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Rescattering electrons offer great potential as probes of molecular properties on ultrafast timescales. The most famous example is molecular tomography, in which high harmonic spectra of oriented molecules are mapped to ``tomographic…

Atomic Physics · Physics 2016-09-28 Zachary B. Walters , Stefano Tonzani , Chris H. Greene

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

High harmonic generation in the interaction of femtosecond lasers with atoms and molecules opens the path to molecular orbital tomography and to probe the electronic dynamics with attosecond-{\AA}ngstr\"{o}m resolutions. Molecular orbital…

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

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

Accurate molecular imaging via high-order harmonic generation relies on comparing the harmonic emission from a molecule and an adequate reference system. However, an ideal reference atom with the same ionization properties as the molecule…

Atomic Physics · Physics 2015-05-28 Elmar V. van der Zwan , Manfred Lein

Orbital tomography has recently been established as a technique to reconstruct molecular orbitals directly from photoemission data using iterative phase retrieval algorithms. In this work, we present a detailed description of steps for…

We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO2 molecules. We unambiguously observe a reversal in phase of the high order harmonic emission for higher harmonic…

Atomic Physics · Physics 2009-11-13 Xibin Zhou , Robynne Lock , Wen Li , Nick Wagner , Margaret. M. Murnane , Henry C. Kapteyn

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

Photoemission orbital tomography provides direct access from laboratory measurements to the real-space molecular orbitals of well-ordered organic semiconductor layers. Specifically, the application of phase retrieval algorithms to…

Materials Science · Physics 2024-04-29 Thi Lan Dinh , G. S. Matthijs Jansen , D. Russell Luke , Wiebke Bennecke , Stefan Mathias

We propose a new method to overcome the nodal plane problem for the tomographic reconstruction of molecular orbitals with twofold mirror antisymmetry in the length form based on high-order harmonic generation. It is shown that, by carrying…

Chemical Physics · Physics 2013-04-30 Xiaosong Zhu , Meiyan Qin , Yang Li , Qingbin Zhang , Zhizhan Xu , Peixiang Lu

We introduce a method for accurate quantum chemical calculations based on a simple variational wave function, defined by a single geminal that couples all the electrons into singlet pairs, combined with a real space correlation factor. The…

Materials Science · Physics 2009-10-22 M. Marchi , S. Azadi , M. Casula , S. Sorella

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

Light beams carrying orbital angular momentum (OAM) have led to stunning applications in various fields from quantum information to microscopy. In this letter, we examine OAM from the recently discovered high-harmonic generation (HHG) in…

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

The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the…

Atomic Physics · Physics 2015-05-19 B. B. Augstein , C. Figueira de Morisson Faria

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

The ability to directly follow and time resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser induced electron diffraction can…

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

This tutorial presents the most important aspects of the molecular self-probing paradigm, which views the process of high harmonic generation as "a molecule being probed by one of its own electrons". Since the properties of the electron…

Atomic Physics · Physics 2021-03-31 Stefan Haessler , Jérémie Caillat , Pascal Salières
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