Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra.

Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra.
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DOI:
10.1038/s41598-021-82232-1
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发表时间:
2021-01-28
期刊:
影响因子:
4.6
通讯作者:
Marangos JP
Marangos JP
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Austin DR;Johnson AS;McGrath F;Wood D;Miseikis L;Siegel T;Hawkins P;Harvey A;Mašín Z;Patchkovskii S;Vacher M;Malhado JP;Ivanov MY;Smirnova O;Marangos JP

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我们提出了一种新的方法来测量几飞秒电子和核动力学在原子和多原子分子使用多维高次谐波产生(HHG)光谱测量,其中的光谱记录为激光强度的函数,形成一个二维的数据集。该方法适用于氙原子和苯分子,后者表现出显着的快速核动力学电离后。我们揭示了强场电离氙原子中返回电子通量的子周期演化的签名,隐含在强场近似中,但以前没有直接观察到。我们进一步提取核自相关函数在强场电离苯阳离子,这是确定有一个衰减的fs,在良好的协议,从直接动力学变分多组态高斯计算得到的fs。我们的方法需要最少的假设系统,甚至是适用于未对齐的多原子分子。
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 fs, in good agreement with the 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.
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