Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra
Abstract We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a...
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Nature Portfolio
2021
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oai:doaj.org-article:24c85f34f06d453da452fac7a3b089102021-12-02T13:57:25ZExtracting sub-cycle electronic and nuclear dynamics from high harmonic spectra10.1038/s41598-021-82232-12045-2322https://doaj.org/article/24c85f34f06d453da452fac7a3b089102021-01-01T00:00:00Zhttps://doi.org/10.1038/s41598-021-82232-1https://doaj.org/toc/2045-2322Abstract We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a two-dimensional data set. The method is applied to xenon atoms and to benzene molecules, the latter exhibiting significant fast nuclear dynamics following ionization. We uncover the signature of the sub-cycle evolution of the returning electron flux in strong-field ionized xenon atoms, implicit in the strong field approximation but not previously observed directly. We furthermore extract the nuclear autocorrelation function in strong field ionized benzene cations, which is determined to have a decay of $$\tau _0 = 4 \pm 1$$ τ 0 = 4 ± 1 fs, in good agreement with the $$ \tau _0 = 3.5$$ τ 0 = 3.5 fs obtained from direct dynamics variational multi-configuration Gaussian calculations. Our method requires minimal assumptions about the system, and is applicable even to un-aligned polyatomic molecules.Dane R. AustinAllan S. JohnsonFelicity McGrathDavid WoodLukas MiseikisThomas SiegelPeter HawkinsAlex HarveyZdeněk MašínSerguei PatchkovskiiMorgane VacherJoão Pedro MalhadoMisha Y. IvanovOlga SmirnovaJon P. MarangosNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-8 (2021) |
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DOAJ |
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DOAJ |
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Medicine R Science Q |
| spellingShingle |
Medicine R Science Q Dane R. Austin Allan S. Johnson Felicity McGrath David Wood Lukas Miseikis Thomas Siegel Peter Hawkins Alex Harvey Zdeněk Mašín Serguei Patchkovskii Morgane Vacher João Pedro Malhado Misha Y. Ivanov Olga Smirnova Jon P. Marangos Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| description |
Abstract We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a two-dimensional data set. The method is applied to xenon atoms and to benzene molecules, the latter exhibiting significant fast nuclear dynamics following ionization. We uncover the signature of the sub-cycle evolution of the returning electron flux in strong-field ionized xenon atoms, implicit in the strong field approximation but not previously observed directly. We furthermore extract the nuclear autocorrelation function in strong field ionized benzene cations, which is determined to have a decay of $$\tau _0 = 4 \pm 1$$ τ 0 = 4 ± 1 fs, in good agreement with the $$ \tau _0 = 3.5$$ τ 0 = 3.5 fs obtained from direct dynamics variational multi-configuration Gaussian calculations. Our method requires minimal assumptions about the system, and is applicable even to un-aligned polyatomic molecules. |
| format |
article |
| author |
Dane R. Austin Allan S. Johnson Felicity McGrath David Wood Lukas Miseikis Thomas Siegel Peter Hawkins Alex Harvey Zdeněk Mašín Serguei Patchkovskii Morgane Vacher João Pedro Malhado Misha Y. Ivanov Olga Smirnova Jon P. Marangos |
| author_facet |
Dane R. Austin Allan S. Johnson Felicity McGrath David Wood Lukas Miseikis Thomas Siegel Peter Hawkins Alex Harvey Zdeněk Mašín Serguei Patchkovskii Morgane Vacher João Pedro Malhado Misha Y. Ivanov Olga Smirnova Jon P. Marangos |
| author_sort |
Dane R. Austin |
| title |
Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| title_short |
Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| title_full |
Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| title_fullStr |
Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| title_full_unstemmed |
Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| title_sort |
extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra |
| publisher |
Nature Portfolio |
| publishDate |
2021 |
| url |
https://doaj.org/article/24c85f34f06d453da452fac7a3b08910 |
| work_keys_str_mv |
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1718392310092267520 |