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Main Authors: Zhang, Xuanchao, Ye, Yang-Cheng, Zhang, Panpan, Duan, Xiangmei, Miller, R. J. Dwayne, Zheng, Fulu, Jha, Ajay, Duan, Hong-Guang
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2512.22912
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author Zhang, Xuanchao
Ye, Yang-Cheng
Zhang, Panpan
Duan, Xiangmei
Miller, R. J. Dwayne
Zheng, Fulu
Jha, Ajay
Duan, Hong-Guang
author_facet Zhang, Xuanchao
Ye, Yang-Cheng
Zhang, Panpan
Duan, Xiangmei
Miller, R. J. Dwayne
Zheng, Fulu
Jha, Ajay
Duan, Hong-Guang
contents In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.
format Preprint
id arxiv_https___arxiv_org_abs_2512_22912
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Controlling Nonadiabatic Transitions Through Engineered Ultrafast Laser Fields at Conical Intersections
Zhang, Xuanchao
Ye, Yang-Cheng
Zhang, Panpan
Duan, Xiangmei
Miller, R. J. Dwayne
Zheng, Fulu
Jha, Ajay
Duan, Hong-Guang
Quantum Physics
Optics
In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.
title Controlling Nonadiabatic Transitions Through Engineered Ultrafast Laser Fields at Conical Intersections
topic Quantum Physics
Optics
url https://arxiv.org/abs/2512.22912