Single-Atom Chemistry

2016 ◽  
Author(s):  
Jens Volker Kratz
Keyword(s):  
Single Atom ◽  
Atom Chemistry

scholarly journals The influence of chemical parameters on the in-situ metal carbonyl complex formation studied with the fast on-line reaction apparatus (FORA)

2021 ◽  
Vol 109 (4) ◽  
pp. 243-260 ◽  
Author(s):  
Yves Wittwer ◽  
Robert Eichler ◽  
Dominik Herrmann ◽  
Andreas Türler
Keyword(s):  
Metal Carbonyl ◽  
Ambient Air ◽  
Single Atom ◽  
Carbonyl Complex ◽  
Carbonyl Complexes ◽  
On Line ◽  
Carrier Gases ◽  
And Performance ◽  
Atom Chemistry

Abstract A new setup named Fast On-line Reaction Apparatus (FORA) is presented which allows for the efficient investigation and optimization of metal carbonyl complex (MCC) formation reactions under various reaction conditions. The setup contains a 252Cf-source producing short-lived Mo, Tc, Ru and Rh isotopes at a rate of a few atoms per second by its 3% spontaneous fission decay branch. Those atoms are transformed within FORA in-situ into volatile metal carbonyl complexes (MCCs) by using CO-containing carrier gases. Here, the design, operation and performance of FORA is discussed, revealing it as a suitable setup for performing single-atom chemistry studies. The influence of various gas-additives, such as CO2, CH4, H2, Ar, O2, H2O and ambient air, on the formation and transport of MCCs was investigated. O2, H2O and air were found to harm the formation and transport of MCCs in FORA, with H2O being the most severe. An exception is Tc, for which about 130 ppmv of H2O caused an increased production and transport of volatile compounds. The other gas-additives were not influencing the formation and transport efficiency of MCCs. Using an older setup called Miss Piggy based on a similar working principle as FORA, it was additionally investigated if gas-additives are mostly affecting the formation or only the transport stability of MCCs. It was found that mostly formation is impacted, as MCCs appear to be much less sensitive to reacting with gas-additives in comparison to the bare Mo, Tc, Ru and Rh atoms.

scholarly journals The influence of gas purification and addition of macro amounts of metal-carbonyl complexes on the formation of single-atom metal-carbonyl-complexes

2021 ◽  
Vol 0 (0) ◽  
Author(s):  
Yves Wittwer ◽  
Robert Eichler ◽  
Ronald Zingg ◽  
Dominik Herrmann ◽  
Andreas Türler
Keyword(s):  
Metal Carbonyl ◽  
Fission Products ◽  
Single Atom ◽  
Gas Purification ◽  
Carbonyl Complexes ◽  
Carrier Gas ◽  
Metal Carbonyl Complexes ◽  
Process Gas ◽  
Atom Chemistry ◽  
Co Gas

Abstract Using the Fast On-line Reaction Apparatus (FORA), the influence of various gas-purification columns onto the formation of metal carbonyl complexes (MCCs) under single-atom chemistry conditions was investigated. MCCs were synthesized from single atoms of Mo, Tc, Ru and Rh being produced by the spontaneous fission of 252Cf and recoiling into a CO-gas containing carrier gas atmosphere. The in-situ synthesized MCCs were volatile enough to be transported by the carrier gas to a charcoal trap where they were adsorbed and their subsequent decay was registered by γ-spectrometry. It was found that the type and combination of purification columns used to clean the applied CO-gas strongly influences the obtained formation and transport yields for all MCCs. With the exception of Rh-carbonyl, intense gas-purification strategies resulted in reduced formation and transport yields for MCCs in comparison with less efficient or even completely missing purification setups. It was postulated that the observed reduction in yield might depend on the content of Fe(CO)5 and Ni(CO)4, as well as potentially other MCCs, in the CO-gas, being formed by the interaction between CO and the steel-surfaces of FORA as well as from impurities in the used charcoal traps. Subsequently, it was shown that macro amounts of Fe(CO)5, Ni(CO)4, Mo(CO)6 and Re2(CO)10 added to the used process gas indeed increase significantly the overall yields for MCCs produced by 252Cf fission products. Ni(CO)4 appeared the most potent to increase the yield. Therefore, it was used in more detailed investigations. Using isothermal chromatography, it was shown that Ni(CO)4 does not affect the speciation of carbonyl species produced by the 252Cf fission product 104Mo. For 107Tc, 110Ru and 111Rh a speciation change cannot be excluded. For 111Rh a speciation change cannot be excluded. An inter-carbonyl transfer mechanism is suggested boosting the formation of MCCs. The current discovery might allow for new opportunities in various research fields, which are currently restricted by the low overall yields for MCCs produced under single-atom chemistry conditions. Examples are the chemical investigation of transactinides or the generation of radioactive ion beams from refractory metals at accelerators.

The study of rhenium pentacarbonyl complexes using single-atom chemistry in the gas phase

2019 ◽  
Vol 21 (13) ◽  
pp. 7147-7154
Author(s):  
Yang Wang ◽  
Shiwei Cao ◽  
Jicai Zhang ◽  
Fangli Fan ◽  
Jie Yang ◽  
...  
Keyword(s):  
Gas Phase ◽  
Single Atom ◽  
Atom Level ◽  
Atom Chemistry

Two experiments prove Re pentacarbonyl could exist stably in the gas phase at the single-atom level.

Kinetic and Thermodynamic Aspects of Tracer-Scale and Single Atom Chemistry

1989 ◽  
Vol 46 (4) ◽  
Author(s):  
R. GUILLAUMONT ◽  
J. P. ADLOFF ◽  
A. PENELOUX
Keyword(s):  
Single Atom ◽  
Atom Chemistry

On the validity of single atom chemistry

1981 ◽  
Vol 43 (6) ◽  
pp. 1129-1133 ◽  
Author(s):  
R.J. Borg ◽  
G.J. Dienes
Keyword(s):  
Single Atom ◽  
Atom Chemistry

Single Atom Image Contrast in Fixed Beam Dark Field Electron Microscopy

1974 ◽  
Vol 32 ◽  
pp. 366-367
Author(s):  
Wah Chi
Keyword(s):  
Scattering Amplitude ◽  
Present Report ◽  
Dark Field ◽  
Image Contrast ◽  
Single Atom ◽  
Optical Theorem ◽  
Hartree Fock ◽  
Heavy Atoms ◽  
Beam Stop ◽  
Fixed Beam

Resolution and contrast are the important factors to determine the feasibility of imaging single heavy atoms on a thin substrate in an electron microscope. The present report compares the atom image characteristics in different modes of fixed beam dark field microscopy including the ideal beam stop (IBS), a wire beam stop (WBS), tilted illumination (Tl) and a displaced aperture (DA). Image contrast between one Hg and a column of linearly aligned carbon atoms (representing the substrate), are also discussed. The assumptions in the present calculations are perfectly coherent illumination, atom object is represented by spherically symmetric potential derived from Relativistic Hartree Fock Slater wave functions, phase grating approximation is used to evaluate the complex scattering amplitude, inelastic scattering is ignored, phase distortion is solely due to defocus and spherical abberation, and total elastic scattering cross section is evaluated by the Optical Theorem. The atom image intensities are presented in a Z-modulation display, and the details of calculation are described elsewhere.

Atomic Spectroscopy in the FIM

1986 ◽  
Vol 44 ◽  
pp. 758-761
Author(s):  
J. J. Hren ◽  
S. D. Walck
Keyword(s):  
Electron Microscope ◽  
Electric Fields ◽  
Atom Probe ◽  
Atomic Spectroscopy ◽  
Single Atom ◽  
Statistical Sampling ◽  
Commercial Instrument ◽  
Available Technology ◽  
High Electric Fields ◽  
Field Ion Microscope

The field ion microscope (FIM) has had the ability to routinely image the surface atoms of metals since Mueller perfected it in 1956. Since 1967, the TOF Atom Probe has had single atom sensitivity in conjunction with the FIM. “Why then hasn't the FIM enjoyed the success of the electron microscope?” The answer is closely related to the evolution of FIM/Atom Probe techniques and the available technology. This paper will review this evolution from Mueller's early discoveries, to the development of a viable commercial instrument. It will touch upon some important contributions of individuals and groups, but will not attempt to be all inclusive. Variations in instrumentation that define the class of problems for which the FIM/AP is uniquely suited and those for which it is not will be described. The influence of high electric fields inherent to the technique on the specimens studied will also be discussed. The specimen geometry as it relates to preparation, statistical sampling and compatibility with the TEM will be examined.

Field ion microscope investigations of atomic processes at surfaces

1989 ◽  
Vol 47 ◽  
pp. 228-229
Author(s):  
G. L. Kellogg ◽  
P. R. Schwoebel
Keyword(s):  
Single Crystal ◽  
Crystal Surface ◽  
Linear Chain ◽  
Atom Probe ◽  
Nucleation And Growth ◽  
Single Atom ◽  
Initial Structure ◽  
Atomic Processes ◽  
Single Crystal Surfaces ◽  
Field Ion Microscope

Although no longer unique in its ability to resolve individual single atoms on surfaces, the field ion microscope remains a powerful tool for the quantitative characterization of atomic processes on single-crystal surfaces. Investigations of single-atom surface diffusion, adatom-adatom interactions, surface reconstructions, cluster nucleation and growth, and a variety of surface chemical reactions have provided new insights to the atomic nature of surfaces. Moreover, the ability to determine the chemical identity of selected atoms seen in the field ion microscope image by atom-probe mass spectroscopy has increased or even changed our understanding of solid-state-reaction processes such as ordering, clustering, precipitation and segregation in alloys. This presentation focuses on the operational principles of the field-ion microscope and atom-probe mass spectrometer and some very recent applications of the field ion microscope to the nucleation and growth of metal clusters on metal surfaces.The structure assumed by clusters of atoms on a single-crystal surface yields fundamental information on the adatom-adatom interactions important in crystal growth. It was discovered in previous investigations with the field ion microscope that, contrary to intuition, the initial structure of clusters of Pt, Pd, Ir and Ni atoms on W(110) is a linear chain oriented in the <111> direction of the substrate.

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