Chemistry of actinide and lanthanide metal ions (M+) in laser ablation of dispersions of inorganic compounds in polyimide and polytetrafluoroethylene

Gibson, John K.

doi:10.1116/1.580616

Cited by 27 publications

(25 citation statements)

References 19 publications

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“…Non-organometallic divalent species identified were: An + =O (oxide), and HO−An + −OH (dihydroxide). These assignments have been discussed in detail elsewhere in the context of MPCA of lighter actinides [1][2][3][4]. As expected in a plume environment with a plethora of radical fragments, bare and oxo-ligated metal ions can combine to produce additional products, as evidenced by the continuum of peaks in Fig.…”

Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 83%

“…Among U, Np, Pu, Am and Cm, only with Am was the hydrogenated species, AmC 4 H + , dominant; for the other actinides, the binary carbide, AnC 4 + was distinctly the preferred product [1][2][3][4]. As seen in Figs.…”

Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 83%

“…2. Although the structures of the identified species cannot be positively assigned based on the MPCA mass spectra alone, it has been concluded [1][2][3][4] that the primary organoactinide ions are consistent with the formation of one or two direct An + −C covalent-type bonds of indeterminate degree of ionicity. The singly-bonded (monovalent actinide center) species are represented as An + −R 1 , and the doubly-bonded (divalent actinide) species as An + =R 2 or R 1 −An + −R 1 .…”

Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 96%

“…This metal/polymer co-ablation (MPCA) approach has been particularly effective for synthesizing new organometallic ions comprising members of the f -element lanthanide (Ln) and actinide (An) series. Studies have been carried out with several lanthanides and the actinides: thorium and uranium [1], neptunium and plutonium [2], americium [3], and curium [4]. A specific advantage of this approach for α-emitting, transuranium nuclides is that only a milligram or less of material is needed.…”

Section: Introductionmentioning

confidence: 98%

“…It has been demonstrated that a variety of gas-phase organometallic ions can be synthesized by laser ablation of a dispersion of a metal oxide in polyimide [1][2][3][4]. This metal/polymer co-ablation (MPCA) approach has been particularly effective for synthesizing new organometallic ions comprising members of the f -element lanthanide (Ln) and actinide (An) series.…”

Section: Introductionmentioning

confidence: 99%

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Berkelium and californium organometallic ions

Gibson¹,

Haire²

2001

Radiochimica Acta

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Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 83%

Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 83%

Section: Organoberkelium and Organocalifornium Ionsmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

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Berkelium and californium organometallic ions

Gibson¹,

Haire²

2001

Radiochimica Acta

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Reactions of actinide ions with ethylene oxide

Gibson

2001

J. Mass Spectrom.

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Naked and oxo-ligated actinide (An) monopositive ions were reacted with ethylene oxide, cyclo-C(2)H(4)O (EtO). Along with An = U, Np, Pu and Am, ions of two lanthanide (Ln) elements, Ln = Tb and Tm, were studied for comparison. Metal and metal oxide ions, M(+), MO(+) and MO(2)(+), were generated by laser ablation and immediately reacted with EtO. Unreacted and product ions were detected by time-of-flight mass spectrometry. It was apparent that the overall reaction cross-sections decreased in the order U(+) > or = Np(+) > Pu(+) > Am(+). A primary reaction channel for each studied metal was the formation of MO(+) from M(+), in accord with the expected exothermicity of oxygen abstraction from EtO. For U, Np and Pu, the dioxides were also major products, indicating OAn(+)--O dissociation energies of at least 350 kJ mol(-1), the energy required for O-atom abstraction from EtO. For Am, Tb and Tm, the dioxides were only very minor products, reflecting the stabilities of the trivalent states and resistance to oxidation to higher valence states; the structures/bonding in these MO(2)(+) are intriguing given that the formal pentavalent bonding state is effectively unattainable. It was demonstrated that EtO, unlike more thermochemically favorable but kinetically restricted O-donors, is effective at achieving facile oxidation of actinide metal ions to the monoxide, and to the dioxide if the second O-abstraction reaction is exothermic. Several intriguing minor products were also identified, most of which incorporate metal--oxygen bonding and are attributed to the oxophilicity of the f-block elements; the contrast to the behavior of first-row d-block transition elements is striking in this regard. Particularly noteworthy was the formation of MH(4)(+) (and MOH(4)(+)), evidently via abstraction of all four H atoms from a single C(2)H(4)O molecule; the structures/bonding in these novel 'hydride' species are indeterminate and warrant further attention.

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Laser Ionization Mass Spectrometry at 55: Quo Vadis?

Azov

Mueller

Makarov

2020

Mass Spectrometry Reviews

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Laser ionization mass spectrometry (LIMS) was one of the first practical methods developed for in situ analysis of the surfaces of solid samples. This review will encompass several aspects related to this analytical method. First, we will discuss the process of laser ionization, the influence of the laser type on its performance, and imaging capabilities of this method. In the second chapter, we will follow the historic development of LIMS instrumentation. After a brief overview of the first-generation instruments developed in 1960-1990 years, we will discuss in detail more recent designs, which appeared during the last 2-3 decades. In the last part of our review, we will cover the recent applications of LIMS for surface analysis. These applications include various types of analyses of solid inorganic, organic, and heterogeneous samples, often in combination with depth profiling and imaging capability.

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Chemistry of actinide and lanthanide metal ions (M+) in laser ablation of dispersions of inorganic compounds in polyimide and polytetrafluoroethylene

Cited by 27 publications

References 19 publications

Berkelium and californium organometallic ions

Berkelium and californium organometallic ions

Reactions of actinide ions with ethylene oxide

Laser Ionization Mass Spectrometry at 55: Quo Vadis?

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