超快强场相干调控氯溴甲烷分子的解离研究

景文泉; 贾利娟; 孙兆鹏; 赵松峰; 束传存

doi:10.7498/aps.73.20241401

摘要

超快强场相干调控分子解离在原子与分子物理、物理化学、量子调控等多个领域引起了重要关注, 在现象理解、机理探究和调控方案等多个方面仍然存在许多值得深入研究的问题. 近期研究表明, 在保持光谱振幅分布不变的条件下, 对最初处于基电子态纯本征态的分子, 通过调制单个超快强紫外激光脉冲的光谱相位分布, 可以有效调控总解离概率和分支比. 本文采用含时量子波包方法, 进一步探讨了光谱相位调控氯溴甲烷(CH₂BrCl)分子的光解离反应, 着重探究了初始振动态对解离反应的影响. 为了凸显超快强场脉冲调控解离机理与弱场的不同, 本文展示了在弱场极限下, 改变单个超快脉冲的谱相位不会影响总解离概率和分支比; 然而在强场极限下, 总解离概率和分支比对单个超快脉冲的谱相位有明显依赖性. 通过分析基电子态振动态布居分布, 发现啁啾脉冲可以有效调控强场极限下诱导的共振拉曼散射(resonance Raman scattering, RRS)现象, 从而导致解离概率和分支比对初始振动态的选择性. 研究结果进一步表明, 通过选择合适的初始振动态并调控啁啾率的值和符号, 可以实现Cl+CH₂Br键的优先断裂. 该研究为理解超快光场相干控制多原子分子光解反应提供了新的视角.

关键词:

Abstract

Coherent control of molecular dissociation in ultrafast strong fields has received considerable attention in various scientific disciplines, such as atomic and molecular physics, physical chemistry, and quantum control. Many fundamental issues still exist regarding the understanding of phenomena, exploration of mechanisms, and development of control strategies. Recent progress has shown that manipulating the spectral phase distribution of a single ultrafast strong ultraviolet laser pulse while maintaining the same spectral amplitude distribution can effectively control the total dissociation probability and branching ratio of molecules initially in the ground state. In this work, the spectral phase control of the photodissociation reaction of chlorobromomethane (CH₂BrCl) is studied in depth by using a time-dependent quantum wave packet method, focusing on the influence of the initial vibrational state on the dissociation reaction. The results show that modifying the spectral phase of a single ultrafast pulse does not influence the total dissociation probability or branching ratio in the weak field limit. However, these factors exhibit significant dependence on the spectral phase of the single ultrafast pulse in the strong field limit. By analyzing the population distribution of vibrational states in the ground electronic state, we observe that chirped pulses can effectively control the resonance Raman scattering (RRS) phenomenon induced in strong fields, thereby selectively affecting the dissociation probability and branching ratio based on initial vibrational states. Furthermore, we demonstrate that by selecting an appropriate initial vibration state and controlling both the value and sign of the chirp rate, it is possible to achieve preferential cleavage of Cl+CH₂Br bonds. This study provides new insights into understanding of ultrafast coherent control of photodissociation reactions in polyatomic molecules.

Keywords:

作者及机构信息

1.
中南大学物理学院, 湖南省超微结构与超快过程重点实验室, 长沙　410083

2.
西北师范大学物理与电子工程学院, 甘肃省原子分子物理与功能材料重点实验室, 兰州　730070

3.
鲁东大学物理与光电工程学院, 理论物理研究所, 烟台　264025

通信作者: 赵松峰, zhaosf@nwnu.edu.cn ; 束传存, cc.shu@csu.edu.cn

基金项目: 国家重点研发计划(批准号: 2022YFA1604204)、国家自然科学基金(批准号: 12164044, 12274470, 61973317)和湖南省杰出青年自然科学基金(批准号: 2022JJ10070)资助的课题.

Authors and contacts

1.
Hunan Key Laboratory of Super Microstructure and Ultrafast Process, School of Physics, Central South University, Changsha 410083, China

2.
Key Laboratory of Atomic and Molecular Physics and Functional Materials of Gansu Province, College of Physics and Electronic Engineering, Northwest Normal University, Lanzhou 730070, China

3.
Institute of Theoretical Physics, School of Physics and Optoelectric Engineering, Ludong University, Yantai 264025, China

Corresponding author: Zhao Song-Feng, zhaosf@nwnu.edu.cn ; Shu Chuan-Cun, cc.shu@csu.edu.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2022YFA1604204), the National Natural Science Foundation of China (Grant Nos. 12164044, 12274470, 61973317), and the Natural Science Foundation of Hunan Province for Distinguished Young Scholars, China (Grant No. 2022JJ10070).

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参考文献

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施引文献

图 1 $ \rm {CH_{2}BrCl} $光解离激光控制示意图　(a)基电子态$ \text{S}_0(\text{a}^{1}\text{A}') $、激发态$ \text{S}_1(\text{a}^{1}\text{A}') $和$ \text{S}_2(\text{a}^{1}\text{A}') $的光解离动力学模型; (b)不同初始振动态$ |\nu'\nu''\rangle $沿着Br—CH₂反应坐标描绘的光解离通道; (c)不同初始振动态$ |\nu'\nu''\rangle $沿Cl—CH₂反应坐标的光解离通道. 其中黑色线、红色线和蓝色线分别表示基电子态$ \text{S}_0(V_0^\text{ad}) $、第一激发电子态$ \text{S}_1(V_1^\text{ad}) $和第二激发电子态$ \text{S}_2(V_2^\text{ad}) $的绝热势能曲线, 红色虚线和黑色虚线分别表示非绝热势能曲线$ V_1^{{\mathrm{di}}} $和$ V_2^{{\mathrm{di}}} $

Fig. 1. Schematic illustration of laser control in the photodissociation process of $ \rm {CH_{2}BrCl} $. (a) The model showcasing the photodissociation dynamics involving the ground electronic state $ \text{S}_0(\text{a}^{1}\text{A}') $, as well as the excited adiabatic electronic states $ \text{S}_1(\text{b}^{1}\text{A}') $ and $ \text{S}_2(\text{c}^{1}\text{A}') $. (b) Photodissociation channel along the Br—CH₂ reaction coordinate for different initial vibrational states $ |\nu'\nu''\rangle $. (c) The channel along the Cl—CH₂ reaction coordinate for the same initial states $ |\nu'\nu''\rangle $. The black, red, and blue solid lines represent the adiabatic potential energy curves of ground electronic state $ \text{S}_0(V_0^\text{ad}) $, the first excited electronic state $ \text{S}_1(V_1^\text{ad}) $, and the second excited electronic state $ \text{S}_2(V_2^\text{ad}) $, respectively. Notably, the red-dashed line and the black-dashed line represent the non-adiabatic potential $ V_1^{\mathrm{di}} $ and $ V_2^{\text{di}} $.

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图 2 CH₂BrCl分子初始振动态为$ |00\rangle $, $ |10\rangle $和$ |20\rangle $时, (a)—(c)基电子态的二维振动本征函数密度分布; (d)—(f)弱场极限下Br+CH₂Cl通道和Cl+CH₂Br通道的含时解离概率(分别用$ P^{\mathrm{Br}} $和$ P^{\mathrm{Cl}} $标记), (g)—(i)相应的含时分支比R; (j)—(l) 强场极限下Br+CH₂Cl和Cl+CH₂Br两个通道的含时解离概率, (m)—(o)相应的含时解离分支比

Fig. 2. For the initial vibrational states of $ |00\rangle $, $ |01\rangle $ and $ |02\rangle $, (a)–(c) two-dimensional vibrational eigenfunction density distributions; (d)–(f) the dissociation probabilities of Br+CH₂Cl and Cl+CH₂Br channels in the weak-field limit (marked with $ P^{\mathrm{Br}} $ and $ P^{\mathrm{Cl}} $, respectively), and (g)–(i) the corresponding time-dependent dissociation branching ratios R; (j)–(l) and (m)–(o) as well as in the strong-field limit.

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图 3 CH₂BrCl分子初始振动态为$ |01\rangle $, $ |02\rangle $和$ |11\rangle $时, (a)—(c)基电子态的二维振动本征函数密度分布; (d)—(f)弱场极限下Br+CH₂Cl通道和Cl+CH₂Br通道的含时解离概率(分别用$ P^{\mathrm{Br}} $和$ P^{\mathrm{Cl}} $标记), (g)—(i)相应的含时分支比R; (j)—(l)强场极限下Br+CH₂Cl和Cl+CH₂Br两个通道的含时解离概率, (m)—(o)相应的含时解离分支比

Fig. 3. For the initial vibrational states of $ |00\rangle $, $ |01\rangle $ and $ |02\rangle $, (a)–(c) two-dimensional vibrational eigenfunction density distributions; (d)–(f) the dissociation probabilities of Br+CH₂Cl and Cl+CH₂Br channels in the weak-field limit (marked with $ P^{\mathrm{Br}} $ and $ P^{\mathrm{Cl}} $, respectively), and (g)–(i) the corresponding time-dependent dissociation branching ratios R; (j)–(l) and (m)–(o) as well as in the strong-field limit.

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图 4 弱场极限下CH₂BrCl分子总解离概率(a)—(f)和分支比(g)—(l)作为啁啾率$ \beta_{0} $和不同初始振动态$ |\nu'\nu''\rangle $的函数

Fig. 4. Dependence of (a)−(f) total dissociation probability and (g)−(l) branching ratio of CH₂BrCl on the chirp rate $ \beta_{0} $ and different initial state $ |\nu'\nu''\rangle $ in the weak-field limit.

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图 5 强场极限下, CH₂BrCl分子总解离概率(a)—(f)和分支比(g)—(l)作为啁啾率$ \beta_{0} $和不同初始振动态$ |\nu'\nu''\rangle $的函数

Fig. 5. (a)–(f) Total dissociation probability and (g)–(l) branching ratio in CH₂BrCl as a function of chirp rate $ \beta_{0} $ and different initial state $ |\nu'\nu''\rangle $ in the strong-field limit.

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图 6 (a) $ |00\rangle $, (b) $ |10\rangle $, (c) $ |20\rangle $, (d) $ |01\rangle $, (e) $ |02\rangle $, (f) $ |11\rangle $分别作为初始振动态时, 基电子态其余振动态末态布居之和$ P(t_{\mathrm{f}}) $随啁啾率$ \beta_{0} $的变化行为. 对于所有不同的初始振动态, $ P(t_{\mathrm{f}}) $的最大值都出现在$ \beta_0=0 $附近

Fig. 6. (a)–(f) Sum of the remaining vibrational states populations $ P(t_{\mathrm{f}}) $ of the ground electronic state for the initial vibrational state (a) $ |00\rangle $, (b) $ |10\rangle $, (c) $ |20\rangle $, (d) $ |01\rangle $, (e) $ |02\rangle $ and (f) $ |11\rangle $ as a function of $ \beta_0 $, respectively. The maximum of $ P(t_{\mathrm{f}}) $ appears near $ \beta_0=0 $ for all different initial vibrational states.

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图 7 随着啁啾率$ \beta_{0} $的改变, (a) $ |00\rangle $, (b) $ |10\rangle $, (c) $ |20\rangle $, (d) $ |01\rangle $, (e) $ |02\rangle $, (f) $ |11\rangle $分别作为初始振动态时, 基电子态不同振动态$ |\nu'\nu''\rangle $的末态布居分布

Fig. 7. Final population distributions of different vibrational states $ |\nu'\nu''\rangle $ for the different initial vibrational state (a) $ |00\rangle $, (b) $ |10\rangle $, (c) $ |20\rangle $, (d) $ |01\rangle $, (e) $ |02\rangle $ and (f) $ |11\rangle $, varying with the chirp rate $ \beta_0 $.

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图 8 强场极限下啁啾脉冲诱导的基电子态振动态共振拉曼散射现象. 初始振动态为$ |00\rangle $, $ |10\rangle $和$ |20\rangle $时, (a)—(i)啁啾率$ \beta_0=0 $, $ \pm30 $ fs²时的初态含时布居$ P_{\nu'\nu''} $、基电子态其余振动态布居之和$ P(t) $、两个激发电子态的含时布居$ P_{1} $和$ P_{2} $

Fig. 8. Resonance Raman scattering phenomenon of the vibrational states of the ground electronic state induced by a chirped pulse in the strong-field limit. For the initial vibrational states of $ |00\rangle $, $ |10\rangle $ and $ |20\rangle $, (a)–(i) the time-dependent populations of the initial state $ P_{\nu'\nu''} $, the total of remaining vibrational states of the ground electronic state $ P(t) $, and the two excited electronic states $ P_{1} $ and $ P_{2} $ with three different chirp rates $ \beta_0=0 $, $ \pm30 $ fs².

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图 9 强场极限下啁啾脉冲诱导的基电子态振动态共振拉曼散射现象. 初始振动态为$ |01\rangle $, $ |02\rangle $和$ |11\rangle $时, (a)—(i)啁啾率$ \beta_0=0 $, $ \pm30 $ fs²时的初态含时布居$ P_{\nu'\nu''} $、基电子态其余振动态布居之和$ P(t) $、两个激发电子态的含时布居$ P_{1} $和$ P_{2} $

Fig. 9. Resonance Raman scattering phenomenon of the vibrational states of the ground electronic state induced by a chirped pulse in the strong-field limit. For the initial vibrational states of $ |01\rangle $, $ |02\rangle $ and $ |11\rangle $, (a)–(i) the time-dependent populations of the initial state $ P_{\nu'\nu''} $, the total of the remaining vibrational states of the ground electronic state $ P(t) $, and the two excited electronic states $ P_{1} $ and $ P_{2} $ with three different chirp rates $ \beta_0=0 $, $ \pm30 $ fs².

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[3]	King W E, Campbell G H, Frank A, Reed B, Schmerge J F, Siwick B J, Stuart B C, Weber P M 2005 J. Appl. Phys. 97 111101 Google Scholar
[4]	Sun Z, Wang C, Zhao W, Yang C 2018 J. Chem. Phys. 149 224307 Google Scholar
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超快强场相干调控氯溴甲烷分子的解离研究