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Effects of Autoionizing Resonances on Wave-Packet Dynamics Studied by Time-Resolved Photoelectron Spectroscopy

Journal Article · · Physical Review Letters
 [1];  [2];  [3];  [4];  [5];  [6];  [7]
  1. Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); OSTI
  2. Missouri Univ. of Science and Technology, Rolla, MO (United States); Kansas State Univ., Manhattan, KS (United States)
  3. Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Jilin Univ., Changchun (China)
  4. Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Univ. of Hong Kong, Pokfulam (Hong Kong)
  5. Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Univ. of Colorado, Boulder, CO (United States); National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
  6. Missouri Univ. of Science and Technology, Rolla, MO (United States); Univ. of Connecticut, Storrs, CT (United States)
  7. Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
+ Show Author Affiliations

Here, we report a combined experimental and theoretical study on the effect of autoionizing resonances in time-resolved photoelectron spectroscopy. The coherent excitation of N2 by ~14.15 eV extreme-ultraviolet photons prepares a superposition of three dominant adjacent vibrational levels (v'=14–16) in the valence b' 1$$Σ^+_u$$ state, which are probed by the absorption of two or three near-infrared photons (800 nm). The superposition manifests itself as coherent oscillations in the measured photoelectron spectra. A quantum-mechanical simulation confirms that two autoionizing Rydberg states converging to the excited A 2Πu and B 2$$Σ^+_u$$ $$N^+_2$$ cores are accessed by the resonant absorption of near-infrared photons. We show that these resonances apply different filters to the observation of the vibrational wave packet, which results in different phases and amplitudes of the oscillating photoelectron signal depending on the nature of the autoionizing resonance. This work clarifies the importance of resonances in time-resolved photoelectron spectroscopy and particularly reveals the phase of vibrational quantum beats as a powerful observable for characterizing the properties of such resonances.

Research Organization:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0023192
OSTI ID:
2422210
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 15 Vol. 130; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (47)

A theoretical study of the rydberg states of N2 obtained from excitations of the valence 3σg, 1πu and 2σu levels journal November 1986
Attosecond transient absorption spectroscopy of molecular nitrogen: Vibrational coherences in the b′ 1Σ+u state journal September 2017
Quantum wave packet revivals journal March 2004
Probing the Dynamics of Rydberg and Valence States of Molecular Nitrogen with Attosecond Transient Absorption Spectroscopy journal February 2016
Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond † journal June 2000
Femtosecond Photoelectron Imaging on Pyrazine:  (1+2‘) REMPI of Deuterated Pyrazine journal June 2004
Femtosecond Study of Multiphoton Ionization Processes in K 2 :  From Pump−Probe to Control # journal January 1996
Sub-10-fs control of dissociation pathways in the hydrogen molecular ion with a few-pulse attosecond pulse train journal September 2016
Conical-intersection dynamics and ground-state chemistry probed by extreme-ultraviolet time-resolved photoelectron spectroscopy journal August 2018
Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy journal November 2019
Time-resolved photoelectron spectroscopy: from wavepackets to observables journal January 2011
Dipole-allowed excited states of N2: Potential energy curves, vibrational analysis, and absorption intensities journal October 2001
Calculation of Rydberg Levels in the Nitrogen Molecule journal August 1965
Nonadiabatic representations of the 1 Σ + u and 1 Π u states of the N 2 molecule journal September 1983
Complete dipole oscillator strength distribution and its moments for N 2   journal February 1985
A b i n i t i o calculations of potential energy curves and transition moments of 1 Σ + g and 1 Σ + u states of N 2 journal January 1987
Femtosecond time‐resolved ionization spectroscopy of ultrafast internal‐conversion dynamics in polyatomic molecules: Theory and computational studies journal December 1991
Femtosecond time‐resolved photoionization and photoelectron spectroscopy studies of ultrafast internal conversion in 1,3,5‐hexatriene journal January 1996
Femtosecond energy- and angle-resolved photoelectron spectroscopy journal May 2000
Isotope effects and spectroscopic assignments in the non-dissociative photoionization spectrum of N 2 journal May 2014
Excited state dynamics in SO 2 . I. Bound state relaxation studied by time-resolved photoelectron-photoion coincidence spectroscopy journal May 2014
A table-top monochromator for tunable femtosecond XUV pulses generated in a semi-infinite gas cell: Experiment and simulations journal July 2016
Time-resolved photoelectron imaging with a femtosecond vacuum-ultraviolet light source: Dynamics in the A∼/B∼- and F∼-bands of SO2 journal February 2017
Time-resolved photoelectron imaging of complex resonances in molecular nitrogen journal April 2021
Time-dependent view of an isotope effect in electron-nuclear nonequilibrium dynamics with applications to N 2 journal May 2018
Ab initio approach to the multichannel quantum defect calculation of the electronic autoionisation in the Hopfield series of N 2 journal December 1983
Studies of photoionization and photodissociation of N2in the 15-30 eV region using intense synchrotron radiation journal August 1991
An ab initio study of singlet and triplet Rydberg states of N 2 journal June 2013
Observation of autoionization dynamics and sub-cycle quantum beating in electronic molecular wave packets journal February 2016
Simultaneous real-time tracking of wave packets evolving on two different potential curves in H 2 + and D 2 + journal September 2005
Imaging the time-dependent structure of a molecule as it undergoes dynamics journal November 2005
Understanding the modulation mechanism in resonance-enhanced multiphoton probing of molecular dynamics journal March 2015
Probing calculated O 2 + potential-energy curves with an XUV-IR pump-probe experiment journal April 2015
Imaging the breakdown of molecular-frame dynamics through rotational uncoupling journal June 2017
Following coherent multichannel nuclear wave packets in pump-probe studies of O 2 with ultrashort laser pulses journal April 2018
Non-Born-Oppenheimer electronic wave packet in molecular nitrogen at 14 eV probed by time-resolved photoelectron spectroscopy journal February 2019
Molecular Dissociative Ionization and Wave-Packet Dynamics Studied Using Two-Color XUV and IR Pump-Probe Spectroscopy journal September 2009
High-Harmonic Spectroscopy of Oriented OCS Molecules: Emission of Even and Odd Harmonics journal December 2012
Two-Pulse Field-Free Orientation Reveals Anisotropy of Molecular Shape Resonance journal July 2014
Direct Imaging of Transient Fano Resonances in N 2 Using Time-, Energy-, and Angular-Resolved Photoelectron Spectroscopy journal April 2016
Two-Color Multiphoton Ionization of Atoms Using High-Order Harmonic Radiation journal May 1995
Complete Characterization of Molecular Dynamics in Ultrashort Laser Fields journal October 2007
Attosecond physics journal February 2009
Measurement and laser control of attosecond charge migration in ionized iodoacetylene journal October 2015
VIBRATIONAL ISOTOPE SHIFTS OF ABSORPTION BANDS OF N 2 IN THE SPECTRAL REGION 720–830 Å journal June 1964
T IME -R ESOLVED P HOTOELECTRON S PECTROSCOPY OF M OLECULES AND C LUSTERS journal October 2001
Probing Rydberg-Rydberg interactions in N 2 by ultrafast EUV-NIR photoelectron spectroscopy journal January 2019

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
autoionization & Auger processes
electronic excitation & ionization
ultrafast phenomena