Probing dynamical symmetries by bicircular high-order harmonic spectroscopy beyond the Born-Oppenheimer approximation

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OriginalspracheEnglisch
Aufsatznummer053438
FachzeitschriftPhysical Review A
Jahrgang101
Ausgabenummer5
PublikationsstatusVeröffentlicht - 28 Mai 2020

Abstract

We explore the possibility of bicircular high-order harmonic spectroscopy to probe the laser-induced dynamics of molecules in a non-Born-Oppenheimer treatment. The numerical solutions of the time-dependent Schrödinger equation for aligned H2 and its isotopologs in ω-2ω bicircular fields show that the intensity ratio between D2 and H2 for harmonic orders 3q is lower than that for orders 3q±1(q∈N). Based on the strong-field approximation, we demonstrate that the interplay of vibrational wave-packet motion and dynamical-symmetry breaking leads to the different ratio. In general, the vibrational motion causes the ratio between isotopologs to increase with q for both harmonic orders 3q and 3q±1. On the other hand, the emission of orders 3q is possible only because of the alignment-induced breaking of the dynamical symmetry. The faster nuclear motion in H2 enhances the symmetry breaking, resulting in the lower D2/H2 ratio for the orders 3q. Therefore, the harmonic orders 3q give access to the attosecond probing of dynamical symmetries in molecules.

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Probing dynamical symmetries by bicircular high-order harmonic spectroscopy beyond the Born-Oppenheimer approximation. / Yue, Shengjun; Brennecke, Simon; Du, Hongchuan et al.
in: Physical Review A, Jahrgang 101, Nr. 5, 053438, 28.05.2020.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Yue, Shengjun ; Brennecke, Simon ; Du, Hongchuan et al. / Probing dynamical symmetries by bicircular high-order harmonic spectroscopy beyond the Born-Oppenheimer approximation. in: Physical Review A. 2020 ; Jahrgang 101, Nr. 5.
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title = "Probing dynamical symmetries by bicircular high-order harmonic spectroscopy beyond the Born-Oppenheimer approximation",
abstract = "We explore the possibility of bicircular high-order harmonic spectroscopy to probe the laser-induced dynamics of molecules in a non-Born-Oppenheimer treatment. The numerical solutions of the time-dependent Schr{\"o}dinger equation for aligned H2 and its isotopologs in ω-2ω bicircular fields show that the intensity ratio between D2 and H2 for harmonic orders 3q is lower than that for orders 3q±1(q∈N). Based on the strong-field approximation, we demonstrate that the interplay of vibrational wave-packet motion and dynamical-symmetry breaking leads to the different ratio. In general, the vibrational motion causes the ratio between isotopologs to increase with q for both harmonic orders 3q and 3q±1. On the other hand, the emission of orders 3q is possible only because of the alignment-induced breaking of the dynamical symmetry. The faster nuclear motion in H2 enhances the symmetry breaking, resulting in the lower D2/H2 ratio for the orders 3q. Therefore, the harmonic orders 3q give access to the attosecond probing of dynamical symmetries in molecules.",
author = "Shengjun Yue and Simon Brennecke and Hongchuan Du and Manfred Lein",
note = "Funding Information: We gratefully acknowledge valuable discussions with Xiaosong Zhu. This work was supported by the China Scholarship Council (CSC) and the National Natural Science Foundation of China (Grant No. 11874030). We thank the Deutsche Forschungsgemeinschaft for support within the Priority Programme Quantum Dynamics in Tailored Intense Fields (QUTIF).",
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T1 - Probing dynamical symmetries by bicircular high-order harmonic spectroscopy beyond the Born-Oppenheimer approximation

AU - Yue, Shengjun

AU - Brennecke, Simon

AU - Du, Hongchuan

AU - Lein, Manfred

N1 - Funding Information: We gratefully acknowledge valuable discussions with Xiaosong Zhu. This work was supported by the China Scholarship Council (CSC) and the National Natural Science Foundation of China (Grant No. 11874030). We thank the Deutsche Forschungsgemeinschaft for support within the Priority Programme Quantum Dynamics in Tailored Intense Fields (QUTIF).

PY - 2020/5/28

Y1 - 2020/5/28

N2 - We explore the possibility of bicircular high-order harmonic spectroscopy to probe the laser-induced dynamics of molecules in a non-Born-Oppenheimer treatment. The numerical solutions of the time-dependent Schrödinger equation for aligned H2 and its isotopologs in ω-2ω bicircular fields show that the intensity ratio between D2 and H2 for harmonic orders 3q is lower than that for orders 3q±1(q∈N). Based on the strong-field approximation, we demonstrate that the interplay of vibrational wave-packet motion and dynamical-symmetry breaking leads to the different ratio. In general, the vibrational motion causes the ratio between isotopologs to increase with q for both harmonic orders 3q and 3q±1. On the other hand, the emission of orders 3q is possible only because of the alignment-induced breaking of the dynamical symmetry. The faster nuclear motion in H2 enhances the symmetry breaking, resulting in the lower D2/H2 ratio for the orders 3q. Therefore, the harmonic orders 3q give access to the attosecond probing of dynamical symmetries in molecules.

AB - We explore the possibility of bicircular high-order harmonic spectroscopy to probe the laser-induced dynamics of molecules in a non-Born-Oppenheimer treatment. The numerical solutions of the time-dependent Schrödinger equation for aligned H2 and its isotopologs in ω-2ω bicircular fields show that the intensity ratio between D2 and H2 for harmonic orders 3q is lower than that for orders 3q±1(q∈N). Based on the strong-field approximation, we demonstrate that the interplay of vibrational wave-packet motion and dynamical-symmetry breaking leads to the different ratio. In general, the vibrational motion causes the ratio between isotopologs to increase with q for both harmonic orders 3q and 3q±1. On the other hand, the emission of orders 3q is possible only because of the alignment-induced breaking of the dynamical symmetry. The faster nuclear motion in H2 enhances the symmetry breaking, resulting in the lower D2/H2 ratio for the orders 3q. Therefore, the harmonic orders 3q give access to the attosecond probing of dynamical symmetries in molecules.

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