Experimental manipulation of fine structures in high harmonic spectrum of aligned CO2 molecules

doi:10.1088/1674-1056/adab65

中国物理B ›› 2025, Vol. 34 ›› Issue (6): 63301-063301.doi: 10.1088/1674-1056/adab65

所属专题： SPECIAL TOPIC — Ultrafast physics in atomic, molecular and optical systems

Experimental manipulation of fine structures in high harmonic spectrum of aligned CO₂ molecules

Ge-Wen Wang(王革文)¹, Yi-Wen Zhao(赵逸文)¹, Yi-Chen Wang(王一琛)¹, Jing Ma(马婧)¹, Bo-Dun Liu(刘博敦)¹, Wei Jiang(姜威)¹, Hong-Jing Liang(梁红静)^2,†, and Ri Ma(马日)^1,‡

1 Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China;
2 College of Science, Jilin Institute of Chemical Technology, Jilin 132022, China

收稿日期:2024-11-16 修回日期:2025-01-07 接受日期:2025-01-17 出版日期:2025-05-16 发布日期:2025-05-16
通讯作者: Hong-Jing Liang, Ri Ma E-mail:lianghongjing@jlict.edu.cn;rma@jlu.edu.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant Nos. 92250306 and 12304302), the Natural Science Foundation of Jilin Province, China (Grant Nos. YDZJ202101ZYTS157 and YDZJ202201ZYTS314), the Scientific Research Foundation of Jilin Province Education Department, China (Grant No. JJKH20230283KJ).

Experimental manipulation of fine structures in high harmonic spectrum of aligned CO₂ molecules

1 Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China;
2 College of Science, Jilin Institute of Chemical Technology, Jilin 132022, China

Received:2024-11-16 Revised:2025-01-07 Accepted:2025-01-17 Online:2025-05-16 Published:2025-05-16
Contact: Hong-Jing Liang, Ri Ma E-mail:lianghongjing@jlict.edu.cn;rma@jlu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grant Nos. 92250306 and 12304302), the Natural Science Foundation of Jilin Province, China (Grant Nos. YDZJ202101ZYTS157 and YDZJ202201ZYTS314), the Scientific Research Foundation of Jilin Province Education Department, China (Grant No. JJKH20230283KJ).

摘要/Abstract

摘要： Molecular high-order harmonic spectroscopy is a significant advancement in ultrafast science, enabling the measurement of multielectron dynamics with attosecond temporal resolution. The fine structures observed in the molecular harmonic spectrum provide crucial insights into the structural or multielectron dynamical effects induced by intense laser fields. In this study, we measure the high-order harmonic spectrum of aligned CO$_{2}$ molecules contributed from short trajectories. Two distinct groups of minima are identified in the plateau region. Our findings indicate that the deeper-lying molecular orbitals and two-center interference play significant roles in molecular harmonic generation. The results pave the way for advancing the understanding of multielectron dynamics in polyatomic molecules under intense laser fields.

关键词: high-order harmonic generation, aligned molecule, multielectron effect

Abstract: Molecular high-order harmonic spectroscopy is a significant advancement in ultrafast science, enabling the measurement of multielectron dynamics with attosecond temporal resolution. The fine structures observed in the molecular harmonic spectrum provide crucial insights into the structural or multielectron dynamical effects induced by intense laser fields. In this study, we measure the high-order harmonic spectrum of aligned CO$_{2}$ molecules contributed from short trajectories. Two distinct groups of minima are identified in the plateau region. Our findings indicate that the deeper-lying molecular orbitals and two-center interference play significant roles in molecular harmonic generation. The results pave the way for advancing the understanding of multielectron dynamics in polyatomic molecules under intense laser fields.

Key words: high-order harmonic generation, aligned molecule, multielectron effect

中图分类号: (Spectra induced by strong-field or attosecond laser irradiation)

33.20.Xx

33.80.Rv (Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states)) 42.65.Ky (Frequency conversion; harmonic generation, including higher-order harmonic generation)

Ge-Wen Wang(王革文), Yi-Wen Zhao(赵逸文), Yi-Chen Wang(王一琛), Jing Ma(马婧), Bo-Dun Liu(刘博敦), Wei Jiang(姜威), Hong-Jing Liang(梁红静), and Ri Ma(马日). Experimental manipulation of fine structures in high harmonic spectrum of aligned CO₂ molecules[J]. 中国物理B, 2025, 34(6): 63301-063301.

参考文献

[1] Corkum P B 1993 Phys. Rev. Lett. 71 1994
[2] Mairesse Y, Higuet J, Dudovich N, Shafir D, Fabre B, Mével E, Constant E, Patchkovskii S, Walters Z, Ivanov M Yu and Smirnova O 2010 Phys. Rev. Lett. 104 213601
[3] Kraus P M, Mignolet B, Baykusheva D, Rupenyan A, Horný L, Penka E F, Grassi G, Tolstikhin O I, Schneider J, Jensen F, Madsen L B, Bandrauk A D, Remacle F and Wörner H J 2015 Science 350 790
[4] Smirnova O, Mairesse Y, Patchkovskii S, Dudovich N, Villeneuve D, Corkum P and Ivanov M Yu 2009 Nature 460 972
[5] Zhang B, Zhao J and Zhao Z X 2018 Chin. Phys. Lett. 35 043201
[6] He L X, He Y Q, Sun S Q, Goetz E, Le A T, Zhu X S, Lan P F, Lu P X and Lin C D 2023 Adv. Photonics 5 56001
[7] Huang Y D, Zhao J, Shu Z, Zhu Y L, Liu J L, Dong W P, Wang X W, Lü Z H, Zhang D W, Yuan J M, Chen J and Zhao Z X 2021 Ultrafast Science 2021 9837107
[8] Wagner N L, Wüest A, Christov I P, Popmintchev T, Zhou X, Murnane M M and Kapteyn H C 2006 Proc. Natl. Acad. Sci. USA 103 13279
[9] Li W, Zhou X, Lock R, Patchkovskii S, Stolow A, Kapteyn H C and Murnane M M 2008 Science 322 1207
[10] Baker S, Robinson J S, Haworth C A, Teng H, Smith R A, Chirila C C, Lein M, Tisch J W G and Marangos J P 2006 Science 312 424
[11] He L X, Yuen C H, He Y Q, Sun S Q, Goetz E, Le A T, Deng Y, Xu C Q, Lan P F, Lu P X and Lin C D 2024 Phys. Rev. Lett. 133 23201
[12] Itatani J, Levesque J, Zeidler D, Niikura H, Pépin H, Kieffer J C, Corkum P B and Villeneuve D M 2004 Nature 432 867
[13] Qin M Y, Zhu X S, Zhang Q B and Lu P X 2012 Opt. Lett. 37 5208
[14] Lin C D and Tong X M 2006 J. Photochem. Photobiol., A: Chem. 182 213
[15] Haessler S, Caillat J, Boutu W, Giovanetti-Teixeira C, Ruchon T, Auguste T, Diveki Z, Breger P, Maquet A, Carré B, Taïeb R and Salières P 2010 Nat. Phys. 6 200
[16] Vozzi C, Negro M, Calegari F, Sansone G, Nisoli M, De Silvestri S and Stagira S 2011 Nat. Phys. 7 822
[17] Wörner H J, Niikura H, Bertrand J B, Corkum P B and Villeneuve D M 2009 Phys. Rev. Lett. 102 103901
[18] Lein M, Hay N, Velotta R, Marangos J P and Knight P L 2002 Phys. Rev. Lett. 88 183903
[19] Tuthill D R, Scarborough T D, Gorman T T, Hamer K A, Jones R R, Gaarde M B, Lopata K, Mauger F, Schafer K J and DiMauro L F 2022 J. Phys. Chem. A 126 8588
[20] Torres R, Siegel T, Brugnera L, Procino I, Underwood J G, Altucci C, Velotta R, Springate E, Froud C, Turcu I C E, Patchkovskii S, Ivanov M Yu, Smirnova O and Marangos J P 2010 Phys. Rev. A 81 051802
[21] Zhou X, Lock R, Li W, Wagner N, Murnane M M and Kapteyn H C 2008 Phys. Rev. Lett. 100 073902
[22] Kanai T, Minemoto S and Sakai H 2005 Nature 435 470
[23] Vozzi C, Calegari F, Benedetti E, Caumes J P, Sansone G, Stagira S, Nisoli M, Torres R, Heesel E, Kajumba N, Marangos J P, Altucci C and Velotta R 2005 Phys. Rev. Lett. 95 153902
[24] Kato K, Minemoto S and Sakai H 2011 Phys. Rev. A 84 021403
[25] Liang H J, Fan X, Feng S, Shan L Y, Gao Q H, Yan B, Ma R and Xu H F 2019 Chin. Phys. B 28 094207
[26] Rupenyan A, Kraus P M, Schneider J and Wörner H J 2013 Phys. Rev. A 87 31401
[27] Rupenyan A, Kraus P M, Schneider J and Wörner H J 2013 Phys. Rev. A 87 33409
[28] Ruberti M, Decleva P and Averbukh V 2018 Phys. Chem. Chem. Phys. 20 8311
[29] Jin C, Wang S J, Zhao S F, Le A T and Lin C D 2020 Phys. Rev. A 102 013108
[30] Bruner B D, Mašín Z, Negro M, Morales F, Brambila D, Devetta M, Faccialà D, Harvey A G, Ivanov M, Mairesse Y, Patchkovskii S, Serbinenko V, Soifer H, Stagira S, Vozzi C, Dudovich N and Smirnova O 2016 Faraday Discuss. 194 369
[31] Shu Z, Liang H J, Wang Y C, Hu S L, Chen S, Xu H F, Ma R, Ding D J and Chen J 2022 Phys. Rev. Lett. 128 183202
[32] Camper A, Ferré A, Blanchet V, Descamps D, Lin N, Petit S, Lucchese R, Salières P, Ruchon T and Mairesse Y 2023 Phys. Rev. Lett. 130 083201
[33] Zhu Y, Jiang Z, Ren Z, Bai G, Wang X, Zhang D, Liu J, Zhao J and Zhao Z 2024 Opt. Express 32 37446
[34] Long J, Chen Y H, Zhu X S, He L X, Lan P F and Lu P X 2023 J. Phys. B: At. Mol. Opt. Phys. 56 055601
[35] McFarland B K, Farrell J P, Bucksbaum P H and Gühr M 2008 Science 322 1232
[36] Fu T T, Zhou S S, Chen J G,Wang J, Guo F M and Yang Y J 2023 Opt. Express 31 30171
[37] Sukiasyan S, McDonald C, Destefani C, Ivanov M Yu and Brabec T 2009 Phys. Rev. Lett. 102 223002
[38] Patchkovskii S, Zhao Z X, Brabec T and Villeneuve D M 2006 Phys. Rev. Lett. 97 123003
[39] Diveki Z, Guichard R, Caillat J, Camper A, Haessler S, Auguste T, Ruchon T, Carré B, Maquet A, Taïeb R and Salières P 2013 Chem. Phys. 414 121
[40] Xiao B, Zhao Y W, Cheng F J, Wang G W, Jiang W, Wang Y C, Hu J, Liang H J and Ma R 2024 Chin. Phys. B 33 054209

Experimental manipulation of fine structures in high harmonic spectrum of aligned CO₂ molecules

Experimental manipulation of fine structures in high harmonic spectrum of aligned CO₂ molecules

RichHTML

PDF (PC)

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

本文评价

推荐阅读 0

[1]	Shu-Shan Zhou(周书山), Yu-Long Li(李玉龙), Zhi-Xue Zhao(赵志学), Man Xing(幸满), Nan Xu(许楠), Hao Wang(王浩), Jun Wang(王俊), Xi Zhao(赵曦), and Mu-Hong Hu(胡木宏). High-order harmonic generation of methane in an elliptically polarized field[J]. 中国物理B, 2025, 34(6): 63202-063202.
[2]	Yu Zhao(赵宇), Xiao-Jin Liu(刘晓瑾), Shuang Wang(王爽), Xiao-Xin Huo(霍晓鑫), Yun-He Xing(邢云鹤), and Jun Zhang(张军). Frequency shifts of high-order harmonics from ZnO crystals by chirped laser pulses[J]. 中国物理B, 2025, 34(3): 33201-033201.
[3]	Ling-Yu Zhang(张玲玉), Zhuo-Xuan Xie(谢卓璇), Can Wang(王灿), Xin-Lei Ge(葛鑫磊), and Jing Guo(郭静). Interference of harmonics emitted by different tunneling momentum channels in laser fields[J]. 中国物理B, 2024, 33(9): 93201-093201.
[4]	Jie Hu(胡杰), Yi-Chen Wang(王一琛), Qiu-Shuang Jing(景秋霜), Wei Jiang(姜威), Ge-Wen Wang(王革文), Yi-Wen Zhao(赵逸文), Bo Xiao(肖礴), Hong-Jing Liang(梁红静), and Ri Ma(马日). Elliptically polarized high-order harmonic generation of Ar atom in an intense laser field[J]. 中国物理B, 2024, 33(5): 54208-054208.
[5]	Si-Qi Zhang(张思琪), Bing Zhang(张冰), Bo Yan(闫博), Xiang-Qian Jiang(姜向前), and Xiu-Dong Sun(孙秀冬). Generating attosecond pulses with controllable polarization from cyclic H₃²⁺ molecules by bichromatic circular fields[J]. 中国物理B, 2024, 33(2): 23301-023301.
[6]	Ling-Yu Zhang(张玲玉), Yong-Lin He(何永林), Zhuo-Xuan Xie(谢卓璇), Fang-Yan Gao(高芳艳), Qing-Yun Xu(徐清芸), Xin-Lei Ge(葛鑫磊), Xiang-Yi Luo(罗香怡), and Jing Guo(郭静). High-order harmonic generation of ZnO crystals in chirped and static electric fields[J]. 中国物理B, 2024, 33(1): 13102-13102.
[7]	Chunyang Zhai(翟春洋), Yinmeng Wu(吴银梦), Lingling Qin(秦玲玲), Xiang Li(李翔), Luke Shi(史璐珂), Ke Zhang(张可), Shuaijie Kang(康帅杰), Zhengfa Li(李整法), Yingbin Li(李盈傧), Qingbin Tang(汤清彬), and Benhai Yu(余本海). Elliptically polarized high-order harmonic generation in nitrogen molecules with cross-linearly polarized two-color laser fields[J]. 中国物理B, 2023, 32(7): 73301-073301.
[8]	Chang-Tong Liang(梁畅通), Jing-Jing Zhang(张晶晶), and Peng-Cheng Li(李鹏程). Phase-coherence dynamics of frequency-comb emission via high-order harmonic generation in few-cycle pulse trains[J]. 中国物理B, 2023, 32(3): 33201-033201.
[9]	Dong-Dong Cao(曹冬冬), Xue-Fei Pan(潘雪飞), Jun Zhang(张军), and Xue-Shen Liu(刘学深). Spectral shift of solid high-order harmonics from different channels in a combined laser field[J]. 中国物理B, 2023, 32(3): 34204-034204.
[10]	Beiyu Wang(汪倍羽), Jiaxin Han(韩嘉鑫), and Cheng Jin(金成). Tailoring OAM spectrum of high-order harmonic generation driven by two mixed Laguerre-Gaussian beams with nonzero radial nodes[J]. 中国物理B, 2023, 32(12): 124208-124208.
[11]	Jiaxin Han(韩嘉鑫), Zhong Guan(管仲), Beiyu Wang(汪倍羽), and Cheng Jin(金成). Calibration of quantitative rescattering model for simulating vortex high-order harmonic generation driven by Laguerre-Gaussian beam with nonzero orbital angular momentum[J]. 中国物理B, 2023, 32(12): 124210-124210.
[12]	Jiang-Hua Luo(罗江华) and Jia-Jun Xiao(肖佳俊). Role of excited states in helium-like ions on high-order harmonic generation[J]. 中国物理B, 2023, 32(11): 113201-113201.
[13]	Shu-Shan Zhou(周书山), Yu-Jun Yang(杨玉军), Yang Yang(杨扬), Ming-Yue Suo(索明月), Dong-Yuan Li(李东垣), Yue Qiao(乔月), Hai-Ying Yuan(袁海颖), Wen-Di Lan(蓝文迪), and Mu-Hong Hu(胡木宏). High-order harmonic generation of the cyclo[18]carbon molecule irradiated by circularly polarized laser pulse[J]. 中国物理B, 2023, 32(1): 13201-013201.
[14]	Yanbo Chen(陈炎波), Baochang Li(李保昌), Xuhong Li(李胥红), Xiangyu Tang(唐翔宇), Chi Zhang(张弛), and Cheng Jin(金成). Effect of laser focus in two-color synthesized waveform on generation of soft x-ray high harmonics[J]. 中国物理B, 2023, 32(1): 14203-014203.
[15]	Long Lin(林龙), Tong-Gang Jia(贾铜钢), Zhi-Bin Wang(王志斌), and Peng-Cheng Li(李鹏程). Probing subcycle spectral structures and dynamics of high-order harmonic generation in crystals[J]. 中国物理B, 2022, 31(9): 93202-093202.