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High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular…

Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding…

We investigate the orientation dependence of molecular high-order harmonic generation (HHG) both numerically and analytically. We show that the molecular recollision electronic wave packets (REWPs) in the HHG are closely related to the…

Atomic Physics · Physics 2009-11-13 Yanjun. Chen , Yan. Li , Shiping. Yang , Jie. Liu

We propose a real-time time-dependent ab__initio approach within a configuration-interaction-singles ansatz to decompose the high-harmonic generation (HHG) signal of molecules in terms of individual molecular-orbital (MO) contributions.…

Chemical Physics · Physics 2025-12-11 Marco Marchetta , Chiara Morassut , Julien Toulouse , Emanuele Coccia , Eleonora Luppi

The rich information content of measurements in the molecular frame rather than the laboratory frame has motivated the development of several methods for aligning gas phase molecules in space. Even so, for asymmetric tops the problem of…

Atomic Physics · Physics 2016-11-23 Varun Makhija , Xiaoming Ren , Drue Gockel , Anh-Thu Le , Vinod Kumarappan

High-order harmonic generation is a powerful and sensitive tool for probing atomic and molecular structures, combining in the same measurement an unprecedented attosecond temporal resolution with a high spatial resolution, of the order of…

Chemical Physics · Physics 2015-06-23 M. Negro , M. Devetta , D. Faccialà , S. De Silvestri , C. Vozzi , S. Stagira

We report theoretical investigations of the tomographic procedure suggested by Itatani {\it et al.} [Nature, {\bf 432} 867 (2004)] for reconstructing highest occupied molecular orbitals (HOMO) using high-order harmonic generation (HHG).…

Atomic Physics · Physics 2009-10-30 Van-Hoang Le , Anh-Thu Le , Rui-Hua Xie , C. D. Lin

High-order harmonic generation (HHG) results from strong-field laser matter interaction and it is one of the main processes that are used to extract electron structural and dynamical information about the atomic or molecular targets with…

Recent measurements on high-order harmonic generation (HHG) from N$_2$ aligned perpendicular to the driving laser polarization [B. K. McFarland {\it el al}, Science {\bf 322}, 1232 (2008)] have shown a maximum at the rotational…

Atomic Physics · Physics 2009-10-30 Anh-Thu Le , R. R. Lucchese , C. D. Lin

High-order harmonic generation (HHG) is a powerful tool for probing electronic structure and ultrafast dynamics in matter. Traditionally studied in atomic and molecular gases, HHG has recently been extended to condensed matter, enabling…

Recently, a method to image molecular electronic wave functions using high harmonic generation (HHG) was introduced by Itatani \textit{et al.\} [Nature {\textbf{432}}, 876 (2004)]. We show that, while the tomographic reconstruction of…

Atomic Physics · Physics 2009-11-13 Elmar V. van der Zwan , Ciprian C. Chirilă , Manfred Lein

We show that the dependence of high-order harmonic generation (HHG) on the molecular orientation can be understood within a theoretical treatment that does not involve the strong field of the laser. The results for H_2 show excellent…

Atomic Physics · Physics 2009-11-10 B. Zimmermann , M. Lein , J. M. Rost

We investigate the orientation dependence of high-order harmonic generation (HHG) from H$_2^+$ with different internuclear distances irradiated by intense laser fields both numerically and analytically. The calculated molecular HHG spectra…

Atomic Physics · Physics 2009-11-13 Yanjun Chen , Jie Liu , Bambi Hu

We demonstrate to image asymmetric molecular orbitals via high-order harmonic generation in a one-color inhomogeneous field. Due to the broken inversion symmetry of the inhomogeneous field in space, the returning electrons with energy in a…

Optics · Physics 2018-03-14 Hua Yuan , Lixin He , Feng Wang , Baoning Wang , Xiaosong Zhu , Pengfei Lan , Peixiang Lu

Attosecond light sources based on high-order harmonic generation (HHG) constitute to date the only table-top solution for producing coherent broadband radiation covering the spectral range from the extreme ultraviolet to the soft X-rays.…

Toroidal vortex is a kind of novel and exotic structured light with potential applications in photonic topology and quantum information. Here, we present the study on high harmonic generation (HHG) from the interaction of the intense…

Optics · Physics 2024-10-10 Zijian Lyu , Yiqi Fang , Yunquan Liu

The influence of large permanent dipoles on molecular orbital tomography via high-order harmonic generation (HHG) is investigated in this work. It is found that, owing to the modification of the angle-dependent ionization rate resulting…

Atomic Physics · Physics 2013-02-27 Xiaosong Zhu , Meiyan Qin , Qingbin Zhang , Yang Li , Zhizhan Xu , Peixiang Lu

An all-optical measurement of high-order fractional molecular echoes is demonstrated by using high-order harmonic generation (HHG). Excited by a pair of time-delayed short laser pulses, the signatures of full and high order fractional (1/2…

Chemical Physics · Physics 2019-10-23 Baoning Wang , Lixin He , Yanqing He , Yinfu Zhang , Renzhi Shao , Pengfei Lan , Peixiang Lu

The detection of electron motion and electronic wavepacket dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide (NO) molecule as an example, we have introduced and demonstrated a new experimental…

Atomic and Molecular Clusters · Physics 2015-04-17 Song Bin Zhang , Denitsa Baykusheva , Peter M. Kraus , Hans Jakob Wörner , Nina Rohringer

We investigated the high-order harmonic generation (HHG) process of diatomic molecular ion $\mathrm{H}_2^+$ in non-Born-Oppenheimer approximations. The corresponding three-dimensional time-dependent Schr\"odinger equation is solved with…

Atomic Physics · Physics 2017-02-28 Mu-Zi Li , Guang-Rui Jia , Xue-Bin Bian
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