Assessment of the Second-Ionization Potential of Lawrencium: Investigating the End of the Actinide Series with a One-Atom-at-a-Time Gas-Phase Ion Chemistry Technique

Kwarsick, Jeffrey T.; Pore, Jennifer L.; Gates, Jacklyn M.; Gregorich, Kenneth E.; Gibson, John K.; Jian, Jiwen; Pang, Gregory K.; Shuh, David K.

doi:10.1021/acs.jpca.1c01961

Assessment of the Second-Ionization Potential of Lawrencium: Investigating the End of the Actinide Series with a One-Atom-at-a-Time Gas-Phase Ion Chemistry Technique

Journal Article · Fri Jul 09 04:00:00 EDT 2021 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.1c01961· OSTI ID:1844939

Kwarsick, Jeffrey T. ^[1]; ^[2]; Gates, Jacklyn M. ^[2]; Gregorich, Kenneth E. ^[2]; ^[2]; Jian, Jiwen ^[2]; Pang, Gregory K. ^[2]; ^[2]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Experiments were performed at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron facility to investigate the electron-transfer reduction reaction of dipositive Lr (Z = 103) with O₂ gas. Ions of ²⁵⁵Lr were produced in the fusion-evaporation reaction ²⁰⁹Bi(⁴⁸Ca,2n) ²⁵⁵Lr and were studied with a novel gas-phase ion chemistry technique. The produced ²⁵⁵Lr²⁺ ions were trapped and O₂ gas was introduced, such that the charge-exchange reaction to reduce ²⁵⁵Lr²⁺ to ²⁵⁵Lr¹⁺ was observed and the reaction rate constant was determined to be k = 1.5(7) × 10^-10 cm³/mol/s. The observation that this reaction proceeds establishes the lower limit on the second ionization potential of Lr to be 13.3(3) eV. This gives further support that the actinide series terminates with Lr. Additionally, this result can be used to better interpret the situation concerning the placement of Lu and Lr on the periodic table within the current framework of the actinide hypothesis. The success of this experimental approach now identifies unique opportunities for future gas-phase reaction studies on actinide and super heavy elements.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Nuclear Physics (NP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1844939

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 31 Vol. 125; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Chemistry of Superheavy Elements Schädel, Matthias Angewandte Chemie International Edition, Vol. 45, Issue 3 https://doi.org/10.1002/anie.200461072	journal	January 2006
The location and composition of Group 3 of the periodic table Vernon, René E. Foundations of Chemistry, Vol. 23, Issue 2 https://doi.org/10.1007/s10698-020-09384-2	journal	September 2020
On the position of La, Lu, Ac and Lr in the periodic table: a perspective Chandrasekar, Aditi; Joshi, Meenakshi; Ghanty, Tapan K. Journal of Chemical Sciences, Vol. 131, Issue 12 https://doi.org/10.1007/s12039-019-1713-7	journal	December 2019
Cold fusion reactions with 48Ca Gäggeler, H. W.; Jost, D. T.; Türler, A. Nuclear Physics A, Vol. 502 https://doi.org/10.1016/0375-9474(89)90689-1	journal	October 1989
Determination of the ionization energy of NpO2 and comparative ionization energies of actinide oxides Gibson, John K.; Haire, Richard G.; Marçalo, Joaquim Journal of Nuclear Materials, Vol. 344, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2005.04.010	journal	September 2005
Simulation of recoil trajectories in gas-filled magnetic separators Gregorich, K. E. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 711 https://doi.org/10.1016/j.nima.2013.01.020	journal	May 2013
Relativistic and quantum electrodynamic effects in superheavy elements Schwerdtfeger, Peter; Pašteka, Lukáš F.; Punnett, Andrew Nuclear Physics A, Vol. 944 https://doi.org/10.1016/j.nuclphysa.2015.02.005	journal	December 2015
Electronic structure and properties of superheavy elements Pershina, V. Nuclear Physics A, Vol. 944 https://doi.org/10.1016/j.nuclphysa.2015.04.007	journal	December 2015
FTICR-MS study of the gas-phase thermochemistry of americium oxides Santos, Marta; Marçalo, Joaquim; Leal, João Paulo International Journal of Mass Spectrometry, Vol. 228, Issue 2-3 https://doi.org/10.1016/s1387-3806(03)00138-6	journal	August 2003
The Chemical and Radioactive Properties of the Heavy Elements: Wartime acceleration in the study of the heavy elements above No. 88, which form a transition series of the rare earth type, has removed them from the unfamiliar. The discovery of elements 95 and 96, of a new isotope of neptunium, of the occurrence of plutonium in nature, and its large-scale production at Hanford, are outlined Seaborg, Glenn T. Chemical & Engineering News, Vol. 23, Issue 23 https://doi.org/10.1021/cen-v023n023.p2190	journal	December 1945
Advances in the Production and Chemistry of the Heaviest Elements Türler, Andreas; Pershina, Valeria Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr3002438	journal	October 2012
All-Electron Scalar Relativistic Basis Sets for the Actinides Pantazis, Dimitrios A.; Neese, Frank Journal of Chemical Theory and Computation, Vol. 7, Issue 3 https://doi.org/10.1021/ct100736b	journal	February 2011
First Ionization Potentials of Fm, Md, No, and Lr: Verification of Filling-Up of 5f Electrons and Confirmation of the Actinide Series Sato, Tetsuya K.; Asai, Masato; Borschevsky, Anastasia Journal of the American Chemical Society, Vol. 140, Issue 44 https://doi.org/10.1021/jacs.8b09068	journal	October 2018
Oxidation Reactions of Lanthanide Cations with N ₂ O and O ₂ : Periodicities in Reactivity Koyanagi, Gregory K.; Bohme, Diethard K. The Journal of Physical Chemistry A, Vol. 105, Issue 39 https://doi.org/10.1021/jp011627m	journal	October 2001
Gas-Phase Oxidation Reactions of Neptunium and Plutonium Ions Investigated via Fourier Transform Ion Cyclotron Resonance Mass Spectrometry Santos, Marta; Marçalo, Joaquim; Pires de Matos, António The Journal of Physical Chemistry A, Vol. 106, Issue 31 https://doi.org/10.1021/jp025733f	journal	August 2002
Oxidation Studies of Dipositive Actinide Ions, An ²⁺ (An = Th, U, Np, Pu, Am) in the Gas Phase: Synthesis and Characterization of the Isolated Uranyl, Neptunyl, and Plutonyl Ions UO ₂ ²⁺ (g), NpO ₂ ²⁺ (g), and PuO ₂ ²⁺ (g) Gibson, John K.; Haire, Richard G.; Santos, Marta The Journal of Physical Chemistry A, Vol. 109, Issue 12 https://doi.org/10.1021/jp0447340	journal	March 2005
Gas-Phase Oxidation of Cm ⁺ and Cm ²⁺ − Thermodynamics of Neutral and Ionized CmO Gibson, John K.; Haire, Richard G.; Santos, Marta The Journal of Physical Chemistry A, Vol. 112, Issue 45 https://doi.org/10.1021/jp8047899	journal	November 2008
Measurement of the first ionization potential of lawrencium, element 103 Sato, T. K.; Asai, M.; Borschevsky, A. Nature, Vol. 520, Issue 7546 https://doi.org/10.1038/nature14342	journal	April 2015
Is the chemistry of lawrencium peculiar? Xu, Wen-Hua; Pyykkö, Pekka Physical Chemistry Chemical Physics, Vol. 18, Issue 26 https://doi.org/10.1039/c6cp02706g	journal	January 2016
Prospects of A and Z identification experiments at LBNL Gates, Jacklyn M. EPJ Web of Conferences, Vol. 131 https://doi.org/10.1051/epjconf/201613108003	journal	January 2016
Relativistic prediction of the ground state of atomic Lawrencium Desclaux, J. -P.; Fricke, B. Journal de Physique, Vol. 41, Issue 9 https://doi.org/10.1051/jphys:01980004109094300	journal	January 1980
Valence basis sets for relativistic energy-consistent small-core actinide pseudopotentials Cao, Xiaoyan; Dolg, Michael; Stoll, Hermann The Journal of Chemical Physics, Vol. 118, Issue 2 https://doi.org/10.1063/1.1521431	journal	January 2003
Small General Purpose Cycloidal‐Focusing Mass Spectrometer Robinson, Charles F.; Hall, Lawrence G. Review of Scientific Instruments, Vol. 27, Issue 7 https://doi.org/10.1063/1.1715618	journal	July 1956
Trochotron Design Principles Monk, G. W.; Werner, G. K. Review of Scientific Instruments, Vol. 20, Issue 2 https://doi.org/10.1063/1.1741475	journal	February 1949
A Large Mass Spectrometer Employing Crossed Electric and Magnetic Fields Mariner, Thomas; Bleakney, Walker Review of Scientific Instruments, Vol. 20, Issue 4 https://doi.org/10.1063/1.1741511	journal	April 1949
The third generation superconducting 28 GHz electron cyclotron resonance ion source VENUS (invited) Lyneis, C.; Leitner, D.; Leitner, M. Review of Scientific Instruments, Vol. 81, Issue 2 https://doi.org/10.1063/1.3271135	journal	February 2010
Parametrization of the ion–polar molecule collision rate constant by trajectory calculations Su, Timothy; Chesnavich, Walter J. The Journal of Chemical Physics, Vol. 76, Issue 10 https://doi.org/10.1063/1.442828	journal	May 1982
Highly excited even Rydberg series of Lu I studied by two-step laser photoionisation spectroscopy Maeda, H.; Mizugai, Y.; Matsumoto, Y. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 22, Issue 18 https://doi.org/10.1088/0953-4075/22/18/002	journal	September 1989
Recent attempts to change the periodic table Scerri, Eric Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 378, Issue 2180 https://doi.org/10.1098/rsta.2019.0300	journal	August 2020
Transition energies of ytterbium, lutetium, and lawrencium by the relativistic coupled-cluster method Eliav, Ephraim; Kaldor, Uzi; Ishikawa, Yasuyuki Physical Review A, Vol. 52, Issue 1 https://doi.org/10.1103/physreva.52.291	journal	July 1995
*Ab initio* pseudopotential and density-functional all-electron study of ionization and excitation energies of actinide atoms Liu, Wenjian; Küchle, Wolfgang; Dolg, Michael Physical Review A, Vol. 58, Issue 2 https://doi.org/10.1103/physreva.58.1103	journal	August 1998
Atomic properties of superheavy elements No, Lr, and Rf Dzuba, V. A.; Safronova, M. S.; Safronova, U. I. Physical Review A, Vol. 90, Issue 1 https://doi.org/10.1103/physreva.90.012504	journal	July 2014
Ionization potentials of superheavy elements No, Lr, and Rf and their ions Dzuba, V. A.; Safronova, M. S.; Safronova, U. I. Physical Review A, Vol. 94, Issue 4 https://doi.org/10.1103/physreva.94.042503	journal	October 2016
Precision Measurement of the First Ionization Potential of Nobelium Chhetri, P.; Ackermann, D.; Backe, H. Physical Review Letters, Vol. 120, Issue 26 https://doi.org/10.1103/physrevlett.120.263003	journal	June 2018
First Direct Measurements of Superheavy-Element Mass Numbers Gates, J. M.; Pang, G. K.; Pore, J. L. Physical Review Letters, Vol. 121, Issue 22 https://doi.org/10.1103/physrevlett.121.222501	journal	November 2018
Resonance Transition Energies and Oscillator Strengths in Lutetium and Lawrencium Zou, Yu; Froese Fischer, C. Physical Review Letters, Vol. 88, Issue 18 https://doi.org/10.1103/physrevlett.88.183001	journal	April 2002
Colloquium : Superheavy elements: Oganesson and beyond Giuliani, S. A.; Matheson, Z.; Nazarewicz, W. Reviews of Modern Physics, Vol. 91, Issue 1 https://doi.org/10.1103/revmodphys.91.011001	journal	January 2019
The Transuranium Elements Seaborg, G. T. Science, Vol. 104, Issue 2704 https://doi.org/10.1126/science.104.2704.379	journal	October 1946
Transition energies of atomic lawrencium Borschevsky, A.; Eliav, E.; Vilkas, M. J. The European Physical Journal D, Vol. 45, Issue 1 https://doi.org/10.1140/epjd/e2007-00130-9	journal	March 2007
Mass Analyses of Cluster Ion Beams by Wien Filter Yano, Katsuki; Be, Suck Hee Japanese Journal of Applied Physics, Vol. 19, Issue 6 https://doi.org/10.1143/jjap.19.1019	journal	June 1980
Ionization Potential of O_2* Samson, James A. R.; Cairns, R. B. Journal of the Optical Society of America, Vol. 56, Issue 6 https://doi.org/10.1364/josa.56.000769	journal	January 1966
Provisional Report on Discussions on Group 3 of The Periodic Table Scerri, Eric Chemistry International, Vol. 43, Issue 1 https://doi.org/10.1515/ci-2021-0115	journal	January 2021
Ion-molecule reactions of Ru ⁺ and Os ⁺ with oxygen in a Penning trap Rieth, U.; Herlert, A.; Kratz, Jens Volker Radiochimica Acta, Vol. 90, Issue 6 https://doi.org/10.1524/ract.2002.90.6.337	journal	June 2002

Similar Records

Comparison of complementary reactions for the production of {sup 261,262}Bh

Journal Article · Fri Aug 15 00:00:00 EDT 2008 · Physical Review. C, Nuclear Physics · OSTI ID:21192118

CONSTITUTION OF THE ACTINIDE SERIES AND A DEDUCED LAW FOR THE ELECTRONIC CONFIGURATION OF THE SERIES' ELEMENTS

Journal Article · Tue Mar 31 23:00:00 EST 1959 · Bol. fac. ing. y agrimensura Montevideo · OSTI ID:4197910

Discovery of the new isotope ²⁵¹Lr and the α-decay fine structure in ²⁵³L

Journal Article · Wed Nov 30 23:00:00 EST 2022 · Physical Review. C · OSTI ID:1906168

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
FIONA mass seprator
actinide elements
ion-molecule reactions
transactinide elements

Assessment of the Second-Ionization Potential of Lawrencium: Investigating the End of the Actinide Series with a One-Atom-at-a-Time Gas-Phase Ion Chemistry Technique

Citation Formats

References (43)

Similar Records

Related Subjects