robert J.

doi:10.1021/jp904549d

Cited by 9 publications

(9 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This switch is necessary since previous attempts at LPI using shorter wavelengths − or longer pulses only yield molecular ions when the laser power is reduced to near threshold, and the ionization efficiency is impractically low. The processes occurring during strong field ionization (SFI) are an area of ongoing spectroscopic and theoretical research, as they underpin the emerging field of attosecond electron dynamics. , Current understanding of SFI is based on the interplay of two distinct ionization regimes, described as adiabatic and nonadiabatic dynamics. ,− Molecular and laser properties affect the transition between them and the final outcome of each, be it intact ionization or heavy fragmentation.…”

Section: Introductionmentioning

confidence: 99%

Strong Field Ionization of β-Estradiol in the IR: Strategies To Optimize Molecular Postionization in Secondary Neutral Mass Spectrometry

2014

View full text Add to dashboard Cite

Strong field laser photoionization of β-estradiol in the 1013–1015 W/cm2 intensity range at wavelengths between 1200 and 2000 nm was examined for both evaporated gas phase molecules and neutral species sputtered from a solid surface under bombardment with 20 keV C60 + ions. It is shown that the ionization efficiency is saturated at laser intensities of the order of 1013 W/cm2, while laser-induced photofragmentation is found to strongly increase between 1013 and 1014 W/cm2 and stay constant at higher intensities. These findings suggest a strategy to improve the postionization efficiency by defocusing the laser beam in order to sample a larger fraction of the sputtered plume, while at the same time optimizing the conditions for intact photoionization of the sputtered molecules. The results reveal a substantial enhancement of the signal of intact postionized molecular ions to a level an order of magnitude above that of the corresponding secondary ions. They also provide an experimental estimate of ∼2.5 × 10–2 as an upper bound for the ion fraction (secondary ion formation probability) of the sputtered molecules.

show abstract

Section: Introductionmentioning

confidence: 99%

Strong Field Ionization of β-Estradiol in the IR: Strategies To Optimize Molecular Postionization in Secondary Neutral Mass Spectrometry

2014

View full text Add to dashboard Cite

show abstract

“…More importantly, when the external field is strong, neither RPA nor LR-TDDFT is sufficient to describe the interaction. Within this strong field regime, the realtime TDHF and TDKS propagations have been implemented in calculations of the multiphoton ionization, 23,29,30,50 the high-order harmonic generation (HHG), 51-55 and the above threshold ionization (ATI), 56 Within the perturbative limit, the gauge behavior of TDHF/TDKS has been mathematically evaluated. 13,57,58 However, gauge behaviors of TDHF/TDKS in the perturbative regime cannot be simply or accurately extrapolated into the real-time dynamics in the nonperturbative regime.…”

Section: Introductionmentioning

confidence: 99%

On the gauge invariance of nonperturbative electronic dynamics using the time-dependent Hartree-Fock and time-dependent Kohn-Sham

Ding

Liang

Chapman

et al. 2011

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

Nonperturbative electronic dynamics using the time-dependent Hartree-Fock (TDHF) and time-dependent Kohn-Sham (TDKS) theories with the adiabatic approximation is a powerful tool in obtaining insights into the interaction between a many-electron system and an external electromagnetic field. In practical applications of TDHF/TDKS using a truncated basis set, the electronic dynamics and molecular properties become gauge-dependent. Numerical simulations are carried out in the length gauge and velocity gauge to verify the extent of gauge-dependence using incomplete basis sets. Electronic dynamics of two many-electron systems, a helium atom and a carbon monoxide molecule in high-intensity linearly polarized radiation fields are performed using the TDHF and TDKS with two selected adiabatic exchange-correlation (xc) functionals. The time evolution of the expectation values of the dipole moment and harmonic spectra are calculated in the two gauges, and the basis set dependence on the gauge-invariance of these properties is investigated.

show abstract

“…Advanced theoretical studies regarding the nonadiabaticity of the electronic response in polyatomic molecules to strong laser fields have been performed using methods of time-dependent configuration interaction with single excitations (TD-CIS) and time-dependent Hartree-Fock theory [21][22][23][24][25][26]. In these studies, simulations are typically performed under so-called nonionizing conditions, in which the continuum is not taken into account.…”

Section: B Intramolecular Nonadiabatic Behavior In Small Conjugated mentioning

confidence: 99%

Laser-driven nonadiabatic electron dynamics in molecules

Miller

Xia

Becker

2016

Optica

View full text Add to dashboard Cite

In this review, we briefly summarize more than a decade of experimental and theoretical investigations regarding the nonadiabatic electron response to intense femtosecond duration laser fields in a variety of molecular systems. Historically, experimental signatures of nonadiabaticity have emerged readily in large, conjugated, or multi-electron systems, disrupting fragmentation behavior and modulating observed rates of ionization. As model theoretical studies performed in H 2 and other diatomic species show, departure from traditional quasi-static or cycle-averaged descriptions of laser-induced ionization is often necessary to accommodate the rich and frequently counterintuitive electron dynamics that characterize the nonadiabatic response. Nonadiabatic effects such as transient electron localization or the observation of multiple ionization bursts per driving field cycle possess the capacity to modulate the signal of many strong-field physical effects, such as high-order harmonic generation, photoelectron momentum distributions, and molecular fragmentation products. As the advancement of experimental technologies expands the pursuit of laserdriven physics further into the mid-infrared wavelength regime, we suggest that these nonadiabatic effects will become increasingly pronounced and relevant to the imaging and control of a wide array of molecular species.

show abstract

Numerical Bound State Electron Dynamics of Carbon Dioxide in the Strong-Field Regime

Cited by 9 publications

References 50 publications

Strong Field Ionization of β-Estradiol in the IR: Strategies To Optimize Molecular Postionization in Secondary Neutral Mass Spectrometry

Strong Field Ionization of β-Estradiol in the IR: Strategies To Optimize Molecular Postionization in Secondary Neutral Mass Spectrometry

On the gauge invariance of nonperturbative electronic dynamics using the time-dependent Hartree-Fock and time-dependent Kohn-Sham

Laser-driven nonadiabatic electron dynamics in molecules

Contact Info

Product

Resources

About