scholarly journals Multi-wave mixing in the high harmonic regime: monitoring electronic dynamics

2021 ◽  
Vol 29 (4) ◽  
pp. 4746
Author(s):  
Shicheng Jiang ◽  
Markus Kowalewski ◽  
Konstantin E. Dorfman
2021 ◽  
Vol 19 (12) ◽  
pp. 123202
Author(s):  
Weifeng Yang ◽  
Yichong Lin ◽  
Xueyi Chen ◽  
Yuxuan Xu ◽  
Hongdan Zhang ◽  
...  

2018 ◽  
Vol 4 (9) ◽  
pp. eaau3783 ◽  
Author(s):  
Hugo J. B. Marroux ◽  
Ashley P. Fidler ◽  
Daniel M. Neumark ◽  
Stephen R. Leone

Dynamics following excitation with attosecond extreme ultraviolet (XUV) pulses arise from enormous numbers of accessible excited states, complicating the retrieval of state-specific time evolutions. We develop attosecond XUV multidimensional spectroscopy here to separate interfering pathways on a near-infrared (NIR) energy axis, retrieving single state dynamics in argon atoms in a two-dimensional (2D) XUV-NIR spectrum. In this experiment, we measure four-wave mixing signal arising from the interaction of XUV attosecond pulses centered around 15 eV with two few-cycle NIR pulses. The 2D spectrum is created by measuring the emitted XUV signal field spectrum while applying narrowband amplitude and phase modulations to one of the NIR pulses. Application of such a technique to systems of high dimensionality will provide for the observation of state-resolved pure electronic dynamics, in direct analogy to phenomena unraveled by multidimensional spectroscopies at optical frequencies.


2001 ◽  
Vol 188 (5-6) ◽  
pp. 383-388 ◽  
Author(s):  
J.T. Mendonça ◽  
H. Crespo ◽  
A. Guerreiro

2016 ◽  
Vol 194 ◽  
pp. 369-405 ◽  
Author(s):  
Barry D. Bruner ◽  
Zdeněk Mašín ◽  
Matteo Negro ◽  
Felipe Morales ◽  
Danilo Brambila ◽  
...  

High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.


2011 ◽  
Vol 106 (2) ◽  
Author(s):  
J. B. Bertrand ◽  
H. J. Wörner ◽  
H.-C. Bandulet ◽  
É. Bisson ◽  
M. Spanner ◽  
...  

2011 ◽  
Vol 13 (9) ◽  
pp. 093010 ◽  
Author(s):  
Michael Spanner ◽  
Jochen Mikosch ◽  
Arjan Gijsbertsen ◽  
Andrey E Boguslavskiy ◽  
Albert Stolow

2014 ◽  
Vol 171 ◽  
pp. 113-132 ◽  
Author(s):  
Denitsa Baykusheva ◽  
Peter M. Kraus ◽  
Song Bin Zhang ◽  
Nina Rohringer ◽  
Hans Jakob Wörner

The sensitivities of high-harmonic generation (HHG) and strong-field ionization (SFI) to coupled electronic and nuclear dynamics are studied, using the nitric oxide (NO) molecule as an example. A coherent superposition of electronic and rotational states of NO is prepared by impulsive stimulated Raman scattering and probed by simultaneous detection of HHG and SFI yields. We observe a fourfold higher sensitivity of high-harmonic generation to electronic dynamics and attribute it to the presence of inelastic quantum paths connecting coherently related electronic states [Kraus et al., Phys. Rev. Lett.111, 243005 (2013)]. Whereas different harmonic orders display very different sensitivities to rotational or electronic dynamics, strong-field ionization is found to be most sensitive to electronic motion. We introduce a general theoretical formalism for high-harmonic generation from coupled nuclear-electronic wave packets. We show that the unequal sensitivities of different harmonic orders to electronic or rotational dynamics result from the angle dependence of the photorecombination matrix elements which encode several autoionizing and shape resonances in the photoionization continuum of NO. We further study the dependence of rotational and electronic coherences on the intensity of the excitation pulse and support the observations with calculations.


2019 ◽  
Author(s):  
Ashley Fidler ◽  
Hugo Marroux ◽  
Erika Warrick ◽  
Etienne Bloch ◽  
Wei Cao ◽  
...  

The autoionization dynamics of the (<sup>2</sup>P<sub>1/2</sub>)ns/d Rydberg states in krypton are investigated using wave-mixing signals generated with subfemtosecond XUV pulses and noncollinear, few-cycle NIR pulses. Despite quantum beat oscillations from the XUV-induced coherence, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states. Experimentally measured lifetimes for the wave-mixing signals emitting from the (<sup>2</sup>P<sub>1/2</sub>)6d/8s, 7d/9s, and 8d/10s resonances compare favorably with lifetimes for the (<sup>2</sup>P<sub>1/2</sub>)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways leads to reporter state-dependent decays in the wave-mixing signals. The results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.<br>


2019 ◽  
Author(s):  
Ashley Fidler ◽  
Hugo Marroux ◽  
Erika Warrick ◽  
Etienne Bloch ◽  
Wei Cao ◽  
...  

The autoionization dynamics of the (<sup>2</sup>P<sub>1/2</sub>)ns/d Rydberg states in krypton are investigated using wave-mixing signals generated with subfemtosecond XUV pulses and noncollinear, few-cycle NIR pulses. Despite quantum beat oscillations from the XUV-induced coherence, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states. Experimentally measured lifetimes for the wave-mixing signals emitting from the (<sup>2</sup>P<sub>1/2</sub>)6d/8s, 7d/9s, and 8d/10s resonances compare favorably with lifetimes for the (<sup>2</sup>P<sub>1/2</sub>)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways leads to reporter state-dependent decays in the wave-mixing signals. The results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.<br>


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