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Hierarchical aggregation in a complex fluid; The Role of isomeric interconversion

Massey, D.*; Williams, C. D.*; Mu, J.*; Masters, A. J.*; 元川 竜平; 青柳 登; 上田 祐生; Antonio, M. R.*

Journal of Physical Chemistry B, 127(9), p.2052 - 2065, 2023/03

 被引用回数:0 パーセンタイル:0(Chemistry, Physical)

There is an ever-increasing body of evidence that metallic complexes, involving amphiphilic ligands, do not form normal solutions in organic solvents. Instead, they form complex fluids with intricate structures. For example, the metallic complexes may aggregate into clusters and these clusters themselves may aggregate into super-clusters. In order to gain a deeper insight into the mechanisms at play, we have used an improved force field to conduct extensive molecular dynamics simulations of a system composed of zirconium nitrate, water, nitric acid, tri-$$n$$-butyl phosphate and $$n$$-octane. The important new finding is that a dynamic equilibrium between the cis and trans isomers of the metal complex is likely to play a key role in the aggregation behavior. The isolated cis and trans isomers have similar energies but simulation indicates that the clusters consist predominantly of cis isomers. With increasing metal concentration, we hypothesize that more clustering occurs and the chemical equilibrium shifts towards the cis isomer. It is possible that such isomeric effects play a role in the liquid-liquid extraction of other species and the inclusion of such effects in flowsheet modelling may lead to a better description of the process.


On the adsorption and reactivity of element 114, flerovium

Yakushev, A.*; Lens, L.*; D$"u$llmann, Ch. E.*; Khuyagbaatar, J.*; J$"a$ger, E.*; Krier, J.*; Runke, J.*; Albers, H. M.*; 浅井 雅人; Block, M.*; et al.

Frontiers in Chemistry (Internet), 10, p.976635_1 - 976635_11, 2022/08

 被引用回数:8 パーセンタイル:88.78(Chemistry, Multidisciplinary)



Improved measurement of the $$0_2^+rightarrow0_1^+$$ $$E$$0 transition strength for $$^{72}$$Se using the SPICE spectrometer

Smallcombe, J.; Garnsworthy, A. B.*; Korten, W.*; Singh, P.*; Ali, F. A.*; Andreoiu, C.*; Ansari, S.*; Ball, G. C.*; Barton, C. J.*; Bhattacharjee, S. S.*; et al.

Physical Review C, 106(1), p.014312_1 - 014312_9, 2022/07

 被引用回数:2 パーセンタイル:47.37(Physics, Nuclear)

The selenium isotopes lie at the heart of a tumultuous region of the nuclear chart where shape coexistence effects grapple with neutron-proton pairing correlations, triaxiality, and the impending proton dripline. In this work a study of $$^{72}$$Se by internal conversion electron and $$gamma$$-ray spectroscopy was undertaken with the SPICE and TIGRESS arrays. New measurements of the branching ratio and lifetime of the $$0_2^+$$ state were performed yielding a determination of $$rho^2(E0; 0_2^+{rightarrow}0_1^+)=29(3)$$ milliunits. Two state mixing calculations were performed that highlighted the importance of interpretation of such $$E0$$ strength values in the context of shape-coexistence.


A Telescoping view of solute architectures in a complex fluid system

元川 竜平; 小林 徹; 遠藤 仁; Mu, J.*; Williams, C. D.*; Masters, A. J.*; Antonio, M. R.*; Heller, W. T.*; 長尾 道弘*

ACS Central Science, 5(1), p.85 - 96, 2019/01

 被引用回数:43 パーセンタイル:87.67(Chemistry, Multidisciplinary)

We present a hierarchical aggregate model of an organic phase containing a coordination species that acts as a fundamental building unit of higher-order structures formed in the organic phase. We aimed to elucidate the fundamental aspects of the microscopic structure and phase separation occurring in ionic separation and recovery systems during solvent extraction. The coordination species aggregate through a hydrogen-bonding network formed by interaction between the hydrophilic part of the coordination species with extracted water and acid molecules. This reduces the hydrophilic surface area, resulting in subsequent formation of small primal clusters of 2 to 3 nm in diameter. The primal clusters further aggregate due to van der Waals interaction to form large aggregates of $$<$$ 10 nm in diameter. The size of the primal cluster does not depend on the concentration of the coordination species, whereas the size of the large aggregate increases as the aggregation number of the primal clusters increases. We conclude that hybrid interaction is a key driving force in the formation and growth of the hierarchical aggregate and the induction of phase separation of the organic phase.


The Application of radiochronometry during the 4th collaborative materials exercise of the nuclear forensics international technical working group (ITWG)

Kristo, M. J.*; Williams, R.*; Gaffney, A. M.*; Kayzar-Boggs, T. M.*; Schorzman, K. C.*; Lagerkvist, P.*; Vesterlund, A.*; Rameb$"a$ck, H.*; Nelwamondo, A. N.*; Kotze, D.*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 315(2), p.425 - 434, 2018/02

 被引用回数:12 パーセンタイル:80.13(Chemistry, Analytical)



Round-robin $$^{230}$$Th-$$^{234}$$U age dating of bulk uranium for nuclear forensics

Gaffney, A.*; Hubert, A.*; Kinman, W. S.*; 間柄 正明; 大久保 綾子; Pointurier, F.*; Schorzman, K. C.*; Steiner, R. E.*; Williams, R. W.*

Journal of Radioanalytical and Nuclear Chemistry, 307(3), p.2055 - 2060, 2016/03

 被引用回数:21 パーセンタイル:89.32(Chemistry, Analytical)

核鑑識のためのウラン年代測定法について、4つの研究機関(ローレンスリバモア国立研究所, ロスアラモス国立研究所, フランス 原子力・代替エネルギー庁, 日本原子力研究開発機構)による共同試料分析を実施した。分析試料としては、ウラン同位体比標準物質であるNBL U050が選定され、同位体希釈質量分析法によって分析が行われた。各研究機関によって推定されたU050のウラン精製日は、1956年3月から1957年10月となり、この推定結果は、測定誤差に起因する精製日の誤差範囲で一致した。一方で、この推定結果は、文献で示されるU500の実際の精製日よりも古い精製日となっており、U050の製造時の精製が不十分であったことが示された。


Identification of deformed intruder states in semi-magic $$^{70}$$Ni

Chiara, C. J.*; Weisshaar, D.*; Janssens, R. V. F.*; 角田 佑介*; 大塚 孝治*; Harker, J. L.*; Walters, W. B.*; Recchia, F.*; Albers, M.*; Alcorta, M.*; et al.

Physical Review C, 91(4), p.044309_1 - 044309_10, 2015/04

 被引用回数:36 パーセンタイル:91.56(Physics, Nuclear)

アルゴンヌ国立研究所にて中性子過剰核$$^{70}$$Niを$$^{70}$$Znの多核子移行反応によって生成し、$$gamma$$線検出器GRETINAを用いて$$gamma$$線分光を行った。その結果、$$2^+_2$$, $$4^+_2$$準位を初めて観測した。これらの準位は小さな模型空間を採用した殻模型計算では再現されないため、陽子の$$f_{7/2}$$軌道からの励起を伴った大きな変形状態であると考えられる。本論文の理論グループが2014年に発表した大規模殻模型計算によって$$^{70}$$Niの励起状態を解析した結果、これらの状態は大きなプロレート変形を持つ状態とよく対応することがわかった。この結果は、中性子過剰ニッケル同位体における変形共存が$$^{68}$$Ni以外にも存在することを実証するとともに、中性子過剰核における大規模殻模型計算の予言能力を確かめるものである。


Li(Zn,Mn)As as a new generation ferromagnet based on a I-II-V semiconductor

Deng, Z.*; Jin, C. Q.*; Liu, Q. Q.*; Wang, X. C.*; Zhu, J. L.*; Feng, S. M.*; Chen, L. C.*; Yu, R. C.*; Arguello, C.*; 後神 達郎*; et al.

Nature Communications (Internet), 2, p.1425_1 - 1425_5, 2011/08

 被引用回数:150 パーセンタイル:93.59(Multidisciplinary Sciences)



Study of $$^{70,72}$$Se nuclear shapes with SPICE and TIGRESS

Smallcombe, J.; Garnsworthy, A. B.*; Korten, W.*; Singh, P.*; Ali, F. A.*; Andreoiu, C.*; Ansari, S.*; Ball, G. C.*; Barton, C. J.*; Bhattacharjee, S. S.*; et al.

no journal, , 

The phenomenon of shape coexistence is prevalent in the Z$$sim$$34 region, with isotopes of neutron-deficient even Ge, Se and Kr each exhibiting the characteristic low-lying coexisting 0+ bands which display quadrupole deformation different to that of the ground states. In the selenium isotopes, $$^{72-78}$$Se seem to show a prolate ground structure with shape coexisting oblate excitation, while in $$^{68}$$Se the oblate structure appears to have become the ground state. The exact nature of the low-lying structure $$^{70}$$Se and any shape coexistence remains uncertain. Combining the Spectrometer for Internal Conversion Electrons (SPICE) with the TIGRESS HPGe Array, a full electron and gamma-ray experimental study of $$^{70}$$Se, $$^{72}$$Se was undertaken at the TRIUMF ISAC-II facility to unveil the low-lying structure of these nuclei. Details of the device and experiment will be presented, alongside the experimental results and possible structural interpretations for both isotopes.

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