-
阿秒瞬态吸收光谱是一种全光学泵浦-探测光谱技术。该技术利用阿秒脉冲(极紫外至软X射线区间)激发或探测应用体系,实时追踪电子跃迁、量子态演化及能量传递等过程,为揭示电子和核相关超快动力学机制提供了前沿研究手段。其核心优势在于:(1)同时具备超快时间(亚飞秒级)和精细光谱(meV级)分辨能力;(2)宽谱阿秒脉冲同时激发多个量子态,实现多能级并行探测;(3)内壳层-价态跃迁的元素与位点特异性,使其能够解析电荷转移、自旋态变化及局域结构演化。目前,阿秒瞬态吸收光谱已在原子分子物理、电子相干动力学及强场物理等研究领域取得重要突破。本文系统阐述了阿秒瞬态吸收光谱的技术原理,重点分析其在气相和凝聚相体系的应用进展,展望其在超快物理化学和量子材料等领域的应用前景。同时,针对阿秒激光发展趋势和探测技术特点,探讨了阿秒瞬态吸收光谱技术未来发展方向。Attosecond transient absorption spectroscopy (ATAS) is an all-optical pump-probe technique that employs attosecond pulses (from the extreme ultraviolet to soft X-ray) to excite or probe a system, enabling real-time tracking of electronic transitions, quantum state evolution, and energy transfer processes. This approach offers key advantages: (1) ultrafast temporal resolution (sub-femtosecond) combined with high spectral resolution (millielectronvolt level); (2) broadband excitation of multiple quantum states, allowing simultaneous detection across multiple energy levels; and (3) element- and site-specific insights afforded by inner-shell to valence transition measurements that reveal charge transfer dynamics, spin state changes, and local structural evolution. To date, significant breakthroughs have been achieved in atomic/molecular physics, electronic coherent dynamics, and strong-field physics using ATAS. This paper systematically reviews the technical principles and theoretical models associated with ATAS employing moderately strong near-infrared pulses, analyzes recent progress in applications to both gas-phase and condensed-phase systems, and explores its future prospects in ultrafast physical chemistry and quantum materials. In gas-phase environments, ATAS has demonstrated significant capabilities in probing energy level shifts and population transfers in atomic systems, as well as capturing nonadiabatic dynamics and charge migration in diatomic and polyatomic molecules. In contrast, within condensed-phase systems, the technique has been effectively used to study the ultrafast dynamics of carriers in semiconductors and to examine the interaction dynamics of localized electrons in insulators and transition metals. Given the rapid evolution of attosecond laser technologies and the distinct advantages of the ATAS detection approach, the paper also outlines potential future directions. These prospects promise to further extend the frontiers of ultrafast spectroscopy and to drive advances across a range of disciplines in both fundamental research and technological applications.
-
[1] Drescher M, Hentschel M, Kienberger R, Uiberacker M, Yakovlev V, Scrinzi A, Westerwalbesloh T, Kleineberg U, Heinzmann U, Krausz F 2002 Nature 419 6909
[2] Li M X, Xie M, Wang H Y, Jia L J, Li J L, Wang W T, Cai J A, Hong X C, Shi X S, Lv Y, Zhao X N, Luo S Z, Jiang W, Peng L, Ding D J 2024 Phys. Rev. Lett. 133 253201
[3] Tao Z S, Chen C, Szilvási T, Keller M, Mavrikakis M, Kapteyn H, Murnane M 2016 Science 353 62
[4] Sansone G, Kelkensberg F, Pérez-Torres J F, Morales F, Kling M F, Siu W, Ghafur O, Johnsson P, Swoboda M, Benedetti E, Ferrari F, Lépine F, Sanz-Vicario J L, Zherebtsov S, Znakovskaya I, L’Huillier A, Ivanov M Y, Nisoli M, Martín F, Vrakking M J J 2010 Nature 465 763
[5] Cattaneo L, Vos J, Bello R Y, Palacios A, Heuser S, Pedrelli L, Lucchini M, Cirelli C, Martín F, Keller U 2018 Nat. Phys. 14 733
[6] Borrego-Varillas R, Lucchini M, Nisoli M 2022 Rep. Prog. Phys. 85 066401
[7] Goulielmakis E, Loh Z, Wirth A, Santra R, Rohringer N, Yakovlev V S, Zherebtsov S, Pfeifer T, Azzeer A M, Kling M F, Leone S R, Krausz F 2010 Nature 466 739
[8] Beck A R, Neumark D M, Leone S R 2015 Chem. Phys. Lett. 624 119
[9] Ramasesha K, Leone S R, Neumark D M 2016 Annu. Rev. Phys. Chem. 67 41
[10] Di Palo N, Inzani G, Dolso G L, Talarico M, Bonetti S, Lucchini M 2024 APL Photonics 9 020901
[11] Kobayashi Y, Leone S R 2022 J. Chem. Phys. 157 180901
[12] 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
[13] Duris J, Li S Q, Driver T, Champenois E G, MacArthur J P, Lutman A A, Zhang Z, Rosenberger P, Aldrich J W, Coffee R, Coslovich G, Decker F, Glownia J M, Hartmann G, Helml W, Kamalov A, Knurr J, Krzywinski J, Lin M, Marangos J P, Nantel M, Natan A, O’Neal J T, Shivaram N, Walter P, Wang A L, Welch J J, Wolf T J A, Xu J Z, Kling M F, Bucksbaum P H, Zholents A, Huang Z, Cryan J P, Marinelli A 2020 Nat. Photonics 14 30
[14] Alqattan H, Hui D D, Pervak V, Hassan M Th 2022 APL Photonics 7 041301
[15] Krausz F, Ivanov M 2009 Rev. Mod. Phys. 81 163
[16] 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
[17] Stooß V, Hartmann M, Birk P, Borisova G D, Ding T, Blättermann A, Ott C, Pfeifer T 2019 Rev. Sci. Instrum. 90 053108
[18] Gaarde M B, Buth C, Tate J L, Schafer K J 2011 Phys. Rev. A 83 013419
[19] Chen S H, Wu M X, Gaarde M B, Schafer K J 2013 Phys. Rev. A 88 033409
[20] Santra R, Dunford R W, Young L 2006 Phys. Rev. A 74 043403
[21] Santra R, Yakovlev V S, Pfeifer T, Loh Z 2011 Phys. Rev. A 83 033405
[22] Wu M X, Chen S H, Camp S, Schafer K J, Gaarde M B 2016 J. Phys. B: At. Mol. Opt. Phys. 49 062003
[23] Hollstein M, Santra R, Pfannkuche D 2017 Phys. Rev. A 95 053411
[24] Timmers H, Zhu X L, Li Z, Kobayashi Y, Sabbar M, Hollstein M, Reduzzi M, Martínez T J, Neumark D M, Leone S R 2019 Nat. Commun. 10 3133
[25] Bækhøj J E, Lévêque C, Madsen L B 2018 Phys. Rev. Lett. 121 023203
[26] Mashiko H, Oguri K, Yamaguchi T, Suda A, Gotoh H 2016 Nat. Phys. 12 741
[27] Zürch M, Chang H, Borja L J, Kraus P M, Cushing S K, Gandman A, Kaplan C J, Oh M H, Prell J S, Prendergast D, Pemmaraju C D, Neumark D M, Leone S R 2017 Nat. Commun. 8 15734
[28] Schultze M, Bothschafter E M, Sommer A, Holzner S, Schweinberger W, Fiess M, Hofstetter M, Kienberger R, Apalkov V, Yakovlev V S, Stockman M I, Krausz F 2013 Nature 493 75
[29] Schultze M, Ramasesha K, Pemmaraju C D, Sato S A, Whitmore D, Gandman A, Prell J S, Borja L J, Prendergast D, Yabana K, Neumark D M, Leone S R 2014 Science 346 1348
[30] Volkov M, Sato S A, Schlaepfer F, Kasmi L, Hartmann N, Lucchini M, Gallmann L, Rubio A, Keller U 2019 Nat. Phys. 15 1145
[31] Jager M F, Ott C, Kraus P M, Kaplan C J, Pouse W, Marvel R E, Haglund R F, Neumark D M, Leone S R 2017 Proc. Natl. Acad. Sci. U. S. A. 114 9558
[32] Bernhardt B, Beck A R, Li X, Warrick E R, Bell M J, Haxton D J, McCurdy C W, Neumark D M, Leone S R 2014 Phys. Rev. A 89 023408
[33] Wang H, Chini M, Chen S Y, Zhang C, He F, Cheng Y, Wu Y, Thumm U, Chang Z H 2010 Phys. Rev. Lett. 105 143002
[34] Wang X W, Chini M, Cheng Y, Wu Y, Tong X, Chang Z H 2013 Phys. Rev. A 87 063413
[35] Cao W, Warrick E R, Neumark D M, Leone S R 2016 New J. Phys. 18 013041
[36] Beck A R, Bernhardt B, Warrick E R, Wu M, Chen S, Gaarde M B, Schafer K J, Neumark D M, Leone S R 2014 New J. Phys. 16 113016
[37] Chini M, Wang X W, Cheng Y, Chang Z H 2014 J. Phys. B: At. Mol. Opt. Phys. 47 124009
[38] Chen S H, Bell M J, Beck A R, Mashiko H, Wu M X, Pfeiffer A N, Gaarde M B, Neumark D M, Leone S R, Schafer K J 2012 Phys. Rev. A 86 063408
[39] Wu M X, Chen S H, Gaarde M B, Schafer K J 2013 Phys. Rev. A 88 043416
[40] Chini M, Wang X W, Cheng Y, Wu Y, Zhao D, Telnov D A, Chu S, Chang Z H 2013 Sci. Rep. 3 1105
[41] Chini M, Zhao B Z, Wang H, Cheng Y, Hu S X, Chang Z H 2012 Phys. Rev. Lett. 109 073601
[42] Ott C, Kaldun A, Raith P, Meyer K, Laux M, Evers J, Keitel C H, Greene C H, Pfeifer T 2013 Science 340 716
[43] Drescher L, Reitsma G, Witting T, Patchkovskii S, Mikosch J, Vrakking M J J 2019 J. Phys. Chem. Lett. 10 265
[44] Chen S H, Wu M X, Gaarde M B, Schafer K J 2013 Phys. Rev. A 87 033408
[45] Kobayashi Y, Chang K F, Zeng T, Neumark D M, Leone S R 2019 Science 365 79
[46] Zinchenko K S, Ardana-Lamas F, Seidu I, Neville S P, van der Veen J, Lanfaloni V U, Schuurman M S, Wörner H J 2021 Science 371 489
[47] Chang K F, Reduzzi M, Wang H, Poullain S M, Kobayashi Y, Barreau L, Prendergast D, Neumark D M, Leone S R 2020 Nat. Commun. 11 4042
[48] Kobayashi Y, Chang K F, Poullain S M, Scutelnic V, Zeng T, Neumark D M, Leone S R 2020 Phys. Rev. A 101 063414
[49] Wei Z R, Li J L, Wang L, See S T, Jhon M H, Zhang Y F, Shi F, Yang M H, Loh Z 2017 Nat. Commun. 8 735
[50] Wei Z R, Li J L, Zhang H M, Lu Y P, Yang M H, Loh Z 2019 J. Chem. Phys. 151 214308
[51] Peng P, Marceau C, Hervé M, Corkum P B, Naumov A Y, Villeneuve D M 2019 Nat. Commun. 10 5269
[52] Peng P, Mi Y H, Lytova M, Britton M, Ding X, Naumov A Yu, Corkum P B, Villeneuve D M 2022 Nat. Photonics 16 45
[53] Holler M, Schapper F, Gallmann L, Keller U 2011 Phys. Rev. Lett. 106 123601
[54] Sabbar M, Timmers H, Chen Y, Pymer A K, Loh Z, Sayres S G, Pabst S, Santra R, Leone S R 2017 Nat. Phys. 13 472
[55] Golubev N V, Vaníček J, Kuleff A I 2021 Phys. Rev. Lett. 127 123001
[56] Kobayashi Y, Neumark D M, Leone S R 2022 Opt. Express 30 5673
[57] Lucchini M, Sato S A, Lucarelli G D, Moio B, Inzani G, Borrego-Varillas R, Frassetto F, Poletto L, Hübener H, De Giovannini U, Rubio A, Nisoli M 2021 Nat. Commun. 12 1021
[58] Géneaux R, Kaplan C J, Yue L, Ross A D, Bækhøj J E, Kraus P M, Chang H, Guggenmos A, Huang M, Zürch M, Schafer K J, Neumark D M, Gaarde M B, Leone S R 2020 Phys. Rev. Lett. 124 207401
[59] Kaplan C J, Kraus P M, Ross A D, Zürch M, Cushing S K, Jager M F, Chang H, Gullikson E M, Neumark D M, Leone S R 2018 Phys. Rev. B 97 205202
[60] Li S, Lu L X, Bhattacharyya S, Pearce C, Li K, Nienhuis E T, Doumy G, Schaller R D, Moeller S, Lin M, Dakovski G, Hoffman D J, Garratt D, Larsen K A, Koralek J D, Hampton C Y, Cesar D, Duris J, Zhang Z, Sudar N, Cryan J P, Marinelli A, Li X S, Inhester L, Santra R, Young L 2024 Science 383 1118
[61] Gutberlet T, Chang H, Zayko S, Sivis M, Ropers C 2023 Opt. Express 31 39757
[62] Volkov M, Pupeikis J, Phillips C R, Schlaepfer F, Gallmann L, Keller U 2019 Opt. Express 27 7886
[63] Géneaux R, Chang H, Schwartzberg A M, Marroux H J B 2021 Opt. Express 29 951
[64] Faccialà D, Toulson B W, Gessner O 2021 Opt. Express 29 35135
[65] Midorikawa K 2022 Nat. Photonics 16 267
[66] Siegrist F, Gessner J A, Ossiander M, Denker C, Chang Y, Schröder M C, Guggenmos A, Cui Y, Walowski J, Martens U, Dewhurst J K, Kleineberg U, Münzenberg M, Sharma S, Schultze M 2019 Nature 571 240
[67] Okino T, Furukawa Y, Nabekawa Y, Miyabe S, Amani Eilanlou A, Takahashi E J, Yamanouchi K, Midorikawa K 2015 Sci. Adv. 1 e1500356
[68] Tzallas P, Skantzakis E, Nikolopoulos L A A, Tsakiris G D, Charalambidis D 2011 Nat. Phys. 7 781
[69] Moulet A, Bertrand J B, Klostermann T, Guggenmos A, Karpowicz N, Goulielmakis E 2017 Science 357 1134
计量
- 文章访问数: 45
- PDF下载量: 2
- 被引次数: 0