Attosecond chronoscopy is central to the understanding of ultrafast electron dynamics in matter from gas to the condensed phase with attosecond temporal resolution. It has, however, not yet been possible to determine the timing of individual partial waves, and steering their contribution has been a substantial challenge. Here, we develop a polarization-skewed attosecond chronoscopy serving as a partial wave meter to reveal the role of each partial wave from the angle-resolved photoionization phase shifts in rare gas atoms. We steer the relative ratio between different partial waves and realize a magnetic-sublevel-resolved atomic phase shift measurement. Our experimental observations are well supported by time-dependent R-matrix numerical simulations and analytical soft-photon approximation analysis. The symmetry-resolved, partial-wave analysis identifies the transition rate and phase shift property in the attosecond photoelectron emission dynamics. Our findings provide critical insights into the ubiquitous attosecond optical timer and the underlying attosecond photoionization dynamics.

CAS Center for Excellence in Ultra intense Laser Science Shanghai China

Centre for Theoretical Atomic Molecular and Optical Physics School of Mathematics and Physics Queen's University Belfast University Road Belfast BT7 1NN Northern Ireland UK

Collaborative Innovation Center of Extreme Optics Shanxi University Taiyuan Shanxi China

Institute of Theoretical Physics Faculty of Mathematics and Physics Charles University 5 Holešovičkách 2 180 00 Prague 8 Czech Republic

Raymond and Beverly Sackler Faculty of Exact Science School of Chemistry and Center for Light Matter Interaction Tel Aviv University 6997801 Tel Aviv Israel

School of Physics and CRANN Institute Trinity College Dublin Dublin 2 Ireland

State Key Laboratory of Precision Spectroscopy East China Normal University Shanghai China

Zobrazit více v PubMed

Nisoli M, Decleva P, Calegari F, Palacios A, Martín F. Attosecond electron dynamics in molecules. Chem. Rev. 2017;117:10760–10825. doi: 10.1021/acs.chemrev.6b00453. PubMed DOI

Paul PM, et al. Observation of a train of attosecond pulses from high harmonic generation. Science. 2001;292:1689–1692. doi: 10.1126/science.1059413. PubMed DOI

Mairesse Y, et al. Attosecond synchronization of high-harmonic soft X-rays. Science. 2003;302:1540–1543. doi: 10.1126/science.1090277. PubMed DOI

Goulielmakis E, et al. Direct measurement of light waves. Science. 2004;305:1267–1269. doi: 10.1126/science.1100866. PubMed DOI

Itatani J, et al. Attosecond streak camera. Phys. Rev. Lett. 2002;88:173903. doi: 10.1103/PhysRevLett.88.173903. PubMed DOI

Guénot D, et al. Measurements of relative photoemission time delays in noble gas atoms. J. Phys. B. 2014;47:245602. doi: 10.1088/0953-4075/47/24/245602. DOI

Palatchi C, et al. Atomic delay in helium, neon, argon and krypton. J. Phys. B. 2014;47:245003. doi: 10.1088/0953-4075/47/24/245003. DOI

Alexandridi C, et al. Attosecond photoionization dynamics in the vicinity of the Cooper minima in argon. Phys. Rev. Res. 2021;3:L012012. doi: 10.1103/PhysRevResearch.3.L012012. DOI

Huppert M, Jordan I, Baykusheva D, von Conta A, Wörner HJ. Attosecond delays in molecular photoionization. Phys. Rev. Lett. 2016;117:093001. doi: 10.1103/PhysRevLett.117.093001. PubMed DOI

Nandi S, et al. Attosecond timing of electron emission from a molecular shape resonance. Sci. Adv. 2020;6:eaba7762. doi: 10.1126/sciadv.aba7762. PubMed DOI PMC

Beaulieu S, et al. Attosecond-resolved photoionization of chiral molecules. Science. 2017;358:1288–1294. doi: 10.1126/science.aao5624. PubMed DOI

Cavalieri AL, et al. Attosecond spectroscopy in condensed matter. Nature. 2007;449:1029–1032. doi: 10.1038/nature06229. PubMed DOI

Lucchini M, et al. Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond. Science. 2016;353:916–919. doi: 10.1126/science.aag1268. PubMed DOI

Tao Z, et al. Direct time-domain observation of attosecond final-state lifetimes in photoemission from solids. Science. 2016;353:62–67. doi: 10.1126/science.aaf6793. PubMed DOI PMC

Jordan I, et al. Attosecond spectroscopy of liquid water. Science. 2020;369:974–979. doi: 10.1126/science.abb0979. PubMed DOI

Klünder K, et al. Probing single-photon ionization on the attosecond time scale. Phys. Rev. Lett. 2011;106:143002. doi: 10.1103/PhysRevLett.106.143002. PubMed DOI

Gong X, et al. Energy-resolved ultrashort delays of photoelectron emission clocked by orthogonal two-color laser fields. Phys. Rev. Lett. 2017;118:143203. doi: 10.1103/PhysRevLett.118.143203. PubMed DOI

Isinger M, et al. Photoionization in the time and frequency domain. Science. 2017;358:893–896. doi: 10.1126/science.aao7043. PubMed DOI

Heck S, et al. Attosecond interferometry of shape resonances in the recoil frame of CF4. Sci. Adv. 2021;7:eabj8121. doi: 10.1126/sciadv.abj8121. PubMed DOI PMC

Gong X, et al. Asymmetric attosecond photoionization in molecular shape resonance. Phys. Rev. X. 2022;12:011002.

Ossiander M, et al. Attosecond correlation dynamics. Nat. Phys. 2017;13:280–285. doi: 10.1038/nphys3941. DOI

Vos J, et al. Orientation-dependent stereo Wigner time delay and electron localization in a small molecule. Science. 2018;360:1326–1330. doi: 10.1126/science.aao4731. PubMed DOI

Gong, X. et al. Attosecond spectroscopy of size-resolved water clusters. PubMed

Dahlström JM, L’Huillier A, Maquet A. Introduction to attosecond delays in photoionization. J. Phys. B. 2012;45:183001. doi: 10.1088/0953-4075/45/18/183001. DOI

Pazourek R, Nagele S, Burgdörfer J. Attosecond chronoscopy of photoemission. Rev. Mod. Phys. 2015;87:765–802. doi: 10.1103/RevModPhys.87.765. DOI

Wigner EP. Lower limit for the energy derivative of the scattering phase shift. Phys. Rev. 1955;98:145–147. doi: 10.1103/PhysRev.98.145. DOI

Smith FT. Lifetime matrix in collision theory. Phys. Rev. 1960;118:349–356. doi: 10.1103/PhysRev.118.349. DOI

Heuser S, et al. Angular dependence of photoemission time delay in helium. Phys. Rev. A. 2016;94:063409. doi: 10.1103/PhysRevA.94.063409. DOI

Ivanov IA, Kheifets AS. Angle-dependent time delay in two-color XUV+IR photoemission of He and Ne. Phys. Rev. A. 2017;96:013408. doi: 10.1103/PhysRevA.96.013408. DOI

Fuchs J, et al. Time delays from one-photon transitions in the continuum. Optica. 2020;7:154–161. doi: 10.1364/OPTICA.378639. DOI

Sörngard J, Dahlström JM, Lindroth E. Study of the possibilities with combinations of circularly and linearly polarized light for attosecond delay investigations. J. Phys. B. 2020;53:134003–134011. doi: 10.1088/1361-6455/ab84c6. DOI

Reid KL, Leahy DJ, Zare RN. Effect of breaking cylindrical symmetry on photoelectron angular distributions resulting from resonance-enhanced two-photon ionization. J. Chem. Phys. 1991;95:1746–1756. doi: 10.1063/1.461023. DOI

Reid KL. Photoelectron angular distributions. Annu. Rev. Phys. Chem. 2003;54:397–424. doi: 10.1146/annurev.physchem.54.011002.103814. PubMed DOI

You D, et al. New method for measuring angle-resolved phases in photoemission. Phys. Rev. X. 2020;10:031070.

Holzmeier F, et al. Influence of shape resonances on the angular dependence of molecular photoionization delays. Nat. Commun. 2021;12:7343. doi: 10.1038/s41467-021-27360-y. PubMed DOI PMC

Busto D, et al. Fano’s propensity rule in angle-resolved attosecond pump-probe photoionization. Phys. Rev. Lett. 2019;123:133201. doi: 10.1103/PhysRevLett.123.133201. PubMed DOI

Leahy DJ, Reid KL, Zare RN. Complete description of two-photon (1 +1’) ionization of NO deduced from rotationally resolved photoelectron angular distributions. J. Chem. Phys. 1991;95:1757–1767. doi: 10.1063/1.461024. DOI

O’Keeffe P, et al. Polarization effects in two-photon nonresonant ionization of argon with extreme-ultraviolet and infrared femtosecond pulses. Phys. Rev. A. 2004;69:051401(R). doi: 10.1103/PhysRevA.69.051401. DOI

Meyer M, et al. Polarization control in two-color above-threshold ionization of atomic helium. Phys. Rev. Lett. 2008;101:193002. doi: 10.1103/PhysRevLett.101.193002. PubMed DOI

Dörner R, et al. Cold target recoil ion momentum spectroscopy: a ’momentum microscope’ to view atomic collision dynamics. Phys. Rep. 2000;330:95–192. doi: 10.1016/S0370-1573(99)00109-X. DOI

Ullrich J, et al. Recoil-ion and electron momentum spectroscopy: Reaction-microscopes. Rep. Prog. Phys. 2003;66:1463–1545. doi: 10.1088/0034-4885/66/9/203. DOI

Corkum PB. Plasma perspective on strong field multiphoton ionization. Phys. Rev. Lett. 1993;71:1994–1997. doi: 10.1103/PhysRevLett.71.1994. PubMed DOI

Popmintchev T, Chen MC, Arpin P, Murnane MM, Kapteyn HC. The attosecond nonlinear optics of bright coherent X-ray generation. Nat. Photon. 2010;4:822–832. doi: 10.1038/nphoton.2010.256. DOI

Brown AC, et al. RMT: R-matrix with time-dependence. solving the semi-relativistic, time-dependent schrödinger equation for general, multielectron atoms and molecules in intense, ultrashort, arbitrarily polarized laser pulses. Computer Phys. Commun. 2020;250:107062. doi: 10.1016/j.cpc.2019.107062. DOI

Maquet A, Taïeb R. Two-colour IR+XUV spectroscopies: The "soft-photon approximation". J. Mod. Opt. 2007;54:1847–1857. doi: 10.1080/09500340701306751. DOI

Deshmukh PC, Banerjee S, Mandal A, Manson ST. Eisenbud-Wigner-Smith time delay in atom-laser interactions. Eur. Phys. J. Spec. Top. 2021;230:4151–4164. doi: 10.1140/epjs/s11734-021-00225-7. DOI

Kennedy DJ, Manson ST. Photoionization of the noble gases: Cross sections and angular distributions. Phys. Rev. A. 1972;5:227–247. doi: 10.1103/PhysRevA.5.227. DOI

Shiner AD, et al. Probing collective multi-electron dynamics in xenon with high-harmonic spectroscopy. Nat. Phys. 2011;7:464–467. doi: 10.1038/nphys1940. DOI

Böwering N, et al. Asymmetry in photoelectron emission from chiral molecules induced by circularly polarized light. Phys. Rev. Lett. 2001;86:1187–1190. doi: 10.1103/PhysRevLett.86.1187. PubMed DOI

Garcia GA, et al. Circular dichroism in the photoelectron angular distribution from randomly oriented enantiomers of camphor. J. Chem. Phys. 2003;119:8781–8784. doi: 10.1063/1.1621379. DOI

Beaulieu S, et al. Photoexcitation circular dichroism in chiral molecules. Nat. Phys. 2018;14:484–489. doi: 10.1038/s41567-017-0038-z. DOI

Chini M, et al. Delay control in attosecond pump-probe experiments. Opt. Express. 2009;17:21459–21464. doi: 10.1364/OE.17.021459. PubMed DOI

Jagutzki O, et al. Position sensitive anodes for MCP read-out using induced charge measurement. Nucl. Instrum. Methods Phys. Res. 2002;477:256–261. doi: 10.1016/S0168-9002(01)01843-5. DOI

Jagutzki O, et al. Multiple hit readout of a microchannel plate detector with a three-layer delay-line anode. IEEE Trans. Nucl. Sci. 2002;49:2477–2483. doi: 10.1109/TNS.2002.803889. DOI

Madsen LB. Strong-field approximation in laser-assisted dynamics. Am. J. Phys. 2005;73:57–62. doi: 10.1119/1.1796791. DOI

Moore LR, et al. The RMT method for many-electron atomic systems in intense short-pulse laser light. J. Mod. Opt. 2011;58:1132–1140. doi: 10.1080/09500340.2011.559315. DOI

Clarke DDA, Armstrong GSJ, Brown AC, van der Hart HW. R-matrix-with-time-dependence theory for ultrafast atomic processes in arbitrary light fields. Phys. Rev. A. 2018;98:053442. doi: 10.1103/PhysRevA.98.053442. DOI

Burke PG, Taylor KT. R-matrix theory of photoionization. Application to neon and argon. J. Phys. B. 1975;8:2620. doi: 10.1088/0022-3700/8/16/020. DOI

Brown AC, Robinson DJ, van der Hart HW. Atomic harmonic generation in time-dependent R-matrix theory. Phys. Rev. A. 2012;86:053420. doi: 10.1103/PhysRevA.86.053420. DOI

The RMT repository. https://gitlab.com/Uk-amor/RMT/rmt (2019).

Anisotropy Parameters for Two-Color Photoionization Phases in Randomly Oriented Molecules: Theory and Experiment in Methane and Deuteromethane