基于多组态含时Hartree-Fock方法研究电子关联对于H2分子强场电离的影响

张斌; 赵健; 赵增秀

doi:10.7498/aps.67.20172701

摘要

发展了三维的处理双原子分子非微扰电子动力学的多组态含时Hartree-Fock方法，并利用该方法研究了电子关联对于H2分子强场电离概率的影响.该方法采用能够精确处理双中心库仑势的椭球坐标系，以及减小双电子积分计算量的有限元-离散变量基函数方法.利用多组态含时Hartree-Fock方法计算了H2分子随分子取向角度变化的XUV光电离结果，并通过与单组态结果的对比研究了电子关联对于单电离和双电离概率的不同影响.研究表明，电子关联对于单电离过程影响很小，而在双电离过程中则发挥了重要作用，导致了电离概率的减小.该方法为进一步研究强场物理过程中的电子关联效应奠定了基础.

关键词:

Abstract

Electron correlation plays an important role in the multielectron interactions of many physical and chemical processes.The investigation of correlation effects in the non-perturbative electronic dynamics (e.g.non-sequential double ionization) when atoms and molecules are subjected to strong laser fields requires non-perturbative theoretical treatments. The direct numerical integration of the time-dependent Schrödinger equation successfully explains many experimental results,but it is computationally prohibitive for systems with more than two electrons.There is clearly a need for a theory which can treat correlation dynamics self-consistently in strong time-dependent electric fields.In this paper we develop a three-dimensional multiconfiguration time-dependent Hartree-Fock method,which can be applied to the non-perturbative electronic dynamics for diatomic molecules,and it can also investigate the effect of electron correlation in strong-field ionization of H2 molecules.This method adopts the prolate spheroidal coordinates (which can treat the two-center Coulomb potential accurately) and the finite-element method together with discrete-variable representation (which lowers the calculation burden from two-electron integrations).For the temporal propagation,we use the efficient short iterative Lanczos algorithm for the equation which governs the configuration expansion coefficients,while an eight-order Runge-Kutta (RK) method and an Bulirsch-Stoer (BS) extrapolation method,both with adaptive precision controls,are implemented to solve the nonlinear orbital equation.While both methods yield correct results,the BS method displays a better stability in the realtime propagation,while the RK method demands less computation.The alignment-dependent ionization probabilities of H2 molecules in intense extreme ultraviolet pulses are calculated.Comparisons between multi-configuration and single-configuration results show that electron correlation has little effect on the single ionization process,but it plays an important role in double ionization,leading to the decrease in the ionization probability.The double ionization probability from the single-configuration space 1σ is about three times larger that from 4σ1π.The ionization probability increases monotonically when the alignment angle increases from 0° to 90°, yielding a ratio of 2.6(1.5) between 90° and 0° for the double (single) ionization process.This method presents the basis for the future study of electron correlation in strong-field processes.

Keywords:

multiconfiguration time-dependent Hartree-Fock /
electron correlation /
strong-field ionization /
hydrogen molecules

作者及机构信息

1.
西北核技术研究所, 西安 710024;

2.
国防科技大学物理系, 长沙 410073

通信作者: 张斌, zhang_bin@nudt.edu.cn

基金项目: 国家重点基础研究发展计划（批准号：2013CB922203）、国家自然科学基金（批准号：11374366）、国防科技大学优秀研究生创新资助（批准号：B110204）和湖南省研究生创新资助（批准号：CX2011B010）资助的课题.

Authors and contacts

1.
Northwest Institute of Nuclear Technology, Xi'an 710024, China;

2.
Department of Physics, National University of Defense Technology, Changsha 410073, China

Corresponding author: Zhang Bin, zhang_bin@nudt.edu.cn

Funds: Project supported by the National Basic Research Program of China (Grant No. 2013CB922203), the National Natural Science Foundation of China (Grant No. 11374366), the Innovation Foundation of NUDT, China (Grant No. B110204), and the Hunan Provincial Innovation Foundation For Postgraduate, China (Grant No. CX2011B010).

参考文献

[1]	Xu G X, Li L M, Wang D M, Chen M B 2009 Quantum Chemistry:Fundamental Principle and Ab-initio Calculation Method (2nd Ed.) (Vol. 1) (Beijing:Science Press) pp869-874 (in Chinese)[徐光宪, 黎乐民, 王德民, 陈敏伯 2009 量子化学——基本原理和从头计算法(下) (第二版)(北京:科学出版社) 第869–874页]
[2]	Becker W, Liu X J, Ho P J, Eberly J H 2012 Rev. Mod. Phys. 84 1011
[3]	Zhao L, Zhang Q, Dong J W, L H, Xu H F 2016 Acta Phys. Sin. 65 223201 (in Chinese)[赵磊, 张琦, 董敬伟, 吕航, 徐海峰 2016 物理学报 65 223201]
[4]	Jin F C, Wang B B 2016 Acta Phys. Sin. 65 224205 (in Chinese)[金发成, 王兵兵 2016 物理学报 65 224205]
[5]	Hu S X 2013 Phys. Rev. Lett. 111 123003
[6]	Ye D F, Liu X, Liu J 2008 Phys. Rev. Lett. 101 233003
[7]	Brabec T, Krausz F 2000 Rev. Mod. Phys. 72 545
[8]	Posthumus J H 2004 Rep. Progr. Phys. 67 623
[9]	Xiao X R, Wang M X, Li M, Geng J W, Liu Y Q, Peng L Y 2016 Acta Phys. Sin. 65 220203 (in Chinese)[肖相如, 王慕雪, 黎敏, 耿基伟, 刘运全, 彭良友 2016 物理学报 65 220203]
[10]	Zhang Z, Peng L Y, Xu M H, Starace A F, Morishita T, Gong Q H 2011 Phys. Rev. A 84 043409
[11]	Guan X, Bartschat K, Schneider B I 2011 Phys. Rev. A 83 043403
[12]	Stapelfeldt H 2003 Rev. Mod. Phys. 75 543
[13]	Kulander K 1987 Phys. Rev. A 36 2726
[14]	Marques M A L, Ullrich C A, Nogueira F, Rubio A, Burke K, Gross E K U 2006 Time-Dependent Density Functional Theory (Heidelberg, Berlin:Springer) pp1-13
[15]	Hochstuhl D, Bonitz M 2012 Phys. Rev. A 86 053424
[16]	Zanghellini J, Kitzler M, Fabian C, Brabec T, Scrinzi A 2003 Laser Phys. 13 1064
[17]	Kitzler M, Zanghellini J, Jungreuthmayer C, Smits M, Scrinzi, Brabec T 2004 Phys. Rev. A 70 041401
[18]	Caillat J, Zanghellini J, Kitzler M, Koch O, Kreuzer W, Scrinzi A 2005 Phys. Rev. A 71 012712
[19]	Kato T, Kono H 2004 Chem. Phys. Lett. 392 533
[20]	Hochstuhl D, Bonitz M 2011 J. Chem. Phys. 134 084106
[21]	Haxton D J, Lawler K V, McCurdy C W 2011 Phys. Rev. A 83 063416
[22]	Liao C T, Li X, Haxton D J, Rescigno T N, Lucchese R R, McCurdy C W, Sandhu A 2017 Phys. Rev. A 95 043427
[23]	Zhang B, Yuan J M, Zhao Z X 2015 Comput. Phys. Commun. 194 84
[24]	Lamb W E, Schlicher R R, Scully M O 1987 Phys. Rev. A 36 2763
[25]	Abramowitz M, Stegun I A 1972 Handbook of Mathmatical Functions (Washington:Dover) p752
[26]	Rescigno T, McCurdy C 2011 Phys. Rev. A 62 032706
[27]	Press W H, Teukolsky S A, Vetterling W T, Flannery B P 2007 Numerical Recipes (3rd Ed.) (New York:Cambridge University Press) pp179-193, 899-928
[28]	Park T J, Light J C 1986 J. Chem. Phys. 85 5870
[29]	Weinhold F, Landis C R 2001 Chem. Educ. Res. Pract. 2 91
[30]	Zhang B, Yuan J M, Zhao Z X 2013 Phys. Rev. Lett. 111 163001
[31]	Zhang B, Yuan J M, Zhao Z X 2012 Phys. Rev. A 85 033421

施引文献

[1]	Xu G X, Li L M, Wang D M, Chen M B 2009 Quantum Chemistry:Fundamental Principle and Ab-initio Calculation Method (2nd Ed.) (Vol. 1) (Beijing:Science Press) pp869-874 (in Chinese)[徐光宪, 黎乐民, 王德民, 陈敏伯 2009 量子化学——基本原理和从头计算法(下) (第二版)(北京:科学出版社) 第869–874页]
[2]	Becker W, Liu X J, Ho P J, Eberly J H 2012 Rev. Mod. Phys. 84 1011
[3]	Zhao L, Zhang Q, Dong J W, L H, Xu H F 2016 Acta Phys. Sin. 65 223201 (in Chinese)[赵磊, 张琦, 董敬伟, 吕航, 徐海峰 2016 物理学报 65 223201]
[4]	Jin F C, Wang B B 2016 Acta Phys. Sin. 65 224205 (in Chinese)[金发成, 王兵兵 2016 物理学报 65 224205]
[5]	Hu S X 2013 Phys. Rev. Lett. 111 123003
[6]	Ye D F, Liu X, Liu J 2008 Phys. Rev. Lett. 101 233003
[7]	Brabec T, Krausz F 2000 Rev. Mod. Phys. 72 545
[8]	Posthumus J H 2004 Rep. Progr. Phys. 67 623
[9]	Xiao X R, Wang M X, Li M, Geng J W, Liu Y Q, Peng L Y 2016 Acta Phys. Sin. 65 220203 (in Chinese)[肖相如, 王慕雪, 黎敏, 耿基伟, 刘运全, 彭良友 2016 物理学报 65 220203]
[10]	Zhang Z, Peng L Y, Xu M H, Starace A F, Morishita T, Gong Q H 2011 Phys. Rev. A 84 043409
[11]	Guan X, Bartschat K, Schneider B I 2011 Phys. Rev. A 83 043403
[12]	Stapelfeldt H 2003 Rev. Mod. Phys. 75 543
[13]	Kulander K 1987 Phys. Rev. A 36 2726
[14]	Marques M A L, Ullrich C A, Nogueira F, Rubio A, Burke K, Gross E K U 2006 Time-Dependent Density Functional Theory (Heidelberg, Berlin:Springer) pp1-13
[15]	Hochstuhl D, Bonitz M 2012 Phys. Rev. A 86 053424
[16]	Zanghellini J, Kitzler M, Fabian C, Brabec T, Scrinzi A 2003 Laser Phys. 13 1064
[17]	Kitzler M, Zanghellini J, Jungreuthmayer C, Smits M, Scrinzi, Brabec T 2004 Phys. Rev. A 70 041401
[18]	Caillat J, Zanghellini J, Kitzler M, Koch O, Kreuzer W, Scrinzi A 2005 Phys. Rev. A 71 012712
[19]	Kato T, Kono H 2004 Chem. Phys. Lett. 392 533
[20]	Hochstuhl D, Bonitz M 2011 J. Chem. Phys. 134 084106
[21]	Haxton D J, Lawler K V, McCurdy C W 2011 Phys. Rev. A 83 063416
[22]	Liao C T, Li X, Haxton D J, Rescigno T N, Lucchese R R, McCurdy C W, Sandhu A 2017 Phys. Rev. A 95 043427
[23]	Zhang B, Yuan J M, Zhao Z X 2015 Comput. Phys. Commun. 194 84
[24]	Lamb W E, Schlicher R R, Scully M O 1987 Phys. Rev. A 36 2763
[25]	Abramowitz M, Stegun I A 1972 Handbook of Mathmatical Functions (Washington:Dover) p752
[26]	Rescigno T, McCurdy C 2011 Phys. Rev. A 62 032706
[27]	Press W H, Teukolsky S A, Vetterling W T, Flannery B P 2007 Numerical Recipes (3rd Ed.) (New York:Cambridge University Press) pp179-193, 899-928
[28]	Park T J, Light J C 1986 J. Chem. Phys. 85 5870
[29]	Weinhold F, Landis C R 2001 Chem. Educ. Res. Pract. 2 91
[30]	Zhang B, Yuan J M, Zhao Z X 2013 Phys. Rev. Lett. 111 163001
[31]	Zhang B, Yuan J M, Zhao Z X 2012 Phys. Rev. A 85 033421

[1]	葛振杰, 苏旭, 白丽华. 反旋双色椭圆偏振激光场中Ar原子的非序列双电离. 物理学报, 2024, 73(9): 093201. doi: 10.7498/aps.73.20231583
[2]	刘义俊, 陈以威, 朱雨剑, 黄焱, 安冬冬, 李庆鑫, 甘祺康, 朱旺, 宋珺威, 王开元, 魏凌楠, 宗其军, 刘硕涵, 李世伟, 刘芝, 张琪, 徐瑛海, 曹新宇, 杨奥, 王浩林, 杨冰, Andy Shen, 于葛亮, 王雷. 转角双层-双层石墨烯中同位旋极化的C = 4陈绝缘态. 物理学报, 2023, 72(14): 147303. doi: 10.7498/aps.72.20230497
[3]	钟国华, 林海青. 芳香超导体: 电-声耦合与电子关联. 物理学报, 2023, 72(23): 237403. doi: 10.7498/aps.72.20231751
[4]	李盈傧, 张可, 陈红梅, 康帅杰, 李整法, 程建国, 吴银梦, 翟春洋, 汤清彬, 许景焜, 余本海. 空间非均匀激光场驱动的原子非次序双电离. 物理学报, 2023, 72(16): 163201. doi: 10.7498/aps.72.20230548
[5]	苏杰, 刘子超, 廖健颖, 李盈傧, 黄诚. 反旋双色椭偏场中Ar非次序双电离电子关联的强度依赖. 物理学报, 2022, 71(19): 193201. doi: 10.7498/aps.71.20221044
[6]	宁辉, 王凯程, 王少萌, 宫玉彬. 强场太赫兹波作用下氢气分子振动动力学研究. 物理学报, 2021, 70(24): 243101. doi: 10.7498/aps.70.20211482
[7]	唐富明, 刘凯, 杨溢, 屠倩, 王凤, 王哲, 廖青. 基于图形处理器加速数值求解三维含时薛定谔方程. 物理学报, 2020, 69(23): 234202. doi: 10.7498/aps.69.20200700
[8]	黄诚, 钟明敏, 吴正茂. 强场非次序双电离中再碰撞动力学的强度依赖. 物理学报, 2019, 68(3): 033201. doi: 10.7498/aps.68.20181811
[9]	林桐, 胡蝶, 时立宇, 张思捷, 刘妍琦, 吕佳林, 董涛, 赵俊, 王楠林. 铁基超导体Li0.8Fe0.2ODFeSe的红外光谱研究. 物理学报, 2018, 67(20): 207102. doi: 10.7498/aps.67.20181401
[10]	吴绍全, 方栋开, 赵国平. 电子关联效应对平行双量子点系统磁输运性质的影响. 物理学报, 2015, 64(10): 107201. doi: 10.7498/aps.64.107201
[11]	何曼丽, 王晓, 张明, 王黎, 宋蕊. 低温等离子体中H2(D2和T2)的振动分布. 物理学报, 2014, 63(12): 125201. doi: 10.7498/aps.63.125201
[12]	刘玉柱, Gerber Thomas, Knopp Gregor. 利用强场多光子电离技术实现对多原子分子离子振动量子态的光学操控. 物理学报, 2014, 63(24): 244208. doi: 10.7498/aps.63.244208
[13]	李文亮, 张季, 姚洪斌. 三种不同表象下多组态含时Hartree Fock理论实现方案. 物理学报, 2013, 62(12): 123202. doi: 10.7498/aps.62.123202
[14]	何曼丽, 王晓, 高思峰. 电子与氢及其同位素分子碰撞的非解离性电离截面研究. 物理学报, 2012, 61(4): 043404. doi: 10.7498/aps.61.043404
[15]	余本海, 李盈傧. 椭圆偏振激光脉冲驱动的氩原子非次序双电离对激光强度的依赖. 物理学报, 2012, 61(23): 233202. doi: 10.7498/aps.61.233202
[16]	余本海, 李盈傧, 汤清彬. 椭圆偏振激光脉冲驱动的氩原子非次序双电离. 物理学报, 2012, 61(20): 203201. doi: 10.7498/aps.61.203201
[17]	张东玲, 汤清彬, 余本海, 陈东. 碰撞阈值下氩原子非次序双电离. 物理学报, 2011, 60(5): 053205. doi: 10.7498/aps.60.053205
[18]	王玮, 孙家法, 刘楣, 刘甦. β型烧绿石结构氧化物超导体AOs2O6(A=K,Rb,Cs)电子能带结构的第一性原理计算. 物理学报, 2009, 58(8): 5632-5639. doi: 10.7498/aps.58.5632
[19]	傅荣堂, 孙鑫. 氢链中的Peierls机理(Ⅰ)——Hartree-Fock解的二聚化. 物理学报, 1992, 41(2): 213-220. doi: 10.7498/aps.41.213
[20]	冯伟国, 孙鑫. 金属表面的电子关联函数(Ⅰ)——Hartree-Fock近似. 物理学报, 1984, 33(12): 1719-1727. doi: 10.7498/aps.33.1719

计量

文章访问数: 7069
PDF下载量: 220
被引次数: 0

姓名
邮箱
手机号码
标题
留言内容
验证码

搜索

留言板