Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Puskar, Nicolette G.; Lin, Yen-Cheng; Gaynor, James D.; Schuchter, Maximilian C.; Chattopadhyay, Siddhartha; Marante, Carlos; Fidler, Ashley P.; Keenan, Clare L.; Argenti, Luca; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1103/physreva.107.033117

Title: Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Journal Article · 26 March 2023 · Physical Review A

DOI: https://doi.org/10.1103/physreva.107.033117 · OSTI ID:2228885

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Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland). Laboratory for Physical Chemistry
Univ. of Central Florida, Orlando, FL (United States)
Princeton Univ., NJ (United States)
Univ. of Chicago, IL (United States)

Attosecond noncollinear four-wave-mixing spectroscopy with one attosecond extreme ultraviolet (XUV) pulse and two few-cycle near-infrared (NIR) pulses was used to measure the autoionization decay lifetimes of inner valence electronic excitations in neon atoms. After a 43-48-eV XUV photon excites a 2s electron into the 2s2p⁶(np) Rydberg series, broadband NIR pulses couple the 2s2p⁶3p XUV-bright state to neighboring 2s2p⁶3s and 2s2p⁶3d XUV-dark states. Controllable delays of one or both NIR pulses with respect to the attosecond XUV pulse reveal the temporal evolution of either the dark or bright states, respectively. Experimental lifetimes for the 3s, 3p, and 3d states are measured to be 7±2, 48±8, and 427±40 fs, respectively, with 95% confidence. Accompanying calculations with two independent ab initio theoretical methods, newstock and astra, verify the findings. The results support the expected trend that the autoionization lifetime should be longer for states that have a smaller penetration in the radial region of the 2s core hole, which in this case is for the higher angular momentum Rydberg orbitals. In conclusion, the underlying theory thus links the lifetime results to electron correlation and provides an assessment of the direct and exchange terms in the autoionization process.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; SC0020311

OSTI ID:: 2228885

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 3 Vol. 107; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (48)

Multiple pulse coherent dynamics and wave packet control of the N ₂ a′′ ¹ Σ+g dark state by attosecond four-wave mixing Warrick, Erika R.; Fidler, Ashley P.; Cao, Wei Faraday Discussions, Vol. 212 https://doi.org/10.1039/C8FD00074C	journal	January 2018
On the Derivation of the Dispersion Formula for Nuclear Reactions Siegert, A. J. F. Physical Review, Vol. 56, Issue 8 https://doi.org/10.1103/PhysRev.56.750	journal	October 1939
Time-resolved four-wave-mixing spectroscopy for inner-valence transitions Ding, Thomas; Ott, Christian; Kaldun, Andreas Optics Letters, Vol. 41, Issue 4 https://doi.org/10.1364/OL.41.000709	journal	January 2016
On possibility of calculating Siegert eigenvalues for autoionizing electronic states Isaacson, A. D.; McCurdy, C. W.; Miller, W. H. Chemical Physics, Vol. 34, Issue 3 https://doi.org/10.1016/0301-0104(78)85174-X	journal	November 1978
Solving the three-body Coulomb breakup problem using exterior complex scaling McCurdy, C. W.; Baertschy, M.; Rescigno, T. N. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 37, Issue 17 https://doi.org/10.1088/0953-4075/37/17/R01	journal	August 2004
Accurate Ground-Term Combinations in Ne i Kaufman, Victor; Minnhagen, Lennart Journal of the Optical Society of America, Vol. 62, Issue 1 https://doi.org/10.1364/JOSA.62.000092	journal	January 1972
The definition of molecular resonance curves by the method of exterior complex scaling Simon, Barry Physics Letters A, Vol. 71, Issue 2-3 https://doi.org/10.1016/0375-9601(79)90165-8	journal	April 1979
Coupled nuclear–electronic decay dynamics of O₂ inner valence excited states revealed by attosecond XUV wave-mixing spectroscopy Lin, Yen-Cheng; Fidler, Ashley P.; Sandhu, Arvinder Faraday Discussions, Vol. 228 https://doi.org/10.1039/D0FD00113A	journal	January 2021
Multiconfigurational Hartree-Fock close-coupling ansatz: Application to the argon photoionization cross section and delays Carette, T.; Dahlström, J. M.; Argenti, L. Physical Review A, Vol. 87, Issue 2 https://doi.org/10.1103/PhysRevA.87.023420	journal	February 2013
Molecular Electronic-Structure Theory Helgaker, Trygve; Jørgensen, Poul; Olsen, Jeppe https://doi.org/10.1002/9781119019572	book	August 2000
Attosecond Time-Resolved Autoionization of Argon Wang, He; Chini, Michael; Chen, Shouyuan Physical Review Letters, Vol. 105, Issue 14 https://doi.org/10.1103/PhysRevLett.105.143002	journal	October 2010
Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy Gaynor, James D.; Fidler, Ashley P.; Kobayashi, Yuki Physical Review A, Vol. 107, Issue 2 https://doi.org/10.1103/PhysRevA.107.023526	journal	February 2023
Effects of Configuration Interaction on Intensities and Phase Shifts Fano, U. Physical Review, Vol. 124, Issue 6 https://doi.org/10.1103/PhysRev.124.1866	journal	December 1961
Rydberg Atoms Gallagher, Thomas F. Cambridge University Press https://doi.org/10.1017/CBO9780511524530	book	January 2009
Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table : Molcas 8 Aquilante, Francesco; Autschbach, Jochen; Carlson, Rebecca K. Journal of Computational Chemistry, Vol. 37, Issue 5 https://doi.org/10.1002/jcc.24221	journal	November 2015
The initial implementation and applications of a general active space coupled cluster method Olsen, Jeppe The Journal of Chemical Physics, Vol. 113, Issue 17 https://doi.org/10.1063/1.1290005	journal	November 2000
Time-resolved atomic inner-shell spectroscopy Drescher, M.; Hentschel, M.; Kienberger, R. Nature, Vol. 419, Issue 6909 https://doi.org/10.1038/nature01143	journal	October 2002
Ultra-Ionization Potentials in Mercury Vapor Shenstone, A. G. Physical Review, Vol. 38, Issue 5 https://doi.org/10.1103/PhysRev.38.873	journal	September 1931
High-resolution experimental and theoretical study of singly and doubly excited resonances in ground-state photoionization of neon Schulz, Konrad; Domke, Michael; Püttner, Ralph Physical Review A, Vol. 54, Issue 4 https://doi.org/10.1103/PhysRevA.54.3095	journal	October 1996
UKRmol+: A suite for modelling electronic processes in molecules interacting with electrons, positrons and photons using the R-matrix method Mašín, Zdeněk Mendeley https://doi.org/10.17632/k3ny7zcfrb	dataset	January 2020
R-matrix theory of photoionization. Application to neon and argon Burke, P. G.; Taylor, K. T. Journal of Physics B: Atomic and Molecular Physics, Vol. 8, Issue 16 https://doi.org/10.1088/0022-3700/8/16/020	journal	November 1975
Recent Advances in Wave Function-Based Methods of Molecular-Property Calculations Helgaker, Trygve; Coriani, Sonia; Jørgensen, Poul Chemical Reviews, Vol. 112, Issue 1 https://doi.org/10.1021/cr2002239	journal	December 2011
Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations Cao, Wei; Warrick, Erika R.; Fidler, Ashley Physical Review A, Vol. 94, Issue 5 https://doi.org/10.1103/PhysRevA.94.053846	journal	November 2016
Doubly Excited Autoionizing Rydberg States of Sr Cooke, W. E.; Gallagher, T. F.; Edelstein, S. A. Physical Review Letters, Vol. 40, Issue 3 https://doi.org/10.1103/PhysRevLett.40.178	journal	January 1978
Density functional-time-dependent local density approximation calculations of autoionization resonances in noble gases Stener, M.; Decleva, P.; Lisini, A. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 28, Issue 23 https://doi.org/10.1088/0953-4075/28/23/009	journal	December 1995
Optically Forbidden Excitations of 2s Electron of Neon Studied by Fast Electron Impact Min, Ge; Lin-Fan, Zhu; Cun-Ding, Liu Chinese Physics Letters, Vol. 25, Issue 10 https://doi.org/10.1088/0256-307X/25/10/034	journal	October 2008
The Dalton quantum chemistry program system: The Dalton program Aidas, Kestutis; Angeli, Celestino; Bak, Keld L. Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 4, Issue 3 https://doi.org/10.1002/wcms.1172	journal	September 2013
Atomic Screening Constants from SCF Functions Clementi, E.; Raimondi, D. L. The Journal of Chemical Physics, Vol. 38, Issue 11 https://doi.org/10.1063/1.1733573	journal	June 1963
UKRmol+: A suite for modelling electronic processes in molecules interacting with electrons, positrons and photons using the R-matrix method Mašín, Zdeněk; Benda, Jakub; Gorfinkiel, Jimena D. Computer Physics Communications, Vol. 249 https://doi.org/10.1016/j.cpc.2019.107092	journal	April 2020
Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses Fidler, Ashley P.; Warrick, Erika R.; Marroux, Hugo J. B. Journal of Physics: Photonics, Vol. 2, Issue 3 https://doi.org/10.1088/2515-7647/ab869c	journal	May 2020
Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy Gaynor, James D.; Fidler, Ashley P.; Lin, Yen-Cheng Physical Review B, Vol. 103, Issue 24 https://doi.org/10.1103/PhysRevB.103.245140	journal	June 2021
Hybrid Gaussian– B -spline basis for the electronic continuum: Photoionization of atomic hydrogen Marante, Carlos; Argenti, Luca; Martín, Fernando Physical Review A, Vol. 90, Issue 1 https://doi.org/10.1103/PhysRevA.90.012506	journal	July 2014
Non-orthogonal internally contracted multi-configurational perturbation theory (NICPT): Dynamic electron correlation for large, compact active spaces Kähler, Sven; Olsen, Jeppe The Journal of Chemical Physics, Vol. 147, Issue 17 https://doi.org/10.1063/1.4999218	journal	November 2017
Resonance phenomena in molecular photoionization: impact of synchrotron radiation Madden, R. P.; Parr, A. G. Applied Optics, Vol. 21, Issue 2 https://doi.org/10.1364/AO.21.000179	journal	January 1982
State-selective probing of CO2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy Fidler, Ashley P.; Lin, Yen-Cheng; Gaynor, James D. Physical Review A, Vol. 106, Issue 6 https://doi.org/10.1103/PhysRevA.106.063525	journal	December 2022
Photodetachment of H − and Li − Lindroth, E. Physical Review A, Vol. 52, Issue 4 https://doi.org/10.1103/PhysRevA.52.2737	journal	October 1995
Autoionization dynamics of ( ² P _1/2 ) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses Fidler, Ashley P.; Marroux, Hugo J. B.; Warrick, Erika R. The Journal of Chemical Physics, Vol. 151, Issue 11 https://doi.org/10.1063/1.5113912	journal	September 2019
A multi-center quadrature scheme for the molecular continuum Gharibnejad, H.; Douguet, N.; Schneider, B. I. Computer Physics Communications, Vol. 263 https://doi.org/10.1016/j.cpc.2021.107889	journal	June 2021
Screening Percentages Based on Slater Effective Nuclear Charge as a Versatile Tool for Teaching Periodic Trends Waldron, Kimberley A.; Fehringer, Erin M.; Streeb, Amy E. Journal of Chemical Education, Vol. 78, Issue 5 https://doi.org/10.1021/ed078p635	journal	May 2001
Calculation of autoionization rates for high-angular-momentum Rydberg states Cooke, W. E.; Gallagher, T. F. Physical Review A, Vol. 19, Issue 6 https://doi.org/10.1103/PhysRevA.19.2151	journal	June 1979
Lorentz Meets Fano in Spectral Line Shapes: A Universal Phase and Its Laser Control Ott, C.; Kaldun, A.; Raith, P. Science, Vol. 340, Issue 6133 https://doi.org/10.1126/science.1234407	journal	May 2013
High-spectral-resolution attosecond absorption spectroscopy of autoionization in xenon Bernhardt, Birgitta; Beck, Annelise R.; Li, Xuan Physical Review A, Vol. 89, Issue 2 https://doi.org/10.1103/PhysRevA.89.023408	journal	February 2014
Multipolariton control in attosecond transient absorption of autoionizing states Yanez-Pagans, S.; Cariker, C.; Shaikh, M. Physical Review A, Vol. 105, Issue 6 https://doi.org/10.1103/PhysRevA.105.063107	journal	June 2022
Resonances in the Photo-Ionization Continuum of Ne I (20-150 eV) Codling, K.; Madden, R. P.; Ederer, D. L. Physical Review, Vol. 155, Issue 1 https://doi.org/10.1103/PhysRev.155.26	journal	March 1967
An MCHF atomic-structure package for large-scale calculations Froese Fischer, Charlotte; Tachiev, Georgio; Gaigalas, Gediminas Computer Physics Communications, Vol. 176, Issue 8 https://doi.org/10.1016/j.cpc.2007.01.006	journal	April 2007
Determinant based configuration interaction algorithms for complete and restricted configuration interaction spaces Olsen, Jeppe; Roos, Björn O.; Jo/rgensen, Poul The Journal of Chemical Physics, Vol. 89, Issue 4 https://doi.org/10.1063/1.455063	journal	August 1988
Implementation of exterior complex scaling in B-splines to solve atomic and molecular collision problems McCurdy, C. William; Martín, Fernando Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 37, Issue 4 https://doi.org/10.1088/0953-4075/37/4/017	journal	February 2004
Why complex absorbing potentials work: A discrete-variable-representation perspective Santra, Robin Physical Review A, Vol. 74, Issue 3 https://doi.org/10.1103/PhysRevA.74.034701	journal	September 2006

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