Effects of Macroscopic Propagation and Multiple Molecular Orbitals on the High-Order Harmonic Generation of Aligned N $$_2$$ and CO $$_2$$ Molecules

Jin, Cheng

doi:10.1007/978-3-319-01625-2_6

Cited by 1 publication

(4 citation statements)

References 55 publications

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“…However, despite the increased uncertainty, as observed the appearance of minima in the cutoff may provide insight toward the interplay of both interference mechanisms. Similar results have been reported in previous measurements. − ,,, …”

Section: Resultssupporting

confidence: 93%

“…Similar results have been reported in previous measurements. [21][22][23]28,29,32 For a 800 nm driving wavelength the observed minimum has a more definitive intensity-dependence, as seen in Figure 2e,f. It appears below 47 eV for all driving intensities and shows a strong linear trend between driving intensity and minimum energy, as shown in Figure 3c,d.…”

Section: ■ Description Of Interferencesmentioning

confidence: 73%

“…Further, at high-intensity 800 nm and low-intensity 1200 nm driving fields, the minimum occurs at the location of the two-center interference, and hence, the HOMO is further suppressed enhancing the multichannel interference, as was possibly seen in our 1200 nm data as well as previously at 800 nm. [22][23][24]28,29,32 We note that the exact wavelength where this interplay between interference mechanisms is observed depends heavily on the degree of alignment, which strongly governs the ratio of yields between the HOMO and HOMO−2, magnitude of the interference, and energetic location of the interference. 28,34,35 Spectral Group Delays.…”

Section: ■ Description Of Interferencesmentioning

confidence: 99%

“…One of the most commonly studied features in high-harmonic spectra is a local minimum in the high-harmonic intensity generated in CO 2 . ,− This minimum was first observed by Kanai et al and attributed to two-center interference (TCI) associated with coherent electron rescattering from the two charge centers in the highest occupied molecular orbital (HOMO). When later observations showed that the energetic location of the minimum depended upon the intensity of the driving field, it was reinterpreted as the result of an interference between coherent generation from the HOMO and HOMO–2. ,,, Now the consensus is that both mechanisms are at play. ,,, Specifically, the contribution from each mechanism is influenced by four parameters: wavelength, intensity, alignment angle, and degree of alignment …”

Section: Introductionmentioning

confidence: 99%

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Investigation of Interferences in Carbon Dioxide through Multidimensional Molecular-Frame High-Harmonic Spectroscopy

et al. 2022

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We present molecular-frame high-harmonic spectroscopic measurements of the spectral intensity and group delay of carbon dioxide. Using four different driving wavelengths and a range of intensities at each wavelength for high-harmonic generation, we observe a well-characterized minimum in the harmonic emission that exhibits both a wavelength and intensity dependence. Using the intensity dependence at each driving wavelength, we classify the minimum as due to either a structural two-center interference or dynamic multichannel interference, consistent with previous literature. By additionally measuring the group delay at each driving wavelength and intensity, we find that the sign of the group delay excursion across the interference is an acute probe of the interference mechanism. The experimental results are confirmed by ab initio time-dependent density functional theory calculations of both the spectral intensity and the phase of the harmonic emission.

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