-
原子分子中的光电离时间延迟是阿秒物理学中的基本现象, 它编码了原子分子中的电子结构和动力学信息. 本文主要研究了一氧化碳(CO)分子最高占据轨道$5\sigma \to k\sigma$通道光电离时间延迟的核间距依赖性. 采用基于李普曼-施温格方程的量子散射理论, 计算了不同核间距下的微分光电离截面和时间延迟. 结果表明, 在截面峰值和极小值能量附近, 光电离时间延迟出现明显极值, 且随核间距显著变化. 分波分析表明, $l=3$分波的形状共振是光电离截面与时间延迟出现峰值的原因, 其有效势场的核间距依赖性决定了光电离时间延迟的峰值能量位置和大小的变化. 在截面极小值附近, 利用双中心干涉模型解释了沿O端和C端出射时的光电离时间延迟分别出现正、负峰值的现象, 并阐明了其随核间距变化的物理机制. 本文的工作揭示了CO分子光电离时间延迟的核间距依赖规律, 有助于推动光电离时间延迟在分子结构及电子动力学探测中的应用.Photoionization time delay in atoms and molecules is a fundamental phenomenon in attosecond physics, encoding essential information about electronic structure and dynamics. Compared with atoms, molecules exhibit anisotropic potentials and additional nuclear degrees of freedom, which make the interpretation of molecular photoionization time delays more intricate but also more informative. In this work, we investigate the dependence of the photoionization time delay on the internuclear distance in the $5\sigma \to k\sigma$ ionization channel of carbon monoxide (CO) molecules. The molecular ground state is obtained using the Hartree–Fock method, and the photoionization process is treated within quantum scattering theory based on the iterative Schwinger variational principle of the Lippmann–Schwinger equation. Numerical calculations are performed with the ePolyScat program to obtain molecular-frame differential photoionization cross sections and time delays at various internuclear distances. Our results show that the extrema of the photoionization time delay occur near the peaks and dips of the differential cross section and shift toward lower energies as the internuclear distance $R$ increases. At low energies, the time delay along the oxygen end increases with $R$, while that along the carbon end decreases, which is attributed to the asymmetric charge distribution and the resulting short-range potential difference between the two atomic sites. Around the shape-resonance energy region, both cross section and time delay display pronounced peaks associated with an $l=3$ quasi-bound state. As $R$ increases, the effective potential barrier broadens, the quasi-bound state energy moves to lower values, and its lifetime becomes longer, leading to enhanced resonance amplitude and increased time delay. In the high-energy region, opposite-sign peaks of time delay are found along the O and C directions, corresponding to minima in the cross section. These features are well explained by a two-center interference model, where increasing $R$ shifts the interference minima and the associated time-delay peaks toward lower energies. This study provides deeper insights into the photoionization dynamics of CO molecules, accounting for the role of nuclear motion, and offers valuable references for studying the photoelectron dynamics of more complex molecular systems.
-
[1] Wigner E P 1955 Phys. Rev. 98 145
[2] Smith F T 1960 Phys. Rev. 119 2098
[3] Hargrove L E, Fork R L, Pollack M A 1964 Appl. Phys. Lett. 5 4
[4] Fork R, Greene B, Shank C 1981 In Conference on Lasers and Electro-Optics (Washington, D.C., USA: Optica Publishing Group), p WL1
[5] Strickland D, Mourou G 1985 Opt. Commun. 56 219
[6] Paul P M, Toma E S, Breger P, Mullot G, Augé F, Balcou P, Muller H G, Agostini P 2001 Science 292 1689
[7] Hentschel M, Kienberger R, Spielmann C, Reider G A, Milosevic N, Brabec T, Corkum P, Heinzmann U, Drescher M, Krausz F 2001 Nature 414 509
[8] Wang X W, Xiao F, Wang J C, Wang L, Zhang B, Liu J L, Zhao J, Zhao Z X 2024 Ultrafast Sci. 4 0080
[9] Itatani J, Quéré F, Yudin G L, Ivanov M Y, Krausz F, Corkum P B 2002 Phys. Rev. Lett. 88 173903
[10] Muller H G 2002 Appl. Phys. B 74 s17
[11] Schultze M, Fieß M, Karpowicz N, Gagnon J, Korbman M, Hofstetter M, Neppl S, Cavalieri A L, Komninos Y, Mercouris T, Nicolaides C A, Pazourek R, Nagele S, Feist J, Burgdörfer J, Azzeer A M, Ernstorfer R, Kienberger R, Kleineberg U, Goulielmakis E, Krausz F, Yakovlev V S 2010 Science 328 1658
[12] Pazourek R, Nagele S, Burgdörfer J 2015 Rev. Mod. Phys. 87 765
[13] Kheifets A S 2023 J. Phys. B: At. Mol. Opt. Phys. 56 022001
[14] Magrakvelidze M, Madjet M E A, Chakraborty H S 2016 Phys. Rev. A 94 013429
[15] Alexandridi C, Platzer D, Barreau L, Busto D, Zhong S Y, Turconi M, Neoričić L, Laurell H, Arnold C L, Borot A, Hergott J F, Tcherbakoff O, Lejman M, Gisselbrecht M, Lindroth E, L’ Huillier A, Dahlström J M, Salières P 2021 Phys. Rev. Res. 3 L012012
[16] Zhong S Y, Vinbladh J, Busto D, Squibb R J, Isinger M, Neoričić L, Laurell H, Weissenbilder R, Arnold C L, Feifel R, Dahlström J M, Wendin G, Gisselbrecht M, Lindroth E, L’ Huillier A 2020 Nat. Commun. 11 5042
[17] Ossiander M, Siegrist F, Shirvanyan V, Pazourek R, Sommer A, Latka T, Guggenmos A, Nagele S, Feist J, Burgdörfer J, Kienberger R, Schultze M 2017 Nat. Phys. 13 280
[18] Cirelli C, Marante C, Heuser S, Petersson C L M, Galán ff J, Argenti L, Zhong S Y, Busto D, Isinger M, Nandi S, Maclot S, Rading L, Johnsson P, Gisselbrecht M, Lucchini M, Gallmann L, Dahlström J M, Lindroth E, L’ Huillier A, Martín F, Keller U 2018 Nat. Commun. 9 955
[19] Holzmeier F, Joseph J, Houver J C, Lebech M, Dowek D, Lucchese R R 2021 Nat. Commun. 12 7343
[20] Huppert M, Jordan I, Baykusheva D, Von Conta A, Wörner H J 2016 Phy. Rev. Lett. 117 093001
[21] Gong X C, Jiang W Y, Tong J H, Qiang J J, Lu P F, Ni H C, Lucchese R, Ueda K, Wu J 2022 Phys. Rev. X 12 011002
[22] Nandi S, Plésiat É, Zhong S Y, Palacios A, Busto D, Isinger M, Neoričić L, Arnold C, Squibb R, Feifel R, et al. 2020 Sci. Adv. 6 eaba7762
[23] Gong X C, Plésiat É, Palacios A, Heck S, Martín F, Wörner H J 2023 Nat. Commun. 14 4402
[24] Desrier A, Berkane M, Lévêque C, Taïeb R, Caillat J 2024 Phys. Rev. A 109 053106
[25] Werner H, Knowles P J, Knizia G, Manby F R, Schütz M 2012 WIREs Comput. Mol. Sci. 2 242
[26] Werner H J, Knowles P J, Manby F R, Black J A, Doll K, Heßelmann A, Kats D, Köhn A, Korona T, Kreplin D A, Ma Q L, Miller T F, Mitrushchenkov A, Peterson K A, Polyak I, Rauhut G, Sibaev M 2020 J. Chem. Phys. 152 144107
[27] Werner H J, Knowles P J, Celani P, Györffy W, Hesselmann A, Kats D, Knizia G, Köhn A, Korona T, Kreplin D, Lindh R, Ma Q L, Manby F R, Mitrushenkov A, Rauhut G, Schütz M, Shamasundar K R, Adler T B, Amos R D, Bennie S J, Bernhardsson A, Berning A, Black J A, Bygrave P J, Cimiraglia R, Cooper D L, Coughtrie D, Deegan M J O, Dobbyn A J, Doll K, Dornbach M, Eckert F, Erfort S, Goll E, Hampel C, Hetzer G, Hill J G, Hodges M, Hrenar T, Jansen G, Köppl C, Kollmar C, Lee S J R, Liu Y, Lloyd A W, Mata R A, May A J, Mussard B, McNicholas S J, Meyer W, Miller III T F, Mura M E, Nicklass A, O’Neill D P, Palmieri P, Peng D, Peterson K A, Pflüger K, Pitzer R, Polyak I, Reiher M, Richardson J O, Robinson J B, Schröder B, Schwilk M, Shiozaki T, Sibaev M, Stoll H, Stone A J, Tarroni R, Thorsteinsson T, Toulouse J, Wang M, Welborn M, Ziegler B. See https://www.molpro.net
[28] Lucchese R R, Takatsuka K, McKoy V 1986 Phys. Rep. 131 147
[29] Gianturco F A, Lucchese R R, Sanna N 1994 J. Chem. Phys. 100 6464
[30] Natalense A P P, Lucchese R R 1999 J. Chem. Phys. 111 5344
[31] Baykusheva D, Wörner H J 2017 J. Chem. Phys. 146 124306
[32] Gong X C, Heck S, Jelovina D, Perry C, Zinchenko K, Lucchese R, Wörner H J 2022 Nature 609 507
[33] Biswas S, Förg B, Ortmann L, Schötz J, Schweinberger W, Zimmermann T, Pi L W, Baykusheva D, Masood H A, Liontos I, Kamal A M, Kling N G, Alharbi A F, Alharbi M, Azzeer A M, Hartmann G, Wörner H J, Landsman A S, Kling M F 2020 Nat. Phys. 16 778
[34] Lu T, Chen F W 2012 J. Comput. Chem. 33 580
[35] Humphrey W, Dalke A, Schulten K 1996 J. Mol. Graph. 14 33
[36] Lucchese R R, Gianturco F 1996 Int. Rev. Phys. Chem. 15 429
[37] Cohen H D, Fano U 1966 Phys. Rev. 150 30
[38] Ueda K, Liu X J, Prümper G, Lischke T, Tanaka T, Hoshino M, Tanaka H, Minkov I, Kimberg V, Gel’ mukhanov F 2006 Chem. Phys. 329 329
[39] Liao Y J, Zhou Y M, Pi L W, Ke Q H, Liang J T, Zhao Y, Li M, Lu P X 2021 Phys. Rev. A 104 013110
计量
- 文章访问数: 26
- PDF下载量: 1
- 被引次数: 0
下载:
