2009
DOI: 10.1021/jp907372k
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Observing the Transition from Stark-Shifted, Strong-Field Resonance to Nonadiabatic Excitation

Abstract: Time-dependent Hartree-Fock simulations for a linear triatomic molecular monocation (CO 2 + ) interacting with a 5 fs, 800 nm, strong field laser pulse were performed to explore the excitation mechanisms in a molecular cation. Fourier analysis of the time-dependent residual dipole moment reveal a nonmonotonic behavior in the amplitude of the 5.18 eV feature in the excitation spectra of the molecular monocation with increasing intensity, suggesting a change in the excitation mechanism. Calculations performed fo… Show more

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Cited by 6 publications
(7 citation statements)
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“…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%
“…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%
“…Klamroth and co-workers used optimal control theory and time-dependent configuration interaction with single excitations (TD-CIS) to shape short, intense pulses for state-selective excitation of N -methylquinoline and employed TD-CIS(D) to simulate dipole switching in lithium cyanide. They also used heuristic methods to include the effects of ionization, dissipation, and dephasing. Li and co-workers combined real-time integration of time-dependent density functional theory with Ehrenfest dynamics to investigate laser-controlled dissociation processes. In previous works, we used TD-HF (time-dependent Hartree−Fock) and TD-CIS methods to simulate the response of CO 2 , polyenes, and polyacenes and their cations to short, intense laser pulses. The approximate simulations that have been carried out to date on polyatomic systems are promising, but there is a need to compare the performance of the various methods.…”
Section: Introductionmentioning
confidence: 99%
“…Klamroth, Saalfrank and co-workers have employed time-dependent configuration interaction with single excitations (TD-CIS) to study electron dynamics, pulse shaping and ionization. Li and co-workers have used Ehrenfest dynamics and real-time integration of TD-DFT to investigate laser controlled dissociation processes. In earlier studies we have used TD-HF and TD-CIS methods to simulate the response of CO 2 , polyenes, and polyacenes and their cations to short, intense laser pulses. …”
Section: Introductionmentioning
confidence: 99%