Direct experimental observation of weakly-bound character of the attached electron in europium anion
Identifieur interne : 000069 ( Pmc/Checkpoint ); précédent : 000068; suivant : 000070Direct experimental observation of weakly-bound character of the attached electron in europium anion
Auteurs : Shi-Bo Cheng [États-Unis] ; A. W. Castleman [États-Unis]Source :
- Scientific Reports [ 2045-2322 ] ; 2015.
Abstract
Direct experimental determination of precise electron affinities (EAs) of lanthanides is a longstanding challenge to experimentalists. Considerable debate exists in previous experiment and theory, hindering the complete understanding about the properties of the atomic anions. Herein, we report the first precise photoelectron imaging spectroscopy of europium (Eu), with the aim of eliminating prior contradictions. The measured EA (0.116 ± 0.013 eV) of Eu is in excellent agreement with recently reported theoretical predictions, providing direct spectroscopic evidence that the additional electron is weakly attached. Additionally, a new experimental strategy is proposed that can significantly increase the yield of the lanthanide anions, opening up the best opportunity to complete the periodic table of the atomic anions. The present findings not only serve to resolve previous discrepancy but also will help in improving the depth and accuracy of our understanding about the fundamental properties of the atomic anions.
Url:
DOI: 10.1038/srep12414
PubMed: 26198741
PubMed Central: 4510523
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">Direct experimental observation of weakly-bound character of the attached electron in
europium anion</title><author><name sortKey="Cheng, Shi Bo" sort="Cheng, Shi Bo" uniqKey="Cheng S" first="Shi-Bo" last="Cheng">Shi-Bo Cheng</name><affiliation wicri:level="1"><nlm:aff id="a1"><institution>Department of Chemistry, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Castleman, A W" sort="Castleman, A W" uniqKey="Castleman A" first="A. W." last="Castleman">A. W. Castleman</name><affiliation wicri:level="1"><nlm:aff id="a1"><institution>Department of Chemistry, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="a2"><institution>Department of Physics, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author></titleStmt><publicationStmt><idno type="wicri:source">PMC</idno><idno type="pmid">26198741</idno><idno type="pmc">4510523</idno><idno type="url">http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4510523</idno><idno type="RBID">PMC:4510523</idno><idno type="doi">10.1038/srep12414</idno><date when="2015">2015</date><idno type="wicri:Area/Pmc/Corpus">000088</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Corpus" wicri:corpus="PMC">000088</idno><idno type="wicri:Area/Pmc/Curation">000088</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Curation">000088</idno><idno type="wicri:Area/Pmc/Checkpoint">000069</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Checkpoint">000069</idno></publicationStmt><sourceDesc><biblStruct><analytic><title xml:lang="en" level="a" type="main">Direct experimental observation of weakly-bound character of the attached electron in
europium anion</title><author><name sortKey="Cheng, Shi Bo" sort="Cheng, Shi Bo" uniqKey="Cheng S" first="Shi-Bo" last="Cheng">Shi-Bo Cheng</name><affiliation wicri:level="1"><nlm:aff id="a1"><institution>Department of Chemistry, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Castleman, A W" sort="Castleman, A W" uniqKey="Castleman A" first="A. W." last="Castleman">A. W. Castleman</name><affiliation wicri:level="1"><nlm:aff id="a1"><institution>Department of Chemistry, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="a2"><institution>Department of Physics, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author></analytic><series><title level="j">Scientific Reports</title><idno type="eISSN">2045-2322</idno><imprint><date when="2015">2015</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en"><p>Direct experimental determination of precise electron affinities (EAs) of lanthanides
is a longstanding challenge to experimentalists. Considerable debate exists in
previous experiment and theory, hindering the complete understanding about the
properties of the atomic anions. Herein, we report the first precise photoelectron
imaging spectroscopy of europium (Eu), with the aim of eliminating prior
contradictions. The measured EA
(0.116 ± 0.013 eV) of Eu is in
excellent agreement with recently reported theoretical predictions, providing direct
spectroscopic evidence that the additional electron is weakly attached.
Additionally, a new experimental strategy is proposed that can significantly
increase the yield of the lanthanide anions, opening up the best opportunity to
complete the periodic table of the atomic anions. The present findings not only
serve to resolve previous discrepancy but also will help in improving the depth and
accuracy of our understanding about the fundamental properties of the atomic
anions.</p></div></front><back><div1 type="bibliography"><listBibl><biblStruct><analytic><author><name sortKey="Drzaic, P S" uniqKey="Drzaic P">P. S. Drzaic</name></author><author><name sortKey="Marks, J" uniqKey="Marks J">J. Marks</name></author><author><name sortKey="Brauman, J X0a I" uniqKey="Brauman J">J.
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<front><journal-meta><journal-id journal-id-type="nlm-ta">Sci Rep</journal-id><journal-id journal-id-type="iso-abbrev">Sci Rep</journal-id><journal-title-group><journal-title>Scientific Reports</journal-title></journal-title-group><issn pub-type="epub">2045-2322</issn><publisher><publisher-name>Nature Publishing Group</publisher-name></publisher></journal-meta><article-meta><article-id pub-id-type="pmid">26198741</article-id><article-id pub-id-type="pmc">4510523</article-id><article-id pub-id-type="pii">srep12414</article-id><article-id pub-id-type="doi">10.1038/srep12414</article-id><article-categories><subj-group subj-group-type="heading"><subject>Article</subject></subj-group></article-categories><title-group><article-title>Direct experimental observation of weakly-bound character of the attached electron in
europium anion</article-title></title-group><contrib-group><contrib contrib-type="author"><name><surname>Cheng</surname><given-names>Shi-Bo</given-names></name><xref ref-type="aff" rid="a1">1</xref></contrib><contrib contrib-type="author"><name><surname>Castleman</surname><given-names>A. W.</given-names><suffix>Jr.</suffix></name><xref ref-type="corresp" rid="c1">a</xref><xref ref-type="aff" rid="a1">1</xref><xref ref-type="aff" rid="a2">2</xref></contrib><aff id="a1"><label>1</label><institution>Department of Chemistry, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></aff><aff id="a2"><label>2</label><institution>Department of Physics, The Pennsylvania State University</institution>, University Park, Pennsylvania 16802,<country>United States</country></aff></contrib-group><author-notes><corresp id="c1"><label>a</label><email>awc@psu.edu</email></corresp></author-notes><pub-date pub-type="epub"><day>22</day><month>07</month><year>2015</year></pub-date><pub-date pub-type="collection"><year>2015</year></pub-date><volume>5</volume><elocation-id>12414</elocation-id><history><date date-type="received"><day>09</day><month>04</month><year>2015</year></date><date date-type="accepted"><day>22</day><month>06</month><year>2015</year></date></history><permissions><copyright-statement>Copyright © 2015, Macmillan Publishers Limited</copyright-statement><copyright-year>2015</copyright-year><copyright-holder>Macmillan Publishers Limited</copyright-holder><license license-type="open-access" xlink:href="http://creativecommons.org/licenses/by/4.0/"><pmc-comment>author-paid</pmc-comment>
<license-p>This work is licensed under a Creative Commons Attribution 4.0
International License. The images or other third party material in this article are
included in the article’s Creative Commons license, unless indicated
otherwise in the credit line; if the material is not included under the Creative
Commons license, users will need to obtain permission from the license holder to
reproduce the material. To view a copy of this license, visit <ext-link ext-link-type="uri" xlink:href="http://creativecommons.org/licenses/by/4.0/">http://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><abstract><p>Direct experimental determination of precise electron affinities (EAs) of lanthanides
is a longstanding challenge to experimentalists. Considerable debate exists in
previous experiment and theory, hindering the complete understanding about the
properties of the atomic anions. Herein, we report the first precise photoelectron
imaging spectroscopy of europium (Eu), with the aim of eliminating prior
contradictions. The measured EA
(0.116 ± 0.013 eV) of Eu is in
excellent agreement with recently reported theoretical predictions, providing direct
spectroscopic evidence that the additional electron is weakly attached.
Additionally, a new experimental strategy is proposed that can significantly
increase the yield of the lanthanide anions, opening up the best opportunity to
complete the periodic table of the atomic anions. The present findings not only
serve to resolve previous discrepancy but also will help in improving the depth and
accuracy of our understanding about the fundamental properties of the atomic
anions.</p></abstract></article-meta></front><floats-group><fig id="f1"><label>Figure 1</label><caption><title>Time-of-flight mass spectrum of Eu<sup>−</sup> and
monoeuropium oxide clusters.</title><p>The inset shows the enlarged spectrum in the range of 140 to
190 m/z.</p></caption><graphic xlink:href="srep12414-f1"></graphic></fig><fig id="f2"><label>Figure 2</label><caption><title>Photoelectron image and corresponding photoelectron spectrum of
Eu<sup>−</sup>.</title><p>The spectrum was obtained at 532 nm photon energy. The inset
shows the enlarged spectrum in the range of 0 to 0.4 eV.</p></caption><graphic xlink:href="srep12414-f2"></graphic></fig><fig id="f3"><label>Figure 3</label><caption><title>Schematic of energy levels in neutral and anionic Eu observed in the
experiment.</title><p>The energy levels of the neutral Eu are obtained from Ref. <xref ref-type="bibr" rid="b43">43</xref>, while those of the anionic Eu are acquired from the
present experiment. The EA of Eu is defined as the energy difference between
the lowest energy levels of the neutral and the anion. Leading electronic
configurations and LS terms are included.</p></caption><graphic xlink:href="srep12414-f3"></graphic></fig><fig id="f4"><label>Figure 4</label><caption><title>Enlarged photoelectron spectrum of Eu<sup>−</sup> between 1.63 and 2.30 eV.</title><p>Transitions from anionic ground state to
different excited states of neutral Eu atom are labeled using different
letter series (A<sub><italic>i</italic></sub>, B<sub><italic>i</italic></sub>, …),
and are indicated by different color lines. Transitions from one excited
anionic state are marked with apostrophe.</p></caption><graphic xlink:href="srep12414-f4"></graphic></fig><table-wrap position="float" id="t1"><label>Table 1</label><caption><title>Atomic energy levels (in eV) in Eu<sup>0/−</sup>.</title></caption><table frame="hsides" rules="groups" border="1"><colgroup><col align="left"></col><col align="char" char="."></col><col align="char" char="."></col><col align="center"></col><col align="center"></col></colgroup><thead valign="bottom"><tr><th align="left" valign="top" charoff="50">Band</th><th align="center" valign="top" char="." charoff="50">Binding energy (eV)</th><th align="center" valign="top" char="." charoff="50">Atomic energy level (eV) (this work)</th><th align="center" valign="top" charoff="50">Atomic energy level (eV) (Ref. <xref ref-type="bibr" rid="b43">43</xref>)</th><th align="center" valign="top" charoff="50">Term of final state</th></tr></thead><tbody valign="top"><tr><td align="left" valign="top" charoff="50">X'</td><td align="center" valign="top" char="." charoff="50">0.039</td><td align="center" valign="top" char="." charoff="50">−0.077</td><td align="center" valign="top" charoff="50">—</td><td align="center" valign="top" charoff="50">—</td></tr><tr><td align="left" valign="top" charoff="50">X</td><td align="center" valign="top" char="." charoff="50">0.116</td><td align="center" valign="top" char="." charoff="50">0</td><td align="center" valign="top" charoff="50">0</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>S</italic><sub>7/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">A</td><td align="center" valign="top" char="." charoff="50">1.725</td><td align="center" valign="top" char="." charoff="50">1.609</td><td align="char" valign="top" char="." charoff="50">1.602</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>D</italic><sub>5/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">A<sub>1</sub></td><td align="center" valign="top" char="." charoff="50">1.746</td><td align="center" valign="top" char="." charoff="50">1.630</td><td align="char" valign="top" char="." charoff="50">1.618</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>D</italic><sub>7/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">A<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">1.773</td><td align="center" valign="top" char="." charoff="50">1.657</td><td align="char" valign="top" char="." charoff="50">1.639</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>D</italic><sub>9/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">A<sub>3</sub></td><td align="center" valign="top" char="." charoff="50">1.797</td><td align="center" valign="top" char="." charoff="50">1.681</td><td align="char" valign="top" char="." charoff="50">1.668</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>D</italic><sub>11/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">A<sub>4</sub></td><td align="center" valign="top" char="." charoff="50">1.830</td><td align="center" valign="top" char="." charoff="50">1.718</td><td align="char" valign="top" char="." charoff="50">1.708</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>D</italic><sub>13/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">B</td><td align="center" valign="top" char="." charoff="50">1.864</td><td align="center" valign="top" char="." charoff="50">1.748</td><td align="char" valign="top" char="." charoff="50">1.744</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>P</italic><sub>7/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">B<sub>1</sub></td><td align="center" valign="top" char="." charoff="50">1.910</td><td align="center" valign="top" char="." charoff="50">1.794</td><td align="char" valign="top" char="." charoff="50">1.806</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>P</italic><sub>9/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">C</td><td align="center" valign="top" char="." charoff="50">1.995</td><td align="center" valign="top" char="." charoff="50">1.879</td><td align="char" valign="top" char="." charoff="50">1.877</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>D</italic><sub>3/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">C<sub>1</sub></td><td align="center" valign="top" char="." charoff="50">2.009</td><td align="center" valign="top" char="." charoff="50">1.893</td><td align="char" valign="top" char="." charoff="50">1.891</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>D</italic><sub>5/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">C<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">2.024</td><td align="center" valign="top" char="." charoff="50">1.908</td><td align="char" valign="top" char="." charoff="50">1.912</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>D</italic><sub>7/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">B<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">2.044</td><td align="center" valign="top" char="." charoff="50">1.928</td><td align="char" valign="top" char="." charoff="50">1.932</td><td align="center" valign="top" charoff="50"><sup>10</sup><italic>P</italic><sub>11/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">C<sub>3</sub></td><td align="center" valign="top" char="." charoff="50">2.063</td><td align="center" valign="top" char="." charoff="50">1.947</td><td align="char" valign="top" char="." charoff="50">1.944</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>D</italic><sub>9/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">D</td><td align="center" valign="top" char="." charoff="50">2.088</td><td align="center" valign="top" char="." charoff="50">1.972</td><td align="char" valign="top" char="." charoff="50">1.970</td><td align="center" valign="top" charoff="50"><sup>8</sup><italic>P</italic><sub>5/2</sub></td></tr><tr><td align="left" valign="top" charoff="50">E</td><td align="center" valign="top" char="." charoff="50">2.261</td><td align="center" valign="top" char="." charoff="50">2.145</td><td align="char" valign="top" char="." charoff="50">2.150</td><td align="center" valign="top" charoff="50"><sup>6</sup><italic>P</italic><sub>7/2</sub></td></tr></tbody></table><table-wrap-foot><fn id="t1-fn1"><p>Experimental binding energies (BEs) have an uncertainty of
±0.013 eV. The present atomic energy
levels are obtained by calculating the energy differences
between peak X and other peaks observed in the photoelectron
spectrum. The referenced spectroscopic data are obtained
from Ref. <xref ref-type="bibr" rid="b43">43</xref>.</p></fn></table-wrap-foot></table-wrap><table-wrap position="float" id="t2"><label>Table 2</label><caption><title>Observed transitions originating from one excited state of
Eu<sup>−</sup>, in eV.</title></caption><table frame="hsides" rules="groups" border="1"><colgroup><col align="left"></col><col align="char" char="."></col><col align="center"></col><col align="char" char="."></col><col align="char" char="."></col></colgroup><thead valign="bottom"><tr><th align="left" valign="top" charoff="50">Band</th><th align="center" valign="top" char="." charoff="50">Binding energy (eV)</th><th align="center" valign="top" charoff="50">Paired peak</th><th align="center" valign="top" char="." charoff="50">Binding energy (eV)</th><th align="center" valign="top" char="." charoff="50">ΔE (eV)</th></tr></thead><tbody valign="top"><tr><td align="left" valign="top" charoff="50">A'</td><td align="center" valign="top" char="." charoff="50">1.650</td><td align="center" valign="top" charoff="50">A</td><td align="center" valign="top" char="." charoff="50">1.725</td><td align="center" valign="top" char="." charoff="50">0.075</td></tr><tr><td align="left" valign="top" charoff="50">A<sub>1</sub>'</td><td align="center" valign="top" char="." charoff="50">1.672</td><td align="center" valign="top" charoff="50">A<sub>1</sub></td><td align="center" valign="top" char="." charoff="50">1.746</td><td align="center" valign="top" char="." charoff="50">0.074</td></tr><tr><td align="left" valign="top" charoff="50">A<sub>2</sub>'</td><td align="center" valign="top" char="." charoff="50">1.699</td><td align="center" valign="top" charoff="50">A<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">1.773</td><td align="center" valign="top" char="." charoff="50">0.074</td></tr><tr><td align="left" valign="top" charoff="50">C'</td><td align="center" valign="top" char="." charoff="50">1.920</td><td align="center" valign="top" charoff="50">C</td><td align="center" valign="top" char="." charoff="50">1.995</td><td align="center" valign="top" char="." charoff="50">0.075</td></tr><tr><td align="left" valign="top" charoff="50">C<sub>2</sub>'</td><td align="center" valign="top" char="." charoff="50">1.950</td><td align="center" valign="top" charoff="50">C<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">2.024</td><td align="center" valign="top" char="." charoff="50">0.074</td></tr><tr><td align="left" valign="top" charoff="50">B<sub>2</sub>'</td><td align="center" valign="top" char="." charoff="50">1.967</td><td align="center" valign="top" charoff="50">B<sub>2</sub></td><td align="center" valign="top" char="." charoff="50">2.044</td><td align="center" valign="top" char="." charoff="50">0.077</td></tr></tbody></table><table-wrap-foot><fn id="t2-fn1"><p>Experimental binding energies (BEs) have an uncertainty of
± 0.013 eV. ΔE represent
the energy differences between peaks A' and A,
A<sub>1</sub>' and A<sub>1</sub>,
A<sub>2</sub>' and A<sub>2</sub> and so
on.</p></fn></table-wrap-foot></table-wrap></floats-group></pmc><affiliations><list><country><li>États-Unis</li></country></list><tree><country name="États-Unis"><noRegion><name sortKey="Cheng, Shi Bo" sort="Cheng, Shi Bo" uniqKey="Cheng S" first="Shi-Bo" last="Cheng">Shi-Bo Cheng</name></noRegion><name sortKey="Castleman, A W" sort="Castleman, A W" uniqKey="Castleman A" first="A. W." last="Castleman">A. W. Castleman</name><name sortKey="Castleman, A W" sort="Castleman, A W" uniqKey="Castleman A" first="A. W." last="Castleman">A. W. Castleman</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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