Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats
Abstract
Electronic wavepackets composed of multiple bound excited states of atomic neon lying between 19.6 and 21.5 eV are launched using an isolated attosecond pulse. Individual quantum beats of the wavepacket are detected by perturbing the induced polarization of the medium with a time-delayed few-femtosecond near-infrared (NIR) pulse via coupling the individual states to multiple neighboring levels. All of the initially excited states are monitored simultaneously in the attosecond transient absorption spectrum, revealing Lorentzian to Fano lineshape spectral changes as well as quantum beats. The most prominent beating of the several that were observed was in the spin–orbit split 3d absorption features, which has a 40 femtosecond period that corresponds to the spin–orbit splitting of 0.1 eV. The few-level models and multilevel calculations confirm that the observed magnitude of oscillation depends strongly on the spectral bandwidth and tuning of the NIR pulse and on the location of possible coupling states.
- Authors:
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1342280
- Alternate Identifier(s):
- OSTI ID: 1213049
- Grant/Contract Number:
- AC02-05CH11231; FG02-13ER16403
- Resource Type:
- Published Article
- Journal Name:
- New Journal of Physics
- Additional Journal Information:
- Journal Name: New Journal of Physics Journal Volume: 16 Journal Issue: 11; Journal ID: ISSN 1367-2630
- Publisher:
- IOP Publishing
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; condensed matter; electrical, magnetic and optical
Citation Formats
Beck, Annelise R., Bernhardt, Birgitta, Warrick, Erika R., Wu, Mengxi, Chen, Shaohao, Gaarde, Mette B., Schafer, Kenneth J., Neumark, Daniel M., and Leone, Stephen R. Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats. United Kingdom: N. p., 2014.
Web. doi:10.1088/1367-2630/16/11/113016.
Beck, Annelise R., Bernhardt, Birgitta, Warrick, Erika R., Wu, Mengxi, Chen, Shaohao, Gaarde, Mette B., Schafer, Kenneth J., Neumark, Daniel M., & Leone, Stephen R. Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats. United Kingdom. https://doi.org/10.1088/1367-2630/16/11/113016
Beck, Annelise R., Bernhardt, Birgitta, Warrick, Erika R., Wu, Mengxi, Chen, Shaohao, Gaarde, Mette B., Schafer, Kenneth J., Neumark, Daniel M., and Leone, Stephen R. Sat .
"Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats". United Kingdom. https://doi.org/10.1088/1367-2630/16/11/113016.
@article{osti_1342280,
title = {Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats},
author = {Beck, Annelise R. and Bernhardt, Birgitta and Warrick, Erika R. and Wu, Mengxi and Chen, Shaohao and Gaarde, Mette B. and Schafer, Kenneth J. and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Electronic wavepackets composed of multiple bound excited states of atomic neon lying between 19.6 and 21.5 eV are launched using an isolated attosecond pulse. Individual quantum beats of the wavepacket are detected by perturbing the induced polarization of the medium with a time-delayed few-femtosecond near-infrared (NIR) pulse via coupling the individual states to multiple neighboring levels. All of the initially excited states are monitored simultaneously in the attosecond transient absorption spectrum, revealing Lorentzian to Fano lineshape spectral changes as well as quantum beats. The most prominent beating of the several that were observed was in the spin–orbit split 3d absorption features, which has a 40 femtosecond period that corresponds to the spin–orbit splitting of 0.1 eV. The few-level models and multilevel calculations confirm that the observed magnitude of oscillation depends strongly on the spectral bandwidth and tuning of the NIR pulse and on the location of possible coupling states.},
doi = {10.1088/1367-2630/16/11/113016},
journal = {New Journal of Physics},
number = 11,
volume = 16,
place = {United Kingdom},
year = {Sat Nov 01 00:00:00 EDT 2014},
month = {Sat Nov 01 00:00:00 EDT 2014}
}
https://doi.org/10.1088/1367-2630/16/11/113016
Web of Science
Works referenced in this record:
Transition probabilities of lines with origin in the 3d′(5/2)2, 3d′(5/2)3 and 3d′(3/2)1 levels of Ne(I).
journal, January 1978
- Martin, Piedad; Campos, Jose
- Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 19, Issue 1
Sub-cycle Oscillations in Virtual States Brought to Light
journal, January 2013
- Chini, Michael; Wang, Xiaowei; Cheng, Yan
- Scientific Reports, Vol. 3, Issue 1
Dynamics of spectral hole burning
journal, February 1988
- Brito Cruz, C. H.; Gordon, J. P.; Becker, P. C.
- IEEE Journal of Quantum Electronics, Vol. 24, Issue 2
Laser-imposed phase in resonant absorption of an isolated attosecond pulse
journal, September 2013
- Chen, Shaohao; Wu, Mengxi; Gaarde, Mette B.
- Physical Review A, Vol. 88, Issue 3
Quantum beat oscillations in the two-color-photoionization continuum of neon and their dependence on the intensity of the ionizing laser pulse
journal, September 2011
- Geiseler, Henning; Rottke, Horst; Steinmeyer, Günter
- Physical Review A, Vol. 84, Issue 3
Light-induced states in attosecond transient absorption spectra of laser-dressed helium
journal, December 2012
- Chen, Shaohao; Bell, M. Justine; Beck, Annelise R.
- Physical Review A, Vol. 86, Issue 6
Transient absorption and reshaping of ultrafast XUV light by laser-dressed helium
journal, January 2011
- Gaarde, Mette B.; Buth, Christian; Tate, Jennifer L.
- Physical Review A, Vol. 83, Issue 1
X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92
journal, July 1993
- Henke, B. L.; Gullikson, E. M.; Davis, J. C.
- Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342
Real-time observation of valence electron motion
journal, August 2010
- Goulielmakis, Eleftherios; Loh, Zhi-Heng; Wirth, Adrian
- Nature, Vol. 466, Issue 7307
High-spectral-resolution attosecond absorption spectroscopy of autoionization in xenon
journal, February 2014
- Bernhardt, Birgitta; Beck, Annelise R.; Li, Xuan
- Physical Review A, Vol. 89, Issue 2
Colloquium : Aligning molecules with strong laser pulses
journal, April 2003
- Stapelfeldt, Henrik; Seideman, Tamar
- Reviews of Modern Physics, Vol. 75, Issue 2
Analysis of Femtosecond Dynamic Absorption Spectra of Nonstationary States
journal, October 1992
- Pollard, W. T.; Mathies, R. A.
- Annual Review of Physical Chemistry, Vol. 43, Issue 1
Tunable frequency-controlled isolated attosecond pulses characterized by either 750 nm or 400 nm wavelength streak fields
journal, January 2010
- Mashiko, Hiroki; Bell, M. Justine; Beck, Annelise R.
- Optics Express, Vol. 18, Issue 25
Transient oscillations and dynamic Stark effect in semiconductors
journal, October 1988
- Lindberg, M.; Koch, S. W.
- Physical Review B, Vol. 38, Issue 11
Application of a numerical-basis-state method to strong-field excitation and ionization of hydrogen atoms
journal, July 2012
- Chen, Shaohao; Gao, Xiang; Li, Jiaming
- Physical Review A, Vol. 86, Issue 1
Breit–Pauli energy levels, lifetimes, and transition probabilities for the beryllium-like to neon-like sequences
journal, May 2004
- Froese Fischer, Charlotte; Tachiev, Georgio
- Atomic Data and Nuclear Data Tables, Vol. 87, Issue 1
Attosecond physics
journal, February 2009
- Krausz, Ferenc; Ivanov, Misha
- Reviews of Modern Physics, Vol. 81, Issue 1
Self-referencing spectral interferometry for measuring ultrashort optical pulses
journal, April 1999
- Iaconis, C.; Walmsley, I. A.
- IEEE Journal of Quantum Electronics, Vol. 35, Issue 4, p. 501-509
Transition probabilities of some lines of Ne(I)
journal, August 1979
- Martin, Piedad; Campos, Jose
- Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 22, Issue 2
Attosecond Time-Resolved Autoionization of Argon
journal, October 2010
- Wang, He; Chini, Michael; Chen, Shouyuan
- Physical Review Letters, Vol. 105, Issue 14
Time-resolved spectroscopy of attosecond quantum dynamics
journal, September 2008
- Pfeifer, Thomas; Abel, Mark J.; Nagel, Phillip M.
- Chemical Physics Letters, Vol. 463, Issue 1-3
Oscillator strengths in Ne I
journal, December 1998
- Seaton, M. J.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 31, Issue 24
Subcycle laser control and quantum interferences in attosecond photoabsorption of neon
journal, June 2013
- Wang, Xiaowei; Chini, Michael; Cheng, Yan
- Physical Review A, Vol. 87, Issue 6
Experimental transition probabilities and J -file sum rule test for the transition array 3p–3d in neutral neon
journal, November 2008
- Bacławski, A.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 41, Issue 22
Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond †
journal, June 2000
- Zewail, Ahmed H.
- The Journal of Physical Chemistry A, Vol. 104, Issue 24
Intensity dependence of light-induced states in transient absorption of laser-dressed helium measured with isolated attosecond pulses
journal, October 2013
- Bell, M. Justine; Beck, Annelise R.; Mashiko, Hiroki
- Journal of Modern Optics, Vol. 60, Issue 17
Alternating absorption features during attosecond-pulse propagation in a laser-controlled gaseous medium
journal, November 2013
- Pfeiffer, Adrian N.; Bell, M. Justine; Beck, Annelise R.
- Physical Review A, Vol. 88, Issue 5
Experimental absolute transition probabilities of lines from the 3d′(3/2)_2 level of Ne i
journal, January 1977
- Martin, Piedad; Campos, Jose
- Journal of the Optical Society of America, Vol. 67, Issue 10
Control of coherent excitation of neon in the extreme ultraviolet regime
journal, January 2011
- Plenge, Jürgen; Wirsing, Andreas; Raschpichler, Christopher
- Faraday Discussions, Vol. 153
Lorentz Meets Fano in Spectral Line Shapes: A Universal Phase and Its Laser Control
journal, May 2013
- Ott, C.; Kaldun, A.; Raith, P.
- Science, Vol. 340, Issue 6133
GRASP92: a package for large-scale relativistic atomic structure calculations
journal, December 2006
- Parpia, F. A.; Froese Fischer, C.; Grant, I. P.
- Computer Physics Communications, Vol. 175, Issue 11-12
Energies, Oscillator Strengths, and Lifetimes for Neon-like Ions Up to Kr XXVII
journal, January 1993
- Hibbert, A.; Ledourneuf, M.; Mohan, M.
- Atomic Data and Nuclear Data Tables, Vol. 53, Issue 1
Control of angular momentum evolution in Stark wave packets
journal, November 2003
- Wen, H.; Rangan, C.; Bucksbaum, P. H.
- Physical Review A, Vol. 68, Issue 5
GRASP92: A package for large-scale relativistic atomic structure calculations
journal, April 1996
- Parpia, F. A.; Fischer, C. Froese; Grant, I. P.
- Computer Physics Communications, Vol. 94, Issue 2-3
Works referencing / citing this record:
Space–time control of free induction decay in the extreme ultraviolet
journal, March 2017
- Bengtsson, S.; Larsen, E. W.; Kroon, D.
- Nature Photonics, Vol. 11, Issue 4
Frequency-resolved optical gating technique for retrieving the amplitude of a vibrational wavepacket
journal, June 2015
- Nabekawa, Yasuo; Furukawa, Yusuke; Okino, Tomoya
- Scientific Reports, Vol. 5, Issue 1
Reconstruction of an excited-state molecular wave packet with attosecond transient absorption spectroscopy
journal, August 2016
- Cheng, Yan; Chini, Michael; Wang, Xiaowei
- Physical Review A, Vol. 94, Issue 2
First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory
journal, June 2018
- Sato, Shunsuke A.; Hübener, Hannes; Rubio, Angel
- The European Physical Journal B, Vol. 91, Issue 6
Attosecond optics and technology: progress to date and future prospects [Invited]
journal, January 2016
- Chang, Zenghu; Corkum, Paul B.; Leone, Stephen R.
- Journal of the Optical Society of America B, Vol. 33, Issue 6
Ab Initio Simulation of Attosecond Transient Absorption Spectroscopy in Two-Dimensional Materials
journal, September 2018
- Sato, Shunsuke; Hübener, Hannes; De Giovannini, Umberto
- Applied Sciences, Vol. 8, Issue 10