Theoretical study of the photodissociation of Li2+ in one-color intense laser fields

Li, Yuanjun; Jiang, Wanyi; Khait, Yuriy G.; Hoffmann, Mark R.

doi:10.1063/1.3585645

Cited by 3 publications

(3 citation statements)

References 71 publications

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“…In this case, the splitting between the upper and lower polariton states is proportional to , where N is the number of coupled molecules. A range of interesting phenomena arising from strong light–matter coupling has been observed in recent years, and theory has played a central role in exploring this new realm of chemistry and physics. − ,− ,− …”

Section: Resultsmentioning

confidence: 99%

“…Under continuous wave radiation, absorption and emission processes conserve quasi-energy within the Floquet approximation, because the photon energy is included in the total quasi-energy (the expectation value of the Floquet Hamiltonian). In fact, the Floquet picture has been effectively employed in many past simulation studies of nonadiabatic dynamics in light fields. − When applying Floquet in an ultrafast context, it is important to note that the Floquet formalism is only rigorously valid for a potential that is periodic in time. However, work by Halász et al suggests that the Floquet approximation can perform well for modeling ultrashort pulses, as well .…”

Section: Introductionmentioning

confidence: 99%

“…The second advantage of Floquet TDCI is that the light-dressed determinants provide a natural basis in which to describe polariton states, in which the excited states of matter and the light field are strongly mixed. Strong light–matter coupling has been implicated in a wide range of intriguing physical phenomena, and strategies for the control of chemical reactions through Floquet physics are in development. − ,− Though the Floquet approximation is not a truly quantum treatment of the light field, a light-dressed state can reasonably be thought of as a state of matter in the presence of some number of photons. Thus, a linear combination of such states describes the entanglement between light and matter states that defines a polariton state.…”

Section: Introductionmentioning

confidence: 99%

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Floquet Time-Dependent Configuration Interaction for Modeling Ultrafast Electron Dynamics

Durden

Levine

2022

J. Chem. Theory Comput.

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Time-dependent electronic structure methods are a valuable tool for simulating spectroscopic experiments. Recent advances in time-dependent configuration interaction (TDCI) algorithms have made them an attractive means of modeling many-electron dynamics, particularly for cases where multireference effects are essential. Here we present an extension to TDCI, Floquet TDCI, where the electronic wave function is expanded in a basis of light-dressed determinants. Our approach is based on our high-performance graphics processing unit (GPU) accelerated implementation of complete active space configuration interaction (CASCI). Simulations of two-photon absorption demonstrate that Floquet TDCI is well-suited for modeling dynamics in intense, ultrashort laser pulses. Accurate results are obtained for pulse energies up to ∼4 × 10–4 J/cm2 per pulse in the most difficult case explored here. By simulation of a set of molecules under continuous wave coupling, we demonstrate the ability of Floquet to describe the entanglement of light and multiple molecules in a cavity (i.e., a cavity polariton). Excellent computational performance is observed: a 320 fs propagation of a large dye (C30N2H22) with a 2 as timestep and a large active space (10 electrons in 11 orbitals), including a monochromatic pulse with three photon states, was performed in 3 h 6 min on a single Tesla V100 GPU. Our Floquet TDCI algorithm scales linearly with the number of photon states and exponentially with the number of photon colors included in the calculation. We argue that its energy-conserving nature makes Floquet TDCI well-suited to drive nonadiabatic molecular dynamics simulations.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Floquet Time-Dependent Configuration Interaction for Modeling Ultrafast Electron Dynamics

Durden

Levine

2022

J. Chem. Theory Comput.

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Effect of laser pulse width on wave packet motion in femotosecond pump-probe pulses

Guo

Feng

2016

Optik

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The dependence of the wave packet process of three-level ladder K 2 molecules on pulse width was investigated via time-dependent wave packet method, and was firstly quantified. There is no Autler-Townes splitting in the photoelectron spectrum with weaker pump intensity or shorter pulse width. The oscillation period of wave packet increases and the oscillation amplitude decreases with increasing pulse width. The pulse width affects Rabi oscillation, which results in the periodical change of the populations of the electronic state. Quantifying its effect on the population of the excited state shows that the change frequency varies with increasing pump intensity.The results illustrates that the needed population in electronic state of interested can be obtained by controlling pulse width, which provide some important basis for light manipulation of molecular processes experimentally.

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Theoretical investigation of femtosecond-resolved photoelectron spectra of three-level ladder K2 molecules

Feng¹,

Wei²,

Xing-Qiang³

et al. 2015

Acta Phys. Sin.

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We investigate the effect of delay time, pulse width and pump wavelength on photoelectron spectra and wave packet forming process of the three-level K2 molecules via time-dependent wave packet approach. There is no Autler-Townes splitting for weaker pump intensity or shorter pulse width. Delay time and pump wavelength can affect peak structure, position, and relative height. The vibration period of wave packet does not vary with pump wavelength, while the oscillating amplitude decreases with increasing pulse width. Results may provide important basis for realizing the optical control of molecules experimentally.

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Theoretical study of the photodissociation of Li2+ in one-color intense laser fields

Cited by 3 publications

References 71 publications

Floquet Time-Dependent Configuration Interaction for Modeling Ultrafast Electron Dynamics

Floquet Time-Dependent Configuration Interaction for Modeling Ultrafast Electron Dynamics

Effect of laser pulse width on wave packet motion in femotosecond pump-probe pulses

Theoretical investigation of femtosecond-resolved photoelectron spectra of three-level ladder K2 molecules

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