Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics

Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic signals different...

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Main Authors: Guanglu Yuan, Ruifeng Lu, Shicheng Jiang, Konstantin Dorfman
Format: Article
Language:English
Published: American Association for the Advancement of Science (AAAS) 2023-01-01
Series:Ultrafast Science
Online Access:https://spj.science.org/doi/10.34133/ultrafastscience.0040
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author Guanglu Yuan
Ruifeng Lu
Shicheng Jiang
Konstantin Dorfman
author_facet Guanglu Yuan
Ruifeng Lu
Shicheng Jiang
Konstantin Dorfman
author_sort Guanglu Yuan
collection DOAJ
description Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic signals different from the case of avoided crossing. The coherence built up when the system crosses the avoided crossing will lead to the oscillatory behavior of the spectrum, while the geometric phase erodes these oscillations in the case of conical intersection. Additionally, the dynamical blueshift and the splitting of the time-resolved spectrum allow capturing the snapshot dynamics with the sub-femtosecond resolution.
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spelling doaj.art-7e10efc05cf64b3b8593a18f0afac36a2023-08-23T16:17:35ZengAmerican Association for the Advancement of Science (AAAS)Ultrafast Science2765-87912023-01-01310.34133/ultrafastscience.0040Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order HarmonicsGuanglu Yuan0Ruifeng Lu1Shicheng Jiang2Konstantin Dorfman3Institute of Ultrafast Optical Physics, MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, Department of Applied Physics, Nanjing University of Science and Technology, Nanjing 210094, China.Institute of Ultrafast Optical Physics, MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, Department of Applied Physics, Nanjing University of Science and Technology, Nanjing 210094, China.State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China.State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China.Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic signals different from the case of avoided crossing. The coherence built up when the system crosses the avoided crossing will lead to the oscillatory behavior of the spectrum, while the geometric phase erodes these oscillations in the case of conical intersection. Additionally, the dynamical blueshift and the splitting of the time-resolved spectrum allow capturing the snapshot dynamics with the sub-femtosecond resolution.https://spj.science.org/doi/10.34133/ultrafastscience.0040
spellingShingle Guanglu Yuan
Ruifeng Lu
Shicheng Jiang
Konstantin Dorfman
Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
Ultrafast Science
title Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
title_full Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
title_fullStr Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
title_full_unstemmed Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
title_short Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics
title_sort conical intersection versus avoided crossing geometric phase effect in molecular high order harmonics
url https://spj.science.org/doi/10.34133/ultrafastscience.0040
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AT ruifenglu conicalintersectionversusavoidedcrossinggeometricphaseeffectinmolecularhighorderharmonics
AT shichengjiang conicalintersectionversusavoidedcrossinggeometricphaseeffectinmolecularhighorderharmonics
AT konstantindorfman conicalintersectionversusavoidedcrossinggeometricphaseeffectinmolecularhighorderharmonics