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Coordination number regulation of molybdenum single-atom nanozyme peroxidase-like specificity

Wang, Y.*; Jia, G.*; Cui, X.*; Zhao, X.*; Zhang, Q.*; Gu, L.*; Zheng, L.*; Li, L. H.*; Wu, Q.*; Singh, D. J.*; et al.

Chem, 7(2), p.436 - 449, 2021/02

 被引用回数:13 パーセンタイル:99.48(Chemistry, Multidisciplinary)

Nanozymes are promising alternatives to natural enzymes, but their use remains limited owing to poor specificity. Overcoming this is extremely challenging due to the intrinsic structural complexity of these systems. We report theoretical design and experimental realization of a series of heterogeneous molybdenum single-atom nanozymes (named Mo$$_{rm{SA}}$$-N$$_{x}$$-C), wherein we find that the peroxidase-like specificity is well regulated by the coordination numbers of single Mo sites. The resulting Mo$$_{rm{SA}}$$-N$$_{3}$$-C catalyst shows exclusive peroxidase-like behavior. It achieves this behavior via a homolytic pathway, whereas Mo$$_{rm{SA}}$$-N$$_{2}$$-C and Mo$$_{rm{SA}}$$-N$$_{4}$$-C catalysts have a different heterolytic pathway. The mechanism of this coordination-number-dependent enzymatic specificity is attributed to geometrical structure differences and orientation relationships of the frontier molecular orbitals.


HPRL; International cooperation to identify and monitor priority nuclear data needs for nuclear applications

Dupont, E.*; Bossant, M.*; Capote, R.*; Carlson, A. D.*; Danon, Y.*; Fleming, M.*; Ge, Z.*; 原田 秀郎; 岩本 修; 岩本 信之; et al.

EPJ Web of Conferences, 239, p.15005_1 - 15005_4, 2020/09

 被引用回数:0 パーセンタイル:0.19

The OECD-NEA High Priority Request List (HPRL) is a point of reference to guide and stimulate the improvement of nuclear data for nuclear energy and other nuclear applications. The HPRL is application-driven and the requests are submitted by nuclear data users or representatives of the user's communities. A panel of international experts reviews and monitors the requests in the framework of an Expert Group mandated by the NEA Nuclear Science Committee Working Party on International Nuclear Data Evaluation Cooperation (WPEC). After approval, individual requests are divided in two priority categories only, whereas a third category now includes groups of generic requests in a well-defined area (e.g., dosimetry, standard). The HPRL is hosted by the NEA in the form of a relational database publicly available on the web. This contribution provides an overview of HPRL entries, status and outlook. Examples of requests successfully completed will be given and new requests will be described with emphasis on updated nuclear data needs in the fields of nuclear energy, neutron standards, dosimetry, and medical applications.


Strong lattice anharmonicity exhibited by the high-energy optical phonons in thermoelectric material

Wu, P.*; Fan, F.-R.*; 萩原 雅人*; 古府 麻衣子; Peng, K.*; 石川 喜久*; Lee, S.*; 本田 孝志*; 米村 雅雄*; 池田 一貴*; et al.

New Journal of Physics (Internet), 22(8), p.083083_1 - 083083_9, 2020/08

 被引用回数:2 パーセンタイル:51.78(Physics, Multidisciplinary)



Shell structure of the neutron-rich isotopes $$^{69,71,73}$$Co

Lokotko, T.*; Leblond, S.*; Lee, J.*; Doornenbal, P.*; Obertelli, A.*; Poves, A.*; Nowacki, F.*; 緒方 一介*; 吉田 数貴; Authelet, G.*; et al.

Physical Review C, 101(3), p.034314_1 - 034314_7, 2020/03

 被引用回数:4 パーセンタイル:79.36(Physics, Nuclear)

中性子過剰核である$$^{69,71,73}$$Coに対する($$p,2p$$)ノックアウト反応が理化学研究所RIBFで測定された。$$gamma-gamma$$ coincidenceの方法で準位構造が決定され、測定された包括的断面積および排他的断面積から暫定的ではあるがスピン・パリティが決定された。殻模型計算との比較により、$$^{69,71,73}$$Coの低励起状態には球形核と変形核が共存することが示唆された。


Nuclear structure of $$^{76}$$Ni from the ($$p$$,$$2p$$) reaction

Elekes, Z.*; Kripk$'o$, $'A$*; Sohler, D.*; Sieja, K.*; 緒方 一介*; 吉田 数貴; Doornenbal, P.*; Obertelli, A.*; Authelet, G.*; 馬場 秀忠*; et al.

Physical Review C, 99(1), p.014312_1 - 014312_7, 2019/01

 被引用回数:7 パーセンタイル:80.58(Physics, Nuclear)

($$p$$,$$2p$$)反応による$$^{76}$$Niの核構造の探索実験を行った。Lenzi, Nowacki, Poves, Sieja相互作用を用いた殻模型計算では実験結果を説明しうる陽子空孔状態が得られており、理論的な断面積計算は実験値とよい一致を与えた。実験で得られたすべての状態を理論的に一意に決定することはできなかったが、過去の実験結果と同様にNi同位体でのZ = 28の大きなshell gapを示す結果が得られた。


Investigation of the electronic structure and lattice dynamics of the thermoelectric material Na-doped SnSe

Wu, P.*; Zhang, B.*; Peng, K. L.*; 萩原 雅之*; 石川 喜久*; 古府 麻衣子; Lee, S. H.*; 組頭 広志*; Hu, C. S.*; Qi, Z. M.*; et al.

Physical Review B, 98(9), p.094305_1 - 094305_7, 2018/09

 被引用回数:5 パーセンタイル:39.54(Materials Science, Multidisciplinary)

熱電材料であるNaドープしたSnSeについて、ARPES, 中性子回折, 中性子非弾性散乱でその電子構造と格子ダイナミクスを測定した結果を報告する。


Liquid-like thermal conduction in intercalated layered crystalline solids

Li, B.; Wang, H.*; 川北 至信; Zhang, Q.*; Feygenson, M.*; Yu, H. L.*; Wu, D.*; 尾原 幸治*; 菊地 龍弥*; 柴田 薫; et al.

Nature Materials, 17(3), p.226 - 230, 2018/03

 被引用回数:71 パーセンタイル:96.98(Chemistry, Physical)

As a generic property, all substances transfer heat through microscopic collisions of constituent particles. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here, we report liquid-like thermal conduction observed in the crystalline AgCrSe$$_{2}$$. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive, and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. These microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.


Atomically dispersed Pt on the surface of Ni particles; Synthesis and catalytic function in hydrogen generation from aqueous ammonia-borane

Li, Z.*; He, T.*; 松村 大樹; Miao, S.*; Wu, A.*; Liu, L.*; Wu, G.*; Chen, P.*

ACS Catalysis, 7(10), p.6762 - 6769, 2017/10

 被引用回数:102 パーセンタイル:96.66(Chemistry, Physical)

We report herein that the single-atom alloy (SAA) made of atomically dispersed Pt on the surface of Ni particles (Pt is surrounded by Ni atoms) exhibits improved catalytic activity on the hydrolytic dehydrogenation of ammonia-borane, a promising hydrogen storage method for onboard applications. Specifically, an addition of 160 ppm of Pt leads to ca. 3-fold activity improvement in comparison to that of pristine Ni/CNT catalyst. The turnover frequency based on the isolated Pt is 12000 mol$$_{rm{H}2}$$ mol$$_{rm{Pt}}$$$$^{-1}$$ min$$^{-1}$$, which is about 21 times the value of the best Pt-based catalyst ever reported. Our simulation results indicate that the high activity achieved stems from the synergistic effect between Pt and Ni, where the negatively charged Pt (Pt$$^{delta -}$$) and positively charged Ni (Ni$$^{delta +}$$) in the Pt-Ni alloy are prone to interact with H and OH of H$$_{2}$$O molecules, respectively, leading to an energetically favorable reaction pathway.


Shell evolution beyond $$Z$$=28 and $$N$$=50; Spectroscopy of $$^{81,82,83,84}$$Zn

Shand, C. M.*; Podoly$'a$k, Zs.*; G$'o$rska, M.*; Doornenbal, P.*; Obertelli, A.*; Nowacki, F.*; Otsuka, T.*; Sieja, K.*; Tostevin, J. A.*; Tsunoda, T.*; et al.

Physics Letters B, 773, p.492 - 497, 2017/10

 被引用回数:18 パーセンタイル:88.47(Astronomy & Astrophysics)

Low-lying states in neutron-rich $$^{81,82.83.84}$$Zn nuclei were measured for the first time via in-beam $$gamma$$-ray spectroscopy at RIKEN. These include the 4$$_1^+$$ to 2$$_1^+$$ in $$^{82}$$Zn and the 2$$_1^+$$ to 0$$_1^+$$ and 4$$_1^+$$ to 2$$_1^+$$ in $$^{84}$$Zn. The reduced E($$2^+$$) energies and increased E(4$$^+$$)/E(2$$^+$$) ratios at $$N$$=52,54 compared to $$^{80}$$Zn attest that the magicity is confined just on the neutron number $$N$$=50 only. The levels observed in $$^{84}$$Zn suggest the onset of deformation towards heavier Zn isotopes. The data were compared to state-of-the-art shell model calculations.


Observation of a $$gamma$$-decaying millisecond isomeric state in $$^{128}$$Cd$$_{80}$$

Jungclaus, A.*; Grawe, H.*; 西村 俊二*; Doornenbal, P.*; Lorusso, G.*; Simpson, G. S.*; S$"o$derstr$"o$m, P.-A.*; 炭竃 聡之*; Taprogge, J.*; Xu, Z. Y.*; et al.

Physics Letters B, 772, p.483 - 488, 2017/09

 被引用回数:7 パーセンタイル:61.99(Astronomy & Astrophysics)

A new high-spin isomer in the neutron-rich nucleus $$^{128}$$Cd was populated in the projectile fission of a $$^{238}$$U beam at the Radioactive Isotope Beam Factory at RIKEN. A half-life of T$$_{1/2}$$ = 6.3(8) ms was measured for the new state which was tentatively assigned a spin/parity of (15$$^-$$). The isomeric state decays via the emission of a 309-keV $$gamma$$ ray with $$E3$$ multipolarity. The experimental results are compared to shell model calculations performed using state-of-the-art realistic effective interactions and to the neighbouring nucleus $$^{129}$$Cd. The comparison with calculations shows that adjustments of the pairing and multipole parts of the effective interaction derived from the CD-Bonn nucleon-nucleon potential are required in order to describe the properties of nuclei in the region around $$^{132}$$Sn.


Type II shell evolution in $$A=70$$ isobars from the $$N geq 40$$ island of inversion

Morales, A. I.*; Benzoni, G.*; Watanabe, H.*; 角田 佑介*; Otsuka, T.*; 西村 俊二*; Browne, F.*; Daido, R.*; Doornenbal, P.*; Fang, Y.*; et al.

Physics Letters B, 765, p.328 - 333, 2017/02

 被引用回数:28 パーセンタイル:94.69(Astronomy & Astrophysics)

The level schemes of neutron-rich isotopes $$^{70}$$Co and $$^{70}$$Ni were populated in the $$beta$$ decay of $$^{70}$$Fe and studied using $$beta$$-delayed $$gamma$$-ray spectroscopy of the $$beta$$ decay, at the RIBF in RIKEN, Japan. The experimental results were compared to state-of-the-art shell-model calculations, and indicate a dominance of prolate deformation in the low-lying states, coexisting with spherical states. The $$beta$$ decay of the $$A=70$$ isobars is shown to progress in accordance to a new type of shell evolution, the so-called Type II, which involves many particle-hole excitations across energy gaps.


$$beta$$ decay of semi-magic $$^{130}$$Cd; Revision and extension of the level scheme of $$^{130}$$In

Jungclaus, A.*; Grawe, H.*; 西村 俊二*; Doornenbal, P.*; Lorusso, G.*; Simpson, G. S.*; S$"o$derstr$"o$m, P. A.*; 炭竃 聡之*; Taprogge, J.*; Xu, Z. Y.*; et al.

Physical Review C, 94(2), p.024303_1 - 024303_8, 2016/08

 被引用回数:15 パーセンタイル:79.72(Physics, Nuclear)

The $$beta$$ decay of the semi-magic nucleus $$^{130}$$Cd has been studied at the RIBF facility at the RIKEN Nishina Center. The high statistics of the present experiment allowed for a revision of the established level scheme of $$^{130}$$In and the observation of additional $$beta$$ feeding to high lying core-excited states in $$^{130}$$In. The experimental results are compared to shell-model calculations employing a model space consisting of the full major $$N=50-82$$ neutron and $$Z=28-50$$ proton shells, and good agreement is found.


First observation of $$gamma$$ rays emitted from excited states south-east of $$^{132}$$Sn; The $$pi$$ g$$_{9/2}^{-1}$$ $$ otimes$$ $$nu f_{7/2}$$ multiplet of $$^{132}$$In$$_{83}$$

Jungclaus, A.*; Gargano, A.*; Grawe, H.*; Taprogge, J.*; 西村 俊二*; Doornenbal, P.*; Lorusso, G.*; Shimizu, Y.*; Simpson, G. S.*; S$"o$derstr$"o$m, P.-A.*; et al.

Physical Review C, 93(4), p.041301_1 - 041301_6, 2016/04

 被引用回数:15 パーセンタイル:79.72(Physics, Nuclear)

For the first time, the decay of excited states in a nucleus situated "south-east" of $$^{132}$$Sn have been observed, in a region where experimental information is limited to ground-state properties. Six $$gamma$$ rays from $$^{133}$$Cd, produced in the fragmentation of a $$^{238}$$U beam at RIBF at RIKEN. The $$gamma$$ rays were studied using the EURICA array of Ge detectors. The new experimental information is compared to results from realistic shell-model calculations, which are the first in this region far from stability. Comparison with calculations suggests that at least four out of six new transitions can be attributed to the particle-hole configuration of one neutron in the $$f_{7/2}$$ and one proton hole in the $$g_{9/2}$$ orbits, respectively. This work constitutes an important first step towards the exploration of nuclear structure in this unknown region of the nuclear chart.


Low-lying excitations in $$^{72}$$Ni

Morales, A. I.*; Benzoni, G.*; Watanabe, H.*; 西村 俊二*; Browne, F.*; Daido, R.*; Doornenbal, P.*; Fang, Y.*; Lorusso, G.*; Patel, Z.*; et al.

Physical Review C, 93(3), p.034328_1 - 034328_14, 2016/03

 被引用回数:19 パーセンタイル:85.24(Physics, Nuclear)

Low-lying excited states in $$^{72}$$Ni have been investigated at RIKEN by studying the $$beta$$ decay of $$^{72}$$Co to $$^{72}$$Ni. $$^{72}$$Co was separated with BigRIPS, implanted into the WaS3ABi Silicon array, and the $$gamma$$ ray measured using the EURICA $$gamma$$ spectrometer. From the analysis, 60 new $$gamma$$-ray transitions and 21 new levels in $$^{72}$$Ni were observed. The new experimental information is compared to shell-model calculations which include neutron excitation across the $$fpg$$ shell. The calculations reproduce rather well the observed states, implying that a clear understanding of these low-lying excitations has been achieved.


Decay properties of $$^{68,69,70}$$Mn; Probing collectivity up to N=44 in Fe isotopic chain

Benzoni, G.*; Morales, A. I.*; Watanabe, H.*; 西村 俊二*; Coraggio, L.*; Itaco, N.*; Gargano, A.*; Browne, F.*; Daido, R.*; Doornenbal, P.*; et al.

Physics Letters B, 751, p.107 - 112, 2015/12

 被引用回数:18 パーセンタイル:81.47(Astronomy & Astrophysics)

The $$beta$$ decays of $$^{68,69,70}$$Mn have been measured at the RIBF facility at RIKEN using the EURICA $$gamma$$ spectrometer combined with an active stopper consisting of a stack of Si detectors. Half-lives and $$beta$$-delayed neutron emission probabilities have been extracted for these decays, together with first experimental information on excited states populated in $$^{69,70}$$Fe. The data indicate a continuously increasing deformation for Fe isotopes up to A=70, and interpreted to be due to the interplay between quadrupole correlation of specific neutron orbitals and the monopole component of the proton-neutron interaction.


$$beta$$ decay of $$^{129}$$Cd and excited states in $$^{129}$$In

Taprogge, J.*; Jungclaus, A.*; Grawe, H.*; 西村 俊二*; Doornenbal, P.*; Lorusso, G.*; Simpson, G. S.*; S$"o$derstr$"o$m, P.-A.*; 炭竃 聡之*; Xu, Z. Y.*; et al.

Physical Review C, 91(5), p.054324_1 - 054324_11, 2015/05

 被引用回数:24 パーセンタイル:87.68(Physics, Nuclear)

The $$beta$$ decay of $$^{129}$$Cd, produced in relativistic fission of a $$^{238}$$U beam, was studied at the RIKEN Nishina Center. From the $$gamma$$-ray analysis, 31 excited states and 69 $$gamma$$ ray transitions were established in the level scheme of $$^{129}$$In, and compared with state-of-the-art shell-model calculations. It was found that the $$beta$$ decay of $$^{129}$$Cd is dominated by Gamow teller transitions, but a non-negligible contribution to the $$beta$$ decay is also made by first-forbidden transitions. To estimate the contribution of first-forbidden transitions is important for calculations of the $$beta$$-decay half-lives of nuclei in this region.


$$beta$$-decay half-lives of 110 neutron-rich nuclei across the $$N$$=82 shell gap; Implications for the mechanism and universality of the astrophysical $$r$$ process

Lorusso, G.*; 西村 俊二*; Xu, Z. Y.*; Jungclaus, A.*; Shimizu, Y.*; Simpson, G. S.*; S$"o$derstr$"o$m, P.-A.*; Watanabe, H.*; Browne, F.*; Doornenbal, P.*; et al.

Physical Review Letters, 114(19), p.192501_1 - 192501_7, 2015/05

 被引用回数:118 パーセンタイル:97.94(Physics, Multidisciplinary)

The $$beta$$-decay half-lives of 110 neutron-rich isotopes of the elements from Rb to Sn were measured at the RIBF Facility at RIKEN, Japan. The new data demonstrate the persistence of shell structure far from stability and have direct implications for the $$r$$-process calculations. In particular, the new half-lives have a global impact on the calculated $$r$$-process elemental abundances, and alleviate the underproduction of isotopes just above and below the A=130 peak, which in the past required the introduction of shell structure modifications. Reaction-network calculations based on the new data reinforce the notion that the r-process abundance pattern may result from the freeze-out of a (n,$$gamma$$)$$_leftarrow^{rightarrow}$$($$gamma$$,n) equilibrium.


Overview of plasma-material interaction experiments on EAST employing MAPES

Ding, F.*; Luo, G.-N.*; Pitts, R.*; Litnovsky, A.*; Gong, X.*; Ding, R.*; Mao, H.*; Zhou, H.*; Wampler, W. R.*; Stangeby, P. C.*; et al.

Journal of Nuclear Materials, 455(1-3), p.710 - 716, 2014/12

 被引用回数:23 パーセンタイル:91.23(Materials Science, Multidisciplinary)

A movable material probe system (Material and Plasma Evaluation System: MAPES) with an independent pumping system and a sample exchange chamber has been developed and installed on a horizontal port of the EAST tokamak for studies of plasma material interaction (PMI). In the 2012 experimental campaign, deposition and erosion were studied for three samples: mock-up of the outer first wall panels (FWPs) in ITER, castellated tungsten, and molybdenum mirrors. The FWPs with carbon deposition layer were exposed to helium plasmas. The maximum erosion rate of the carbon was valuated to be 8 nm/s. The castellated tungsten with rectangular cells and roof-like shaped cells was exposed to deuterium plasmas to compare amount of deposits on the gap surface. The amount of carbon and boron impurities on the gap surface of the roof-like shaped cells were reduced to less than 30% compared with that of the rectangular cells. The molybdenum mirrors of which protective ducts are installed in front were exposed to deuterium plasmas in order to investigate effects of length of the ducts. It was found that the reflectivity of the mirrors with 60 mm-long protective ducts is kept the initial reflectivity.


Identification of a millisecond isomeric state in $$^{129}$$Cd$$_{81}$$ via the detection of internal conversion and Compton electrons

Taprogge, J.*; Jungclaus, A.*; Grawe, H.*; 西村 俊二*; Xu, Z. Y.*; Doornenbal, P.*; Lorusso, G.*; N$'a$cher, E.*; Simpson, G. S.*; S$"o$derstr$"o$m, P.-A.*; et al.

Physics Letters B, 738, p.223 - 227, 2014/11

 被引用回数:20 パーセンタイル:81.46(Astronomy & Astrophysics)

The decay of an isomeric state in the neutron-rich nucleus $$^{129}$$Cd was observed via the detection of internal conversion and Compton electrons. This measurement provided the first experimental information on excited states in this nucleus. The isomer was populated in the projectile fission of a $$^{238}$$U beam at the RIBF facility at RIKEN. From the measured yields of $$gamma$$ rays and internal conversion electrons, E3 multipolarity was tentatively assigned to the isomeric transition. A half-life of 3.6(2) ms was determined for this new state which, by comparison with shell-model calculations, was tentatively assigned a spin of (21/2$$^+$$).


Yrast 6$$^+$$ seniority isomers of $$^{136,138}$$Sn

Simpson, G. S.*; Gey, G.*; Jungclaus, A.*; Taprogge, J.*; 西村 俊二*; Sieja, K.*; Doornenbal, P.*; Lorusso, G.*; S$"o$derstr$"o$m, P.-A.*; 炭竃 聡之*; et al.

Physical Review Letters, 113(13), p.132502_1 - 132502_6, 2014/09

 被引用回数:56 パーセンタイル:92.53(Physics, Multidisciplinary)

Delayed $$gamma$$-ray cascades, originating from the decay of 6$$^+$$ isomeric states, in the very neutron-rich, semimagic isotopes $$^{136,138}$$Sn were observed following the projectile fission of a $$^{238}$$U beam at RIBF, RIKEN. The wave functions of these isomeric states are proposed to be predominantly a fully aligned pair of f$$_{7/2}$$ neutrons. Shell-model calculations, performed using a realistic effective interaction, reproduce well the energies of the excited states of these nuclei and the measured transition rates, with the exception of the $$B(E$$2;6$$^+ rightarrow 4^+$$) rate of $$^{136}$$Sn, which deviates from a simple seniority scheme. Empirically reducing the $$nu f$$$$_{7/2}^{2}$$ orbit matrix elements produces a 4+1 state with almost equal seniority 2 and 4 components, correctly reproducing the experimental $$B(E$$2;6$$^+ rightarrow 4^+$$) rate of $$^{136}$$Sn. These data provide a key benchmark for shell-model interactions far from stability.

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