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physica status solidi (b)

Fine Structure of the Luminescence of Solid Neon and Its Relation to Exciton Trapping and Desorption Induced by Excitonic Excitation

W. Laasch, Herbert Hagedorn, T. Kloiber, Georg Zimmerer

Published Apr 1, 1990• 15 citations
Publisher

Abstract

Abstract The luminescence of Ne* centers in solid Ne is investigated. The samples are excited with synchrotron radiation in the excitonic range. By an appropriate selection of the excitation energy and by time correlated measurement of the emission spectra, overlapping luminescence bands are separated and assigned to Ne* centers in different electronic states (1P1, 3P1, 3P2) and different environments in the bulk and at the surface of the solid. Lifetime measurements and excitation spectra of spectrally selected luminescence bands support the assignments, Electronic relaxation from n ≧ 2 free excitons to the n = 1 state is found to be less effective than exciton trapping into Ne* centers. Resonance fluorescence of free Ne* atoms indicates a close connection between exciton trapping and desorption.

DOI
10.1002/pssb.2221580236

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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 $4{f}^{14}5{d}^{0}6{s}^{2}{\phantom{\rule{4pt}{0ex}}}^{1}{S}_{0}$ ground-state configuration to $4{f}^{14}5{d}^{0}6s6p$ and $4{f}^{13}5{d}^{1}6{s}^{2}$ configurations. The two lowest-energy bands were assigned to outer-shell transitions to $6s6p{\phantom{\rule{4pt}{0ex}}}^{3}{P}_{1}$ 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 $4{f}^{13}5{d}^{1}6{s}^{2}$ 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 ${C}_{4v}$ 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.

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Nous avons étudié la luminescence des gaz rares solides excités par bombardement électronique. La partie haute énergie du spectre comprend des raies très fines à une énergie comparable à celle de l'exciton libre observé en réflectivité ou en absorption et une ou plusieurs bandes larges environ 1,5 eV en dessous des raies fines. Les raies fines sont dues à la recombinaison d'excitons libres ou faiblement piégés. Les bandes larges sont émises par des excitons moléculaires, formés d'atomes excités autopiégés sur un atome voisin dans son état fondamental. La différence de 1 à 2 eV entre la raie de résonance atomique et la bande de luminescence du solide est due en partie à l'énergie de liaison de l'exciton moléculaire et en partie à l'énergie potentielle de répulsion dans l'état final entre les deux atomes à une distance nettement inférieure à la distance interatomique à l'équilibre.

Le Journal de Physique Colloques•Apr 1, 1974•6 citations
Abstract The luminescence of Ne* centers in solid Ne is investigated. The samples are excited with synchrotron radiation in the excitonic range. By an appropriate selection of the excitation energy and by time correlated measurement of the emission spectra, overlapping luminescence bands are separated and assigned to Ne* centers in different electronic states (1P1, 3P1, 3P2) and different environments in the bulk and at the surface of the solid. Lifetime measurements and excitation spectra of spectrally selected luminescence bands support the assignments, Electronic relaxation from n ≧ 2 free excitons to the n = 1 state is found to be less effective than exciton trapping into Ne* centers. Resonance fluorescence of free Ne* atoms indicates a close connection between exciton trapping and desorption.
This paper presents the first results on a correlation between the luminescence of excitons self-trapped at the surface of solid argon and desorption. Recently, Jennison and Emin showed that localisation of electronic excitation at the surface of the crystal is an essential condition, and that especially self-trapping of excitons can lead to desorption of neutral atoms1. In the case of solid argon, self-trapping of excitons at the surface has been proved to exist2. It leads to characteristic luninescence bands which were also measured with electron excitation techniques3. Two of them exactly coincide with the 3P1 and 1P1 emission of isolated argon atoms and were not understood up to now. In the course of this work it turned out that they are emitted by desorbing neutral atoms.
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 4f145d06s21S04{f}^{14}5{d}^{0}6{s}^{2}{\phantom{\rule{4pt}{0ex}}}^{1}{S}_{0}4f145d06s21S0​ ground-state configuration to 4f145d06s6p4{f}^{14}5{d}^{0}6s6p4f145d06s6p and 4f135d16s24{f}^{13}5{d}^{1}6{s}^{2}4f135d16s2 configurations. The two lowest-energy bands were assigned to outer-shell transitions to 6s6p3P16s6p{\phantom{\rule{4pt}{0ex}}}^{3}{P}_{1}6s6p3P1​ and 1P1{}^{1}{P}_{1}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=1J=1J=1 states arising from the 4f135d16s24{f}^{13}5{d}^{1}6{s}^{2}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+21+21+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{C}_{4v}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{}^{1}{P}_{1}1P1​ absorption band consisted of simple, unstructured fluorescence bands.
Site-selective excitation has been used to simplify complex emission recorded in the visible spectral region for atomic europium isolated in the solid rare gases. In addition to y(8)P resonance fluorescence, excitation of the y(8)P state produces emission from the z(6)P state and the metastable a(10)D state. Very weak emission at 690 nm is tentatively assigned to the J = 9/2 level of the z(10)P state. Eu atoms isolated in the red and blue sites exhibit very different temperature dependence both spectrally and temporally. For the y(8)P state emission the red site atoms exhibit small Stokes shifts and yield radiative lifetimes while the emission from the blue site loses intensity and the temporal profiles shorten dramatically between 10 and 16 K indicating very efficient non-radiative relaxation in this site. An analysis of the Stokes shifts exhibited for the y(8)P state in each site supports the attributions made in a previous publication [O. Byrne and J.G. McCaffrey, J. Chem. Phys. 134, 124501 (2011)] that the smaller blue tetravacancy site has a greater repulsive interaction with the guest. With the exception of the y(8)P state resonance fluorescence, the recorded decay profiles of all the other emissions exhibit multiple components. This behaviour has been attributed to the existence of multiple crystal field levels arising from the splitting of the distinct spin-orbit levels from which emission occurs.
The electronic transitions of ytterbium atoms in a solid Xe matrix grown at 4.8 K are investigated. Absorption bands are detected in the regions of the gas-phase 6s2 1S0 → 4f135d6s2 and 6s2 1S0 → 6s6p 1P1 transitions. Both bands indicate that Yb atoms occupy multiple trapping sites, of which three are identified. Emission induced by the 6s2 1S0 → 6s6p 1P1 excitation is found to be concentrated entirely in the region of the 6s6p 3PJ → 6s2 1S0 decay, whereas the singlet emission is completely quenched. Multiple emission peaks are observed and the effects of annealing and prolonged irradiation on their amplitudes are found to be significant and are interpreted as a consequence of Yb population transfer from one type of site to another. Modeling of the ground-state site structure and stability predicts three Yb/Xe occupation types, substitutional (ss), tetravacancy (tv) and hexavacancy (hv), in order of decreasing stability. Their tentative associations with observed absorption and emission features are discussed. Time correlated single photon spectroscopy is used to determine the lifetimes of the individual emission bands. They are found to be different from each other with indications of a mixture of short- and long- lived 6s6p 3PJ fine-structure components and demonstrate distinct temperature dependencies. A dramatic decrease in the lifetime of the emission peak tentatively assigned to the most stable site with temperature is explained by a competition between the radiative and non-radiative decay paths of the 6s6p 3P1 state. The mechanism of the latter can be attributed to electron–phonon coupling as confirmed by a model of the temperature-dependence of the lifetime.
We have examined the luminescence from highly excited self-trapped one-center states, the relaxation processes of the band excitations, and the mechanisms of formation of highly excited quasiatomic centers in low-temperature crystals of the light rare gases and their solid solutions. The fundamental channel of population of highly excited emitting centers involves hole self-trapping with formation of two-center R2+ states; dissociative recombination of these forms one-center np5(n + 1)p excitations. We discuss the effect of self-trapping of highly excited states on the population of the lowest emitting centers in neon and argon crystals.
Nous avons étudié la luminescence des gaz rares solides excités par bombardement électronique. La partie haute énergie du spectre comprend des raies très fines à une énergie comparable à celle de l'exciton libre observé en réflectivité ou en absorption et une ou plusieurs bandes larges environ 1,5 eV en dessous des raies fines. Les raies fines sont dues à la recombinaison d'excitons libres ou faiblement piégés. Les bandes larges sont émises par des excitons moléculaires, formés d'atomes excités autopiégés sur un atome voisin dans son état fondamental. La différence de 1 à 2 eV entre la raie de résonance atomique et la bande de luminescence du solide est due en partie à l'énergie de liaison de l'exciton moléculaire et en partie à l'énergie potentielle de répulsion dans l'état final entre les deux atomes à une distance nettement inférieure à la distance interatomique à l'équilibre.