Electronically non-adiabatic processes are essential parts of photochemical process, collisions of excited species, electron transfer processes, and quantum information processing. Various non-adiabatic dynamics metho...Electronically non-adiabatic processes are essential parts of photochemical process, collisions of excited species, electron transfer processes, and quantum information processing. Various non-adiabatic dynamics methods and their numerical implementation have been developed in the last decades. This review summarizes the most significant development of mixed quantum-classical methods and their applications which mainly include the Liouville equa- tion, Ehrenfest mean-field, trajectory surface hopping, and multiple spawning methods. The recently developed quantum trajectory mean-field method that accounts for the decoherence corrections in a parameter-free fashion is discussed in more detail.展开更多
The dissociative chemisorption of N_(2) is the rate-limiting step for ammonia synthesis in industry.Here,we investigated the role of initially vibrational excitation and ro-tational excitation of N_(2) for its reactiv...The dissociative chemisorption of N_(2) is the rate-limiting step for ammonia synthesis in industry.Here,we investigated the role of initially vibrational excitation and ro-tational excitation of N_(2) for its reactivity on the Fe(111)surface,based on a recently developed six-dimensional potential energy surface.Six-dimensional quantum dynamics study was carried out to investi-gate the effect of vibrational excitation for incidence energy below 1.6 eV,due to sig-nificant quantum effects for this reaction.The effects of vibrational and rotational excitations at high incidence energies were revealed by quasiclassical trajectory calculations.We found that raising the translational energy can enhance the dissociation probability to some extent,however,the vibrational excitation or rotational excitation can promote disso-ciation more efficiently than the same amount of translational energy.This study provides valuable insight into the mode-specific dynamics of this heavy diatom-surface reaction.展开更多
The study of optomechanical systems has attracted much attention, most of which are concentrated in the physics in the smallamplitude regime. While in this article, we focus on optomechanics in the extremely-large-amp...The study of optomechanical systems has attracted much attention, most of which are concentrated in the physics in the smallamplitude regime. While in this article, we focus on optomechanics in the extremely-large-amplitude regime and consider both classical and quantum dynamics. Firstly, we study classical dynamics in a membrane-in-the-middle optomechanical system in which a partially reflecting and flexible membrane is suspended inside an optical cavity. We show that the membrane can present self-sustained oscillations with limit cycles in the shape of sawtooth-edged ellipses and exhibit dynamical multistability. Then, we study the dynamics of the quantum fluctuations around the classical orbits. By using the logarithmic negativity, we calculate the evolution of the quantum entanglement between the optical cavity mode and the membrane during the mechanical oscillation. We show that there is some synchronism between the classical dynamical process and the evolution of the quantum entanglement.展开更多
基金supported by the National Key R&D Program of China(No.2017YFB0203405)the National Natural Science Foundation of China(No.21421003)
文摘Electronically non-adiabatic processes are essential parts of photochemical process, collisions of excited species, electron transfer processes, and quantum information processing. Various non-adiabatic dynamics methods and their numerical implementation have been developed in the last decades. This review summarizes the most significant development of mixed quantum-classical methods and their applications which mainly include the Liouville equa- tion, Ehrenfest mean-field, trajectory surface hopping, and multiple spawning methods. The recently developed quantum trajectory mean-field method that accounts for the decoherence corrections in a parameter-free fashion is discussed in more detail.
基金supported by the National Key R&D Program of China(No.2018YFE0203003)the National Natural Science Foundation of China(No.22173099 and No.22173101)the Liaoning Revitalization Talents Program(No.XLYC1907190)。
文摘The dissociative chemisorption of N_(2) is the rate-limiting step for ammonia synthesis in industry.Here,we investigated the role of initially vibrational excitation and ro-tational excitation of N_(2) for its reactivity on the Fe(111)surface,based on a recently developed six-dimensional potential energy surface.Six-dimensional quantum dynamics study was carried out to investi-gate the effect of vibrational excitation for incidence energy below 1.6 eV,due to sig-nificant quantum effects for this reaction.The effects of vibrational and rotational excitations at high incidence energies were revealed by quasiclassical trajectory calculations.We found that raising the translational energy can enhance the dissociation probability to some extent,however,the vibrational excitation or rotational excitation can promote disso-ciation more efficiently than the same amount of translational energy.This study provides valuable insight into the mode-specific dynamics of this heavy diatom-surface reaction.
基金supported by the National Natural Science Foundation of China(Grant Nos.11175094 and 91221205)the National Key Basic Research Program of China(Grant No.2011CB9216002)
文摘The study of optomechanical systems has attracted much attention, most of which are concentrated in the physics in the smallamplitude regime. While in this article, we focus on optomechanics in the extremely-large-amplitude regime and consider both classical and quantum dynamics. Firstly, we study classical dynamics in a membrane-in-the-middle optomechanical system in which a partially reflecting and flexible membrane is suspended inside an optical cavity. We show that the membrane can present self-sustained oscillations with limit cycles in the shape of sawtooth-edged ellipses and exhibit dynamical multistability. Then, we study the dynamics of the quantum fluctuations around the classical orbits. By using the logarithmic negativity, we calculate the evolution of the quantum entanglement between the optical cavity mode and the membrane during the mechanical oscillation. We show that there is some synchronism between the classical dynamical process and the evolution of the quantum entanglement.
