Theoretical study of molecular electronic and rotational coherences by high-order-harmonic generation

Zhang, Song Bin; Baykusheva, Denitsa; Kraus, Peter M.; Wörner, Hans Jakob; Rohringer, Nina

doi:10.1103/physreva.91.023421

Cited by 15 publications

(16 citation statements)

References 57 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This feature reflects the nodal plane of the molecular orbital, which contains the laser polarization in this specific configuration. This feature is not visible in the experimental data, because the fraction of excited molecules is on the order of 1% (refs 34 , 35 ) and the molecules are not aligned at the considered delays, whereas 100% excitation and perfect alignment was assumed in the calculations.…”

Section: Resultsmentioning

confidence: 96%

“…The rapid regular oscillation originates from the electronic dynamics, illustrated in the inset, whereas the two features around 5 and 10 ps correspond to rotational revivals. The amplitude modulations observed around 8–9.5 ps are a characteristic signature of multi-level quantum beats3435. Figure 1b shows a cut through the three-dimensional photoelectron momentum distribution recorded at a delay of 1.56 ps.…”

Section: Resultsmentioning

confidence: 97%

“…1a . These calculations have been done with the methods described in refs 34 , 35 . They include the rotational levels of both populated electronic states of NO and fully account for the coupled electronic and rotational dynamics on the relevant time scales.…”

Section: Resultsmentioning

confidence: 99%

See 2 more Smart Citations

Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering

et al. 2017

Self Cite

View full text Add to dashboard Cite

Strong-field photoelectron holography and laser-induced electron diffraction (LIED) are two powerful emerging methods for probing the ultrafast dynamics of molecules. However, both of them have remained restricted to static systems and to nuclear dynamics induced by strong-field ionization. Here we extend these promising methods to image purely electronic valence-shell dynamics in molecules using photoelectron holography. In the same experiment, we use LIED and photoelectron holography simultaneously, to observe coupled electronic-rotational dynamics taking place on similar timescales. These results offer perspectives for imaging ultrafast dynamics of molecules on femtosecond to attosecond timescales.

show abstract

Section: Resultsmentioning

confidence: 96%

Section: Resultsmentioning

confidence: 97%

See 1 more Smart Citation

Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering

et al. 2017

Self Cite

View full text Add to dashboard Cite

show abstract

“…Time-domain studies of electrons in atoms, molecules, and the condensed phase offer new approaches to understanding electronic structure and electronic correlations (see, e.g., [1][2][3][4][5][6]). Electronic wave packets have been measured in the valence shell of atomic ions using transient absorption [7,8] or sequential double ionization [9,10] and in the valence shell of neutral molecules using high-harmonic spectroscopy [11][12][13].…”

Section: Introductionmentioning

confidence: 99%

Preparing attosecond coherences by strong-field ionization

2016

Self Cite

View full text Add to dashboard Cite

Strong-field ionization (SFI) has been shown to prepare wave packets with few-femtosecond periods. Here, we explore whether this technique can be extended to the attosecond time scale. We introduce an intuitive model, which is based on the Fourier transform of the subcycle SFI rate, for predicting the bandwidth of ionic states that can be coherently prepared by SFI. The coherent bandwidth decreases considerably with increasing central wavelength of the ionizing pulse but it is much less sensitive to its intensity. Many-body calculations based on time-dependent configuration-interaction singles support these results. The influence of channel interactions and laser-induced dynamics within the ion is discussed. Our results further predict that multicycle femtosecond pulses can coherently prepare subfemtosecond wave packets with higher selectivity and versatility compared to single-cycle pulses with an additional sensitivity to the mutual parity of the prepared states.

show abstract

“…[37][38][39] Alternatively, electronic coherences in neutral molecules can be prepared by impulsive stimulated Raman scattering (ISRS) and followed by a second time-delayed pulse, which generates high harmonics from the coherent superposition of states. [40][41][42] All experiments described in this section employ pump-probe schemes for following electronic dynamics in atoms and molecules. They have all remained limited to the few-femtosecond time scale because of the necessity of a near-infrared pulse as either the pump or probe.…”

Section: A Time-resolved Electronic Spectroscopymentioning

confidence: 99%

Perspectives of Attosecond Spectroscopy for the Understanding of Fundamental Electron Correlations

Kraus

Wörner

2018

Angew Chem Int Ed

Self Cite

View full text Add to dashboard Cite

The description of the electronic structure of molecules in terms of molecular orbitals is a highly successful concept in chemistry. However, it commonly fails if the electrons in a molecule are strongly correlated and cannot be treated as independent particles. Electron correlation is essential to understand inner-valence X-ray spectroscopies, it can drive ultrafast charge migration in molecules, and it is responsible for many exotic properties of strongly correlated materials. Time-resolved spectroscopy with attosecond resolution is generally capable of following electronic motion in real time and can thus provide experimental access to electron-correlation-driven phenomena. High-harmonic spectroscopy in particular uses the precisely timed laser-driven recollision of electrons to interrogate the electronic structure and dynamics of the investigated system on a sub-femtosecond timescale. In this Review, the capabilities of high-harmonic spectroscopy to follow electronic motion in molecules are discussed. Both qualitative and quantitative approaches to unraveling the detailed dynamical responses of molecular systems following ionization are presented. A new theoretical formalism for the reconstruction of correlation-driven charge migration is introduced. The importance of electron-ion entanglement and electronic coherence in the reconstruction of attosecond hole dynamics are discussed. These advances make high-harmonic spectroscopy a promising technique to decode fundamental electron correlations and to provide experimental data on the complex manifestations of multi-electron dynamics.

show abstract

Theoretical study of molecular electronic and rotational coherences by high-order-harmonic generation

Abstract: The detection of electron motion and electronic wavepacket dynamics is one of the core goals 33.20.Xx, 42.50.Hz, 42.65.Ky PACS:

Cited by 15 publications

References 57 publications

Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering

Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering

Preparing attosecond coherences by strong-field ionization

Perspectives of Attosecond Spectroscopy for the Understanding of Fundamental Electron Correlations

Contact Info

Product

Resources

About