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Title: High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix

Abstract

Here, we present an experimental and theoretical study of the absorption and emission spectra of Yb atoms in a solid Ne matrix at a resolution of 0.025 nm. Five absorption bands were identified as due to transitions from the 4 f14 5 d0 6 s2 1 S 0 ground-state configuration to 4 f14 5 d0 6 s 6 p and 4 f13 5 d1 6 s2 configurations. The two lowest-energy bands were assigned to outer-shell transitions to 6 s 6 p 3 P 1 and 1 P 1 atomic states and displayed the structure of a broad doublet and an asymmetric triplet, respectively. The remaining three higher-frequency bands were assigned to inner-shell transitions to distinct J = 1 states arising from the 4 f13 5 d1 6 s2 configuration and were highly structured with narrow linewidths. A classical simulation was performed to identify the stability and symmetry of possible trapping sites in the Ne crystal. It showed that the overarching 1 + 2 structure of the high-frequency bands could be predominantly ascribed to crystal-field splitting in the axial field of a 10-atom vacancy of C 4 v symmetry. Their prominent substructures were shown to be manifestations of phonon sidebands associated with the zero-phonon lines on each crystal-field state. Unprecedented for a metal–rare-gas system, resolution of individual phonon states on an allowed electronic transition was possible under excitation spectroscopy which reflects the semiquantum nature of solid Ne. In contrast to the absorption spectra, emission spectra produced by steady-state excitation into the 1 P 1 absorption band consisted of simple, unstructured fluorescence bands.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3]; ORCiD logo [4]; ORCiD logo [3];  [3];  [5]; ORCiD logo [6];  [1]; ORCiD logo [5]; ORCiD logo [7]
  1. Chinese Academy of Sciences (CAS), Shenzhen (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of Science and Technology of China, Hefei (China)
  5. Skolkovo Institute of Science and Technology, Moscow (Russian Federation)
  6. Skolkovo Institute of Science and Technology, Moscow (Russian Federation); Moscow State University (Russian Federation)
  7. Argonne National Lab. (ANL), Argonne, IL (United States); Michigan State Univ., East Lansing, MI (United States). National Superconducting Cyclotron Lab.
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Nuclear Physics (NP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Russian Science Foundation
OSTI Identifier:
1869194
Grant/Contract Number:  
AC02-06CH11357; 17-13-01466
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 104; Journal Issue: 6; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; atomic spectra; electronic structure of atoms & molecules; Jahn-Teller effect; Van der Waals interaction

Citation Formats

Lambo, R., Xu, C. -Y., Pratt, S. T., Xu, H., Zappala, J. C., Bailey, K. G., Lu, Z. -T., Mueller, P., O'Connor, T. P., Kamorzin, B. B., Bezrukov, D. S., Xie, Y. -Q., Buchachenko, A. A., and Singh, J. T. High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix. United States: N. p., 2021. Web. doi:10.1103/physreva.104.062809.
Lambo, R., Xu, C. -Y., Pratt, S. T., Xu, H., Zappala, J. C., Bailey, K. G., Lu, Z. -T., Mueller, P., O'Connor, T. P., Kamorzin, B. B., Bezrukov, D. S., Xie, Y. -Q., Buchachenko, A. A., & Singh, J. T. High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix. United States. https://doi.org/10.1103/physreva.104.062809
Lambo, R., Xu, C. -Y., Pratt, S. T., Xu, H., Zappala, J. C., Bailey, K. G., Lu, Z. -T., Mueller, P., O'Connor, T. P., Kamorzin, B. B., Bezrukov, D. S., Xie, Y. -Q., Buchachenko, A. A., and Singh, J. T. Thu . "High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix". United States. https://doi.org/10.1103/physreva.104.062809. https://www.osti.gov/servlets/purl/1869194.
@article{osti_1869194,
title = {High-resolution spectroscopy of neutral Yb atoms in a solid Ne matrix},
author = {Lambo, R. and Xu, C. -Y. and Pratt, S. T. and Xu, H. and Zappala, J. C. and Bailey, K. G. and Lu, Z. -T. and Mueller, P. and O'Connor, T. P. and Kamorzin, B. B. and Bezrukov, D. S. and Xie, Y. -Q. and Buchachenko, A. A. and Singh, J. T.},
abstractNote = {Here, we present an experimental and theoretical study of the absorption and emission spectra of Yb atoms in a solid Ne matrix at a resolution of 0.025 nm. Five absorption bands were identified as due to transitions from the 4f145d06s21S0 ground-state configuration to 4f145d06s6p and 4f135d16s2 configurations. The two lowest-energy bands were assigned to outer-shell transitions to 6s6p3P1 and 1P1 atomic states and displayed the structure of a broad doublet and an asymmetric triplet, respectively. The remaining three higher-frequency bands were assigned to inner-shell transitions to distinct J=1 states arising from the 4f135d16s2 configuration and were highly structured with narrow linewidths. A classical simulation was performed to identify the stability and symmetry of possible trapping sites in the Ne crystal. It showed that the overarching 1+2 structure of the high-frequency bands could be predominantly ascribed to crystal-field splitting in the axial field of a 10-atom vacancy of C4v symmetry. Their prominent substructures were shown to be manifestations of phonon sidebands associated with the zero-phonon lines on each crystal-field state. Unprecedented for a metal–rare-gas system, resolution of individual phonon states on an allowed electronic transition was possible under excitation spectroscopy which reflects the semiquantum nature of solid Ne. In contrast to the absorption spectra, emission spectra produced by steady-state excitation into the 1P1 absorption band consisted of simple, unstructured fluorescence bands.},
doi = {10.1103/physreva.104.062809},
journal = {Physical Review A},
number = 6,
volume = 104,
place = {United States},
year = {Thu Dec 16 00:00:00 EST 2021},
month = {Thu Dec 16 00:00:00 EST 2021}
}

Works referenced in this record:

Proposal for a Sensitive Search for the Electric Dipole Moment of the Electron with Matrix-Isolated Radicals
journal, August 2006


Photophysics of metal atoms in rare-gas complexes, clusters and matrices
journal, October 1999

  • Crepin-Gilbert, C.; Tramer, A.
  • International Reviews in Physical Chemistry, Vol. 18, Issue 4
  • DOI: 10.1080/014423599229901

Enhanced spin coherence of rubidium atoms in solid parahydrogen
journal, July 2019


Optical pumping of rubidium atoms frozen in solid argon
journal, December 2013


Optical Excitation and Decay Dynamics of Ytterbium Atoms Embedded in a Solid Neon Matrix
journal, August 2011


Monte Carlo simulations of the structures and optical absorption spectra of Na atoms in Ar clusters, surfaces, and solids
journal, September 1994

  • Boatz, Jerry A.; Fajardo, Mario E.
  • The Journal of Chemical Physics, Vol. 101, Issue 5
  • DOI: 10.1063/1.467532

Empirically Modified Potentials of Interaction between Rare Gases for Matrix Isolation Problems
journal, August 2019

  • Bezrukov, D. S.; Kleshchina, N. N.; Kalinina, I. S.
  • Russian Journal of Physical Chemistry A, Vol. 93, Issue 8
  • DOI: 10.1134/S003602441908003X

Measurement of the Hyperfine Quenching Rate of the Clock Transition in Yb 171
journal, July 2014


Quantum guidelines for solid-state spin defects
journal, April 2021


Structural Form of Vibronic Bands in Crystals
journal, December 1964

  • Wagner, Max
  • The Journal of Chemical Physics, Vol. 41, Issue 12
  • DOI: 10.1063/1.1725839

The Dipolar Broadening of Magnetic Resonance Lines in Crystals
journal, November 1948


Electronic interaction anisotropy between open-shell lanthanide atoms and helium from cold collision experiment
journal, September 2005

  • Krems, R. V.; Buchachenko, A. A.
  • The Journal of Chemical Physics, Vol. 123, Issue 10
  • DOI: 10.1063/1.2052687

Energies, Landé Factors, and Lifetimes for Some Excited Levels of Neutral Ytterbium (Z = 70)
journal, March 2011


Electronic spectroscopy of ytterbium in a neon matrix
journal, November 2012

  • Lambo, R.; Buchachenko, A. A.; Wu, L.
  • The Journal of Chemical Physics, Vol. 137, Issue 20
  • DOI: 10.1063/1.4768419

Crystal field splitting on D↔S transitions of atomic manganese isolated in solid krypton
journal, May 2010

  • Byrne, O.; Collier, M. A.; Ryan, M. C.
  • Low Temperature Physics, Vol. 36, Issue 5
  • DOI: 10.1063/1.3432260

Hyperfine structure and isotope shift of transitions in Yb I using UV and deep-UV cw laser light and the angular distribution of fluorescence radiation
journal, June 2002

  • Zinkstok, R.; Duijn, E. J. van; Witte, S.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 35, Issue 12
  • DOI: 10.1088/0953-4075/35/12/305

Trapping sites of Li atom in the rare gas crystals Ar, Kr, and Xe: Analysis of stability and manifestation in the EPR spectra
journal, February 2020

  • Tarakanova, A. S.; Buchachenko, A. A.; Bezrukov, D. S.
  • Low Temperature Physics, Vol. 46, Issue 2
  • DOI: 10.1063/10.0000535

Evolutionary method for predicting surface reconstructions with variable stoichiometry
journal, May 2013


Electric dipole moments of atoms, molecules, nuclei, and particles
journal, January 2019


Modeling of Manganese Atom and Dimer Isolated in Solid Rare Gases: Structure, Stability, and Effect on Spin Coupling
journal, March 2017

  • Kleshchina, Nadezhda N.; Korchagina, Kseniia A.; Bezrukov, Dmitry S.
  • The Journal of Physical Chemistry A, Vol. 121, Issue 12
  • DOI: 10.1021/acs.jpca.6b12444

Detection of atomic nuclear reaction products via optical imaging
journal, June 2019


Optical Absorption Spectra of Alkali Atoms in Rare-Gas Matrices
journal, January 1965


Ultralong Spin-Coherence Times for Rubidium Atoms in Solid Parahydrogen via Dynamical Decoupling
journal, July 2020


Longitudinal Spin Relaxation of Optically Pumped Rubidium Atoms in Solid Parahydrogen
journal, October 2016


Advances in the theoretical understanding of photon upconversion in rare-earth activated nanophosphors
journal, January 2015


Magnetic trapping of rare-earth atoms at millikelvin temperatures
journal, September 2004

  • Hancox, Cindy I.; Doret, S. Charles; Hummon, Matthew T.
  • Nature, Vol. 431, Issue 7006
  • DOI: 10.1038/nature02938

Eu/RG absorption and excitation spectroscopy in the solid rare gases: State dependence of crystal field splitting and Jahn–Teller coupling
journal, March 2011

  • Byrne, Owen; McCaffrey, John G.
  • The Journal of Chemical Physics, Vol. 134, Issue 12
  • DOI: 10.1063/1.3564947

Nonadiabatic dynamics and electronic energy relaxation of Cl( 2 P ) atoms in solid Ar
journal, September 1996

  • Krylov, A. I.; Gerber, R. B.; Coalson, R. D.
  • The Journal of Chemical Physics, Vol. 105, Issue 11
  • DOI: 10.1063/1.472305

Stable axially symmetric atomic impurity in an fcc solid—Ba in rare gases
journal, September 2019

  • Kleshchina, Nadezhda N.; Kalinina, Inna S.; Leibin, Iosif V.
  • The Journal of Chemical Physics, Vol. 151, Issue 12
  • DOI: 10.1063/1.5118876

Imaging individual barium atoms in solid xenon for barium tagging in nEXO
journal, April 2019


Experiment versus molecular dynamics simulation: Spectroscopy of Ba–(Ar) n clusters
journal, January 1994

  • Visticot, J. P.; de Pujo, P.; Mestdagh, J. M.
  • The Journal of Chemical Physics, Vol. 100, Issue 1
  • DOI: 10.1063/1.466986

Absorption spectroscopy of heavy alkaline earth metals Ba and Sr in rare gas matrices—CCSD(T) calculations and atomic site occupancies
journal, January 2016

  • Davis, Barry M.; McCaffrey, John G.
  • The Journal of Chemical Physics, Vol. 144, Issue 4
  • DOI: 10.1063/1.4940688

Applications of Huang–Rhys theory in semiconductor optical spectroscopy
journal, September 2019


An investigation of the sites occupied by atomic barium in solid xenon—A 2D-EE luminescence spectroscopy and molecular dynamics study
journal, March 2018

  • Davis, Barry M.; Gervais, Benoit; McCaffrey, John G.
  • The Journal of Chemical Physics, Vol. 148, Issue 12
  • DOI: 10.1063/1.5019890

Optical spectra of Yb atoms and dimers in rare gas matrices
journal, November 1988

  • Suzer, Sefik; Andrews, Lester
  • The Journal of Chemical Physics, Vol. 89, Issue 9
  • DOI: 10.1063/1.455576

Orientation-dependent hyperfine structure of polar molecules in a rare-gas matrix: A scheme for measuring the electron electric dipole moment
journal, September 2018


Metal atom (Zn, Cd and Mg) luminescence in solid neon
journal, August 2012

  • Healy, Brendan; Kerins, Paul; McCaffrey, John G.
  • Low Temperature Physics, Vol. 38, Issue 8
  • DOI: 10.1063/1.4739854

Heat- and light-induced transformations of Yb trapping sites in an Ar matrix
journal, November 2015

  • Tao, L. -G.; Kleshchina, N. N.; Lambo, R.
  • The Journal of Chemical Physics, Vol. 143, Issue 17
  • DOI: 10.1063/1.4934999

Long Electronic Spin Relaxation Times of Cs Atoms in Solid 4 He
journal, February 1995


Luminescence of Atomic Barium in Rare Gas Matrices: A Two-Dimensional Excitation/Emission Spectroscopy Study
journal, August 2018

  • Davis, Barry; McCaffrey, John G.
  • The Journal of Physical Chemistry A, Vol. 122, Issue 37
  • DOI: 10.1021/acs.jpca.8b05140

Investigations of the Optical Spectroscopy of Atomic Sodium Isolated in Solid Argon and Krypton: Experiments and Simulations.
journal, March 2010

  • Ryan, Maryanne; Collier, Martin; Pujo, Patrick de
  • The Journal of Physical Chemistry A, Vol. 114, Issue 9
  • DOI: 10.1021/jp905596a

Dipolar Broadening of Magnetic Resonance Lines in Magnetically Diluted Crystals
journal, April 1953


Triplet emission of atomic ytterbium isolated in a xenon matrix
journal, July 2019

  • Kleshchina, N. N.; Kalinina, I. S.; Lambo, R.
  • Low Temperature Physics, Vol. 45, Issue 7
  • DOI: 10.1063/1.5111293

A degenerate model of vibronic transitions for analyzing 4f–5d spectra
journal, August 2014


Extended Analysis of the Emission Spectrum of Neutral Ytterbium (Yb I)
journal, July 1979


Generic accommodations of an atom in the Lennard-Jones fcc and hcp rare-gas solids: A computational study
journal, May 2021

  • Ozerov, Georgiy K.; Bezrukov, Dmitry S.; Buchachenko, Alexei A.
  • Physical Review B, Vol. 103, Issue 18
  • DOI: 10.1103/PhysRevB.103.184110

Subnanometer optical linewidth of thulium atoms in rare-gas crystals
journal, February 2019