Pump and probe ultrafast electron dynamics in LiH: a computational study

Nest, Mathias; Remacle, Françoise; Levine, R. D.

doi:10.1088/1367-2630/10/2/025019

Cited by 93 publications

(81 citation statements)

References 80 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…1 (For recent reviews see Lepine et al, 2,3 Kling 4 and Ivanov. 5 ) Theoretical studies of pure electron dynamics, [6][7][8][9][10][11][12][13][14][15][16] where the nuclei were fixed and only the time evolution of the electronic wavepacket was allowed, have demonstrated oscillatory charge migration.…”

Section: Introductionmentioning

confidence: 99%

Communication: Oscillating charge migration between lone pairs persists without significant interaction with nuclear motion in the glycine and Gly-Gly-NH-CH3 radical cations

Vacher

Bearpark

Robb

2014

The Journal of Chemical Physics

View full text Add to dashboard Cite

Coupled electron-nuclear dynamics has been studied, using the Ehrenfest method, for four conformations of the glycine molecule and a single conformation of Gly-Gly-NH-CH 3 . The initial electronic wavepacket was a superposition of eigenstates corresponding to ionization from the σ lone pairs associated with the carbonyl oxygens and the amine nitrogen. For glycine, oscillating charge migration (when the nuclei were frozen) was observed for the 4 conformers studied with periods ranging from 2 to 5 fs, depending on the energy gap between the lone pair cationic states. When coupled nuclear motion was allowed (which was mainly NH 2 partial inversion), the oscillations hardly changed. For Gly-Gly-NH-CH 3 , charge migration between the carbonyl oxygens and the NH 2 lone pair can be observed with a period similar to glycine itself, also without interaction with nuclear motion. These simulations suggest that charge migration between lone pairs can occur independently of the nuclear motion. © 2014 AIP Publishing LLC. [http://dx

show abstract

Section: Introductionmentioning

confidence: 99%

Communication: Oscillating charge migration between lone pairs persists without significant interaction with nuclear motion in the glycine and Gly-Gly-NH-CH3 radical cations

Vacher

Bearpark

Robb

2014

The Journal of Chemical Physics

View full text Add to dashboard Cite

show abstract

“…The multiconfiguration time-dependent Hartree-Fock (MCTDHF) algorithm [24][25][26][27][28][29][30][31][32] is an adaptive method for calculating nonpertubative electronic dynamics in molecules. In a recently described numerical implementation [33,34] that we use here, all electrons are active, all orbitals are time-dependent, and any number of them may be ionized.…”

Section: Methodsmentioning

confidence: 99%

Ultrafast population transfer to excited valence levels of a molecule driven by x-ray pulses

Haxton

McCurdy

2014

Phys. Rev. A

View full text Add to dashboard Cite

First-principles quantum mechanical calculations of an intense-field ultrafast two-color core hole stimulated Raman process in nitric oxide are presented. They employ the Multiconfiguration TimeDependent Hartree-Fock (MCTDHF) method with all 15 electrons active. These calculations demonstrate a robust excitation localized on an atom through a core-electron stimulated Raman transition, the first step in proposed stimulated X-ray Raman spectroscopy experiments. A total population transfer of approximately 41% into valence excited states and 30% ionization is obtained via two concurrent 1.31fs pulses of maximum intensity 0.5 and 3 ×10 17 W cm −2 . It is found that both resonant and nonresonant (via the continuum) Raman transitions contribute. All aspects of these calculations except for AC stark shifts are converged with a modest basis of 11 orbitals, demonstrating the efficiency of MCTDHF for the treatment of nonperturbative electronic dynamics in molecules.

show abstract

“…LiH electronic states have been extensively studied by us [7,52,[58][59][60] and others. [61][62][63][64] The electronic states were computed at MRCI level using the quantum chemistry code MOLPRO [65], see Supplemental Materials (SM) for details.…”

Section: Non Equilibrium Electron-nuclei Dynamicsmentioning

confidence: 99%

“…[18,20,[53][54][55][56][57] For the polar LiH molecule, changing the value of the CEP of the nearly one cycle pulse allows selecting excited states of opposite polarities, depending on whether the electric field at its maximum points to the Li or to the H atoms. [7,58] As a result, the non stationary electronic wave packet built at the end of the pulse has a different ionic character, either Li δ + H δ − or Li δ − H δ + , and this steers the nuclear dynamics to different dissociation asymptotes. We further show that changing the value of the CEP by π prepares at the end of the pulse non stationary states that are not only of complementary polarity but also of opposite coherence.…”

Section: Introductionmentioning

confidence: 99%

Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse

2017

View full text Add to dashboard Cite

Dynamical computations demonstrate considerable selectivity over the fragmentation channels of the LiH molecule via the polarization and the carrier envelope phase (CEP) of a single ultrashort one cycle strong IR pulse. For aligned molecules, control of the CEP allows building non stationary coherent electronic wave packets of contrasting ionic character, either Li δ + H δ − or Li δ − H δ + . The complementary coherences are maintained all the way to dissociation. The direction of the electric field at its maximum points either towards the Li or towards the H atom, which selectively steers the nuclear dynamics to specific dissociation products.3

show abstract

Pump and probe ultrafast electron dynamics in LiH: a computational study

Cited by 93 publications

References 80 publications

Communication: Oscillating charge migration between lone pairs persists without significant interaction with nuclear motion in the glycine and Gly-Gly-NH-CH3 radical cations

Communication: Oscillating charge migration between lone pairs persists without significant interaction with nuclear motion in the glycine and Gly-Gly-NH-CH3 radical cations

Ultrafast population transfer to excited valence levels of a molecule driven by x-ray pulses

Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse

Contact Info

Product

Resources

About