中红外飞秒激光场中氮分子高次谐波的多轨道干涉特性研究

李贵花; 谢红强; 姚金平; 储蔚; 程亚; 柳晓军; 陈京; 谢新华

doi:10.7498/aps.65.224208

摘要

通过系统研究氮分子高次谐波产生过程中的电子超快动力学过程，实验上发现在中红外飞秒强激光场驱动下高次谐波谱的截止区附近存在清晰的谐波谱极小值.进一步研究表明谐波谱极小值对应的光子能量强烈依赖于驱动激光脉冲的光强和波长，而与分子取向角无关，由此推断该极小值来源于氮分子最高占据分子轨道和次最高占据分子轨道产生的高次谐波之间的相消干涉.本研究结果将对极端强场条件下多轨道电子超快动力学研究起到积极推动作用.

关键词:

Abstract

Recently, three major types of minima (i.e., Cooper-like minimum, two-center interference minimum and multi-channel interference minimum) have been observed in high-order harmonic generation (HHG) spectra. Identification of the origin of the minimum in a HHG spectrum is critical for self-probing of the molecular structures and dynamics, which has been an important subject in attosecond physics. In this paper, we report the investigation of the multi-electron dynamics in HHG from N2 molecules driven by intense mid-infrared laser pulses. Based on a pump-probe experimental setup, clear spectral minima in the cutoff region of high harmonic spectra from N2 molecules are observed in measurements with mid-infrared laser pulses at three wavelengths (i.e., 1300, 1400 and 1500 nm). A systematic investigation has been carried out for clarifying the origin of these minima. We carefully measured the spectral minima under three different experimental conditions:1) different alignment angles of molecules; 2) various peak laser intensities; 3) tunable driving laser wavelengths. Experimental results show that the positions of the spectral minima do not depend on the alignment angles of molecules. In addition, the measured spectral minima shift almost linearly with the laser intensity for all three wavelengths, and the positions of the spectral minima strongly depend on the wavelengths of the driven field. These findings are in conflict with the Cooper-like and two-center interference minima predictions, providing strong evidences on the dynamic multi-channel interference origin of these minima. Besides, we theoretically calculated the positions of multi-channel interference minima by using a classical three-step model and found out perfect agreements between the experimental results and theoretical calculations, which again strongly support the multi-channel interference picture. Moreover, the advantages of the observed dynamic multi-channel interference based on HHG driven by long wavelength lasers are discussed. The long wavelength driver lasers are attractive for not only generating coherent XUV radiation and attosecond pulses, but also investigating structures and dynamics of molecules in strong laser fields.

Keywords:

作者及机构信息

1.
华东交通大学理学院, 南昌 330013;

2.
东华理工大学理学院, 南昌 330013;

3.
中国科学院上海光学精密机械研究所, 强场激光物理国家重点实验室, 上海 201800;

4.
中国科学院武汉物理与数学研究所, 波谱与原子分子物理国家重点实验室, 武汉 430071;

5.
北京应用物理与计算数学研究所, 北京 100088;

6.
维也纳技术大学光子学研究所, 奥地利维也纳A-1040

通信作者: 程亚, ya.cheng@siom.ac.cn

基金项目: 国家重点基础研究发展计划（973计划）（批准号：2014CB921300，2013CB922201）、国家自然科学基金（批准号：11127901，11134010，61575211，11304330，11404357，61405220，11274050，11334009，61605227）和上海市扬帆计划（批准号：14YF1406100，16YF1412700）资助的课题.

Authors and contacts

1.
School of Science, East China Jiatong University, Nanchang 330013, China;

2.
School of Science, East China University of Technology, Nanchang 330013, China;

3.
State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China;

4.
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, China;

5.
Institute of Applied Physics and Computational Mathematics, Beijing 100088, China;

6.
Photonics Institute, Vienna University of Technology, A-1040 Vienna, Austria, EU

Corresponding author: Cheng Ya, ya.cheng@siom.ac.cn

Funds: Project supported by National Basic Research Program of China (Grant Nos. 2014CB921300, 2013CB922201), the National Natural Science Foundation of China (Grant Nos. 11127901, 11134010, 61575211, 11304330, 11404357, 61405220, 11274050, 11334009, 61605227), and the Shanghai Sailing Program, China (Grant Nos. 14YF1406100, 16YF1412700).

参考文献

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[31]	Xiong H, Xu H, Fu Y, Yao J, Zeng B, Chu W, Cheng Y, Xu Z, Takahashi E J, Midorikawa K, Liu X, Chen J 2009Opt. Lett. 34 1747
[32]	Xu H, Xiong H, Zeng Z, Fu Y, Yao J, Li R, Cheng Y, Xu Z 2008Phys. Rev. A 78 033841
[33]	Ni J, Yao J, Zeng B, Chu W, Li G, Zhang H, Jing C, Chin S L, Cheng Y, Xu Z 2011Phys. Rev. A 84 063846
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[43]	Keldysh L V 1965Sov. Phys. JETP 20 1307

施引文献

[1]	McPherson A, Gibson G, Jara H, Johann U, Luk T S, McIntyre I A, Boyer K, Rhodes C K 1987J. Opt. Soc. Am. B 4 595
[2]	Chen Z Y, Pukhov A 2016Nat. Commun. 7 12515
[3]	Corkum P 1993Phys. Rev. Lett. 71 1994
[4]	Santra R, Gordon A 2006Phys. Rev. Lett. 96 073906
[5]	Gibson E A, Paul A, Wagner N, Tobey R, Gaudiosi D, Backus S, Christov I P, Aquila A, Gullikson E M, Attwood D T, Murnane M M, Kapteyn H C 2003Science 302 95
[6]	Corkum P B, Burnett N H, Ivanov M Y 1994Opt. Lett. 19 1870
[7]	Zeng B, Chu W, Li G, Yao J, Ni J, Zhang H, Cheng Y, Xu Z, Wu Y, Chang Z 2012Phys. Rev. A 85 033839
[8]	Itatani J, Levesque J, Zeidler D, Niikura H, Pepin H, Kieffer J C, Corkum P B, Villeneuve D M 2004Nature 432 867
[9]	Haessler S, Caillat J, Boutu W, Giovanetti-Teixeira C, Ruchon T, Auguste T, Diveki Z, Breger P, Maquet A, Carre B, Taieb R, Salieres P 2010Nat. Phys. 6 200
[10]	Vozzi C, Negro M, Calegari F, Sansone G, Nisoli M, De Silvestri S, Stagira S 2011Nat. Phys. 7 822
[11]	Uiberacker M, Uphues T, Schultze M, Verhoef A J, Yakovlev V, Kling M F, Rauschenberger J, Kabachnik N M, Schroder H, Lezius M, Kompa K L, Muller H G, Vrakking M J, Hendel S, Kleineberg U, Heinzmann U, Drescher M, Krausz F 2007Nature 446 627
[12]	Smirnova O, Mairesse Y, Patchkovskii S, Dudovich N, Villeneuve D, Corkum P, Ivanov M Y 2009Nature 460 972
[13]	Dudovich N, Smirnova O, Levesque J, Mairesse Y, Ivanov M Y, Villeneuve D M, Corkum P B 2006Nat. Phys. 2 781
[14]	Xu H, Xiong H, Zeng B, Chu W, Fu Y, Yao J, Chen J, Liu X, Cheng Y, Xu Z 2010Opt. Lett. 35 472
[15]	Li W, Zhou X, Lock R, Patchkovskii S, Stolow A, Kapteyn H C, Murnane M M 2008Science 322 1207
[16]	McFarland B K, Farrell J P, Bucksbaum P H, Ghr M 2008Science 322 1232
[17]	Yao J, Li G, Jia X, Hao X, Zeng B, Jing C, Chu W, Ni J, Zhang H, Xie H, Zhang C, Zhao Z, Chen J, Liu X, Cheng Y, Xu Z 2013Phys. Rev. Lett. 111 133001
[18]	Wörner H J, Bertrand J B, Hockett P, Corkum P B, Villeneuve D M 2010Phys. Rev. Lett. 104 233904
[19]	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 Y, Smirnova O, Marangos J P 2010Phys. Rev. A 81 051802
[20]	Bertrand J B, Wörner H J, Hockett P, Villeneuve D M, Corkum P B 2012Phys. Rev. Lett. 109 143001
[21]	Higuet J, Ruf H, Thiré N, Cireasa R, Constant E, Cormier E, Descamps D, Mével E, Petit S, Pons B, Mairesse Y, Fabre B 2011Phys. Rev. A 83 053401
[22]	Wahlström C G, Larsson J, Persson A, Starczewski T, Svanberg S, Salières P, Balcou P, L'Huillier A 1993Phys. Rev. A 48 4709
[23]	Lein M, Hay N, Velotta R, Marangos J, Knight P 2002Phys. Rev. Lett. 88 183903
[24]	Lein M, Hay N, Velotta R, Marangos J, Knight P 2002Phys. Rev. A 66 023805
[25]	Le A T, Tong X M, Lin C 2006Phys. Rev. A 73 041402
[26]	Kanai T, Minemoto S, Sakai H 2005Nature 435 470
[27]	Kato K, Minemoto S, Sakai H 2011Phys. Rev. A 84 021403
[28]	Vozzi C, Calegari F, Benedetti E, Caumes J P, Sansone G, Stagira S, Nisoli M, Torres R, Heesel E, Kajumba N, Marangos J, Altucci C, Velotta R 2005Phys. Rev. Lett. 95 153902
[29]	Diveki Z, Camper A, Haessler S, Auguste T, Ruchon T, Carré B, Salières P, Guichard R, Caillat J, Maquet A, Taïeb R 2012New J. Phys. 14 023062
[30]	Krause J, Schafer K, Kulander K 1992Phys. Rev. Lett. 68 3535
[31]	Xiong H, Xu H, Fu Y, Yao J, Zeng B, Chu W, Cheng Y, Xu Z, Takahashi E J, Midorikawa K, Liu X, Chen J 2009Opt. Lett. 34 1747
[32]	Xu H, Xiong H, Zeng Z, Fu Y, Yao J, Li R, Cheng Y, Xu Z 2008Phys. Rev. A 78 033841
[33]	Ni J, Yao J, Zeng B, Chu W, Li G, Zhang H, Jing C, Chin S L, Cheng Y, Xu Z 2011Phys. Rev. A 84 063846
[34]	Antoine P, L'Huillier A, Lewenstein M 1996Phys. Rev. Lett. 77 1234
[35]	Popmintchev T, Chen M C, Bahabad A, Gerrity M, Sidorenko P, Cohen O, Christov I P, Murnane M M, Kapteyn H C 2009PNAS 106 10516
[36]	Popmintchev T, Chen M C, Cohen O, Grisham M E, Rocca J J, Murnane M M, Kapteyn H C 2008Opt. Lett. 33 2128
[37]	Cirmi G, Lai C J, Granados E, Huang S W, Sell A, Hong K H, Moses J, Keathley P, Kärtner F X 2012J. Phys. B:At. Mol. Opt. Phys. 45 205601
[38]	Chen M C, Arpin P, Popmintchev T, Gerrity M, Zhang B, Seaberg M, Popmintchev D, Murnane M M, Kapteyn H C 2010Phys. Rev. Lett. 105 173901
[39]	Seideman T 1995J. Chem. Phys. 103 7887
[40]	Ortigoso J, Rodríguez M, Gupta M, Friedrich B 1999J. Chem. Phys. 110 3870
[41]	Kanai T, Takahashi E, Nabekawa Y, Midorikawa K 2007Phys. Rev. Lett. 98 153904
[42]	Lewenstein M, Salières P, L'Huillier A 1995Phys. Rev. A 52 4747
[43]	Keldysh L V 1965Sov. Phys. JETP 20 1307

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