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論文

Reevaluation of structures in $$^{70}$$Se from combined conversion-electron and $$gamma$$-ray spectroscopy

Smallcombe, J.; Garnsworthy, A. B.*; Korten, W.*; Singh, P.*; Muir, D.*; Pr$'o$chniak, L.*; Ali, F. A.*; Andreoiu, C.*; Ansari, S.*; Ball, G. C.*; et al.

Physical Review C, 110(2), p.024318_1 - 024318_16, 2024/08

 被引用回数:0 パーセンタイル:0.00(Physics, Nuclear)

In the selenium isotopes various shape phenomena are present, in particular the emergence of a dominant oblate deformation in the most neutron-deficient isotopes has been observed. The scenario of shape coexisting oblate and prolate bands has been proposed across the isotopic chain, with the crossing point of such bands being located near $$^{70}$$Se, where no coexistence has yet been identified. To determine the presence or absence of any low-lying $$0^+$$ state in $$^{70}$$Se, confirm the level structure, and interpret the nuclear deformation with theoretical models. A combined internal conversion electron and $$gamma$$-ray spectroscopy study was undertaken with the SPICE and TIGRESS spectrometers at the TRIUMF-ISAC-II facility. Nuclear models were provided by the Generalised Triaxial Rotor Model (GTRM) and the collective Generalised Bohr Hamiltonian (GBH). Despite a comprehensive search, no evidence was found for the existence of a $$0^+$$ state below 2 MeV in $$^{70}$$Se. Significant discrepancies to the previously established positive parity level scheme were found. GBH calculations using UNEDF1 mass parameters were found to reproduce the revised low-lying level structure well. $$^{70}$$Se does not have a well defined axial shape. The 2$$_2^{+}$$ state at 1601 keV resembles a quasi-$$gamma$$ excitation rather than a member of a shape coexisting band; the presence of such a band is all but ruled out.

論文

System of radiological protection; Towards a consistent framework on earth and in space

R$"u$hm, W.*; 伴 信彦*; Chen, J.*; Li, C.*; Dobynde, M.*; Durante, M.*; El-Jaby, S.*; 込山 立人*; 小笹 晃太郎*; 佐藤 達彦; et al.

Journal of Medical Physics - Zeitschrift f$"u$r medizinische Physik -, 34(1), p.4 - 13, 2024/02

 被引用回数:0 パーセンタイル:0.00(Radiology, Nuclear Medicine & Medical Imaging)

国際放射線防護委員会(ICRP)は、過去90年間に渡って世界各国や国際的な放射線防護の枠組み作りに貢献してきた。2019年、ICRPは宇宙飛行士の放射線防護に関わる様々な問題に対応したタスクグループ(TG115)を立ち上げ、地上の放射線防護体系と宇宙の放射線防護体系との共通の枠組み作りに取り組んでいる。本論文では、現時点でICRPが定めている宇宙放射線防護体系についてとりまとめて報告する。

論文

Microscopic origin of the spin-reorientation transition in the kagome topological magnet TbMn$$_{6}$$Sn$$_{6}$$

Huang, Z.*; Wang, W.*; Ye, H.*; Bao, S.*; Shangguan, Y.*; Liao, J.*; Cao, S.*; 梶本 亮一; 池内 和彦*; Deng, G.*; et al.

Physical Review B, 109(1), p.014434_1 - 014434_9, 2024/01

 被引用回数:0 パーセンタイル:0.00(Materials Science, Multidisciplinary)

TbMn$$_{6}$$Sn$$_{6}$$ is a correlated topological magnet with a Mn-based kagome lattice, in which a Chern gap opens at the Dirac point at low temperatures. The magnetic moment direction of the ferrimagnetic order changes from in the kagome plane to the out-of-plane upon cooling, which is essential for generating the Chern gap, but the underlying mechanism for the spin reorientation remains elusive. Here, we investigate the spin-reorientation transition in TbMn$$_{6}$$Sn$$_{6}$$ using neutron scattering. We provide direct evidence for the spin-reorientation transition and unveil the coexistence of two Tb modes at 200 K. To account for these results, we put forward a model based on SU(N) spin-wave theory, in which there is a temperature evolution of the ground state Tb $$4f$$ orbitals, driven by the crystalline electric field, single-ion anisotropy, and exchange interactions between Tb and Mn ions. Our findings shed light on the complex magnetism of TbMn$$_{6}$$Sn$$_{6}$$, despite its relatively simple ground state magnetic structure, and provide insights into the mechanisms for tuning magnetic topological materials.

論文

Chiral Dirac fermion in a collinear antiferromagnet

Zhang, A.*; Deng, K.*; Sheng, J.*; Liu, P.*; Kumar, S.*; 島田 賢也*; Jiang, Z.*; Liu, Z.*; Shen, D.*; Li, J.*; et al.

Chinese Physics Letters, 40(12), p.126101_1 - 126101_8, 2023/12

 被引用回数:6 パーセンタイル:84.64(Physics, Multidisciplinary)

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, itis predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral "Dirac-like" fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Here, by combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions.

論文

ICRU Report 98, Stochastic nature of radiation interactions; Microdosimetry

Braby, L. A.*; Conte, V.*; Dingfelder, M.*; Goodhead, D. T.*; Pinsky, L. S.*; Rosenfeld, A. B.*; 佐藤 達彦; Waker, A. J.*; Guatelli, S.*; Magrin, G.*; et al.

Journal of ICRU, 23(1), p.1 - 168, 2023/12

マイクロドジメトリ分野で使われる物理量などの定義はICRUが1983年に発刊したレポートにまとめられているが、いくつか曖昧な点がある。本稿では、それら物理量の定義を明確にするとともに、マイクロドジメトリ分野における理論・実践・応用を包括的に解説する。

論文

Validation of the $$^{10}$$Be ground-state molecular structure using $$^{10}$$Be($$p,palpha$$)$$^{6}$$He triple differential reaction cross-section measurements

Li, P. J.*; Beaumel, D.*; Lee, J.*; Assi$'e$, M.*; Chen, S.*; Franchoo, S.*; Gibelin, J.*; Hammache, F.*; Harada, T.*; 延与 佳子*; et al.

Physical Review Letters, 131(21), p.212501_1 - 212501_7, 2023/11

 被引用回数:6 パーセンタイル:75.19(Physics, Multidisciplinary)

$$^{10}$$Beのクラスター構造を($$p,palpha$$)反応を用いて調査した。三重微分断面積が実験的に測定され、Tohsaki-Horiuchi-Schuck-R$"o$pke波動関数の方法や反対称化分子動力学を用いた歪曲波インパルス近似計算と比較した。実験データと理論計算の顕著な一致が確認され、$$^{10}$$Beの比較的コンパクトな分子状態を確認した。

論文

First observation of $$^{28}$$O

近藤 洋介*; Achouri, N. L.*; Al Falou, H.*; Atar, L.*; Aumann, T.*; 馬場 秀忠*; Boretzky, K.*; Caesar, C.*; Calvet, D.*; Chae, H.*; et al.

Nature, 620(7976), p.965 - 970, 2023/08

 被引用回数:18 パーセンタイル:95.53(Multidisciplinary Sciences)

非常に中性子が過剰な原子核$$^{28}$$Oは、陽子、中性子ともに魔法数であることから古くからその性質に興味が持たれていたが、酸素の最後の束縛核$$^{24}$$Oよりも中性子が4個も多いため、これまで観測されてこなかった。この論文では、理化学研究所RIBFにて$$^{29}$$Fからの1陽子ノックアウト反応によって$$^{28}$$Oを生成し、そこから放出される中性子を測定することによって初めてその観測に成功した。核構造の観点からは、$$^{28}$$Oでは二重閉殻が保たれているか興味が持たれていたが、実験で得られた分光学的因子が殻模型計算で予言されて程度の大きいことから、閉殻構造をもたない可能性が高いことがわかった。

論文

Level structures of $$^{56,58}$$Ca cast doubt on a doubly magic $$^{60}$$Ca

Chen, S.*; Browne, F.*; Doornenbal, P.*; Lee, J.*; Obertelli, A.*; 角田 佑介*; 大塚 孝治*; 茶園 亮樹*; Hagen, G.*; Holt, J. D.*; et al.

Physics Letters B, 843, p.138025_1 - 138025_7, 2023/08

 被引用回数:6 パーセンタイル:87.68(Astronomy & Astrophysics)

$$^{57,59}$$Scからの1陽子ノックアウト反応を用いて、$$^{56}$$Caと$$^{58}$$Caのガンマ崩壊を観測した。$$^{56}$$Caでは1456(12)keVの$$gamma$$線遷移が、$$^{58}$$Caでは1115(34)keVの遷移が観測された。どちらの遷移も暫定的に$$2^{+}_{1} rightarrow 0^{+}_{gs}$$と割り当てられた。有効核子間相互作用をわずかに修正した広い模型空間での殻模型計算では、$$2^{+}_{1}$$準位エネルギー、2中性子分離エネルギー、反応断面積が実験とよく一致し、N=34閉殻の上に新しい殻が形成されていることを裏付けた。その構成要素である$$0_{f5/2}$$$$0_{g9/2}$$軌道はほぼ縮退しており、これは$$^{60}$$Caが二重魔法核である可能性を排除し、Ca同位体のドリップラインを$$^{70}$$Caあるいはそれ以上にまで広げる可能性がある。

論文

Si-addition contributes to overcoming the strength-ductility trade-off in high-entropy alloys

Wei, D.*; Gong, W.; 都留 智仁; Lobzenko, I.; Li, X.*; Harjo, S.; 川崎 卓郎; Do, H.-S.*; Bae, J. W.*; Wagner, C.*; et al.

International Journal of Plasticity, 159, p.103443_1 - 103443_18, 2022/12

 被引用回数:67 パーセンタイル:99.58(Engineering, Mechanical)

Face-centered cubic single-phase high-entropy alloys (HEAs) containing multi-principal transition metals have attracted significant attention, exhibiting an unprecedented combination of strength and ductility owing to their low stacking fault energy (SFE) and large misfit parameter that creates severe local lattice distortion. Increasing both strength and ductility further is challenging. In the present study, we demonstrate via meticulous experiments that the CoCrFeNi HEA with the addition of the substitutional metalloid Si can retain a single-phase FCC structure while its yield strength (up to 65%), ultimate strength (up to 34%), and ductility (up to 15%) are simultaneously increased, owing to a synthetical effect of the enhanced solid solution strengthening and a reduced SFE. The dislocation behaviors and plastic deformation mechanisms were tuned by the addition of Si, which improves the strain hardening and tensile ductility. The present study provides new strategies for enhancing HEA performance by targeted metalloid additions.

論文

Rediscovery of Hall-Petch strengthening in bulk ultrafine grained pure Mg at cryogenic temperature; A Combined ${it in situ}$ neutron diffraction and electron microscopy study

Zheng, R.*; Gong, W.; Du, J.-P.*; Gao, S.*; Liu, M.*; Li, G.*; 川崎 卓郎; Harjo, S.; Ma, C.*; 尾方 成信*; et al.

Acta Materialia, 238, p.118243_1 - 118243_15, 2022/10

 被引用回数:31 パーセンタイル:96.96(Materials Science, Multidisciplinary)

Grain refinement can lead to the strengthening of metallic materials according to the Hall-Petch relationship. However, our recent results suggested that grain boundary sliding is the dominant deformation mode in bulk ultrafine grained (UFG) pure Mg at room temperature, leading to softening. Here, for the first time, we report that the Hall-Petch strengthening can be regained in bulk UFG pure Mg at cryogenic temperature. At 77K, the UFG pure Mg with a mean grain size of 0.6 $$mu$$m exhibited ultrahigh tensile yield strength and ultimate tensile strength of 309 MPa and 380 MPa, respectively. Combined ${it in situ}$ neutron diffraction and electron microscopy investigation indicated that residual dislocation structures and deformation twins hardly formed in the UFG specimen during tensile test at 298K. In contrast, fast accumulation of lattice defects and remarkable reorientation were evident at 77K, suggesting that the grain-boundary-mediated process was suppressed and the plastic deformation was dominated by dislocation slip and deformation twinning. In addition, all the pure Mg specimens exhibited pronounced strain hardening at 77 K, which was mainly attributed to the suppressed grain boundary sliding and dynamic recovery. The mean dislocation density and relative fractions of dislocations with various Burgers vectors of the UFG specimen deformed at 77K were determined quantitatively from neutron diffraction data.

論文

First observation of the de Haas-van Alphen effect and Fermi surfaces in the unconventional superconductor UTe$$_2$$

青木 大*; 酒井 宏典; Opletal, P.; 常盤 欣文; 石塚 淳*; 柳瀬 陽一*; 播磨 尚朝*; 仲村 愛*; Li, D.*; 本間 佳哉*; et al.

Journal of the Physical Society of Japan, 91(8), p.083704_1 - 083704_5, 2022/08

 被引用回数:44 パーセンタイル:97.97(Physics, Multidisciplinary)

de Haas-van Alphen oscillation was successfully observed in an unconventional superconductor UTe$$_2$$ using high-quality single crystals. From this observation, Fermi surfaces of this compound were determined to be cylinders elongated along the c-direction, in consistent with theoretical expectation. However, the extremely large cyclotron effective masses ranging 32 to 57 m$$_0$$, in consistent with the electronic specific heat, far exceed calculated values.

論文

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:5 パーセンタイル:70.77(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.

論文

First observation of a shape isomer and a low-lying strongly-coupled prolate band in neutron-deficient semi-magic $$^{187}$$Pb

Zhang, W. Q.*; Andreyev, A. N.; Liu, Z.*; Seweryniak, D.*; Huang, H.*; Li, Z. H.*; Li, J. G.*; Guo, C. Y.*; 他34名*

Physics Letters B, 829, p.137129_1 - 137129_7, 2022/06

 被引用回数:6 パーセンタイル:76.40(Astronomy & Astrophysics)

Prompt and delayed $$gamma$$-ray spectroscopy of the neutron-deficient, semi-magic isotope $$^{187}$$Pb has been performed at the Argonne Gas-Filled Analyzer. A new 5.15(15)-$$mu$$s isomeric state at only 308 keV above the spherical 3/2$$^{-}$$ ground state is identified and classified as a shape isomer. A strongly-coupled band is observed on top of the isomer, which is nearly identical to the one built on the prolate 7/2$$^{-}$$[514] Nilsson state in the isotone $$^{185}$$Hg. Based on this similarity and on the result of the potential-energy surface calculations, the new isomer in $$^{187}$$Pb is proposed to originate from the same configuration. The retarded character of the 308-keV transition can be well explained by the significant difference between the prolate parent and spherical daughter configurations, leading to the shape isomerism. The combined results of the present work and the previous $$alpha$$-decay and laser spectroscopy studies present evidence for triple shape coexistence at low energy in the negative-parity configurations of $$^{187}$$Pb, which is well reproduced by the potential-energy surface calculations.

論文

Solving the puzzles of the decay of the heaviest known proton-emitting nucleus $$^{185}$$Bi

Doherty, D. T.*; Andreyev, A. N.; Seweryniak, D.*; Woods, P. J.*; Carpenter, M. P.*; Auranen, K.*; Ayangeakaa, A. D.*; Back, B. B.*; Bottoni, S.*; Canete, L.*; et al.

Physical Review Letters, 127(20), p.202501_1 - 202501_6, 2021/11

 被引用回数:10 パーセンタイル:66.31(Physics, Multidisciplinary)

$$^{185}$$Bi is the heaviest known proton emitting isotope. Its decay had been observed, but the assumed ground-state lifetime ($$sim$$$$60~mu$$s) was incorrect, leading to unexplained hindrance. With two new experiments at Argonne National Laboratory, two states were clearly identified. One is the proton-emitting ground-state (spin 1/2$$^+$$, half-life: 2.8$$^{+2.3}_{-1.0}$$ $$mu$$s), the second is a 58(2) $$mu$$s $$gamma$$-decaying isomer. The new data show the inversion of the ground and isomeric states compared to neighboring Bi isotopes. This is the only known example of a ground-state proton decay to a daughter nucleus ($$^{184}$$Pb) with a major shell closure.

論文

The $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe cross section from the surrogate ratio method and its effect on the $$^{60}$$Fe nucleosynthesis

Yan, S. Q.*; Li, X. Y.*; 西尾 勝久; Lugaro, M.*; Li, Z. H.*; 牧井 宏之; Pignatari, M.*; Wang, Y. B.*; Orlandi, R.; 廣瀬 健太郎; et al.

Astrophysical Journal, 919(2), p.84_1 - 84_7, 2021/10

 被引用回数:2 パーセンタイル:13.66(Astronomy & Astrophysics)

The long-lived $$^{60}$$Fe (with a half-life of 2.62 Myr) is a crucial diagnostic of active nucleosynthesis in the Milky Way galaxy and in supernovae near the solar system. The neutron-capture reaction $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe on $$^{59}$$Fe (half-life=44.5 days) is the key reaction for the production of $$^{60}$$Fe in massive stars. This reaction cross section has been previously constrained by the Coulomb dissociation experiment, which offered partial constraint on the E1 $$gamma$$-ray strength function but a negligible constraint on the M1 and E2 components. In this work, for the first time, we use the surrogate ratio method to experimentally determine the $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe cross sections in which all the components are included. We derived a Maxwellian-averaged cross section of 27.5$$pm$$3.5 mb at $$kT$$ = 30 keV and 13.4$$pm$$1.7 mb at $$kT$$ = 90 keV, roughly 10%-20% higher than previous estimates. We analyzed the impact of our new reaction rates in nucleosynthesis models of massive stars and found that uncertainties in the production of $$^{60}$$Fe from the $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe rate are at most 25$$%$$. We conclude that stellar physics uncertainties now play a major role in the accurate evaluation of the stellar production of $$^{60}$$Fe.

論文

Phase transition and chemical reactivity of 1H-tetrazole under high pressure up to 100 GPa

Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; 服部 高典; Wang, Y.*; Dong, X.*; et al.

Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09

 被引用回数:4 パーセンタイル:28.78(Chemistry, Physical)

窒素に富む分子の圧力有機相転移や重合は、環境にやさしい高エネルギー密度材料の開発にとって非常に重要であるため、広く注目されている。本論文では、その場ラマン,IR,X線回折,中性子回折、および理論計算をもちい、100GPaまでの1H-テトラゾールの相転移挙動と化学反応の研究を紹介する。2.6GPa以上での相転移が確認され、その高圧構造は、以前に報告されたユニットセル内に2つの分子をもつものではなく、1つの分子をものであることが分かった。1H-テトラゾールは、おそらく窒素-窒素結合ではなく炭素-窒素結合により、100GPa以下で可逆的に重合する。私たちの研究は、1H-テトラゾールの高圧相の構造モデルを更新し、もっともらしい分子間結合の経路を初めて提示した。これにより、窒素に富む化合物の相転移と化学反応の理解が進み、新しい高エネルギー密度材料の設計に役立つと考えられる。

論文

Expansion of agriculture in northern cold-climate regions; A Cross-sectoral perspective on opportunities and challenges

Unc, A.*; Altdorff, D.*; Abakumov, E.*; Adl, S.*; Baldursson, S.*; Bechtold, M.*; Cattani, D. J.*; Firbank, L. G.*; Grand, S.*; Gudjonsdottir, M.*; et al.

Frontiers in Sustainable Food Systems (Internet), 5, p.663448_1 - 663448_11, 2021/07

 被引用回数:41 パーセンタイル:93.03(Food Science & Technology)

本レビュー論文では、関連分野を研究する科学者の意識調査と既存文献の調査を実施し、地球温暖化の加速が寒冷な北方地域を地域および世界の農業セクター拡大にとってますます魅力的なターゲットにしていることを明らかにした。ただし、こうした活動の持続可能な長期的発展は、信頼性のある関連知見に対し全てのステークホルダーが容易にアクセスできる場合にのみ実現できる、という共通認識があることも明らかになった。特に、北方地域における農業の拡大は、温室効果ガス収支や生物多様性、生態系サービスに対し、負の影響をもたらす傾向にあることが明らかになってきている。以上より、寒冷な北方地域における農業の拡大と強化は、社会的な向上とニュートラルな環境影響とを両立できる計画の下で遂行される必要がある。

論文

Development of a reference database for beta-delayed neutron emission

Dimitriou, P.*; Dillmann, I.*; Singh, B.*; Piksaikin, V.*; Rykaczewski, K. P.*; Tain, J. L.*; Algora, A.*; Banerjee, K.*; Borzov, I. N.*; Cano-Ott, D.*; et al.

Nuclear Data Sheets, 173, p.144 - 238, 2021/03

 被引用回数:27 パーセンタイル:95.10(Physics, Nuclear)

核分裂の発見以降、核分裂片から放出される遅発中性子の存在には、数多くの関心が集められてきた。原子力発電では、遅発中性子は原子炉動特性の計算や炉の安全運転において非常に重要な役割を演じている。それに加え、遅発中性子は、核構造や天体核、特に新世代のRIビーム施設の中心課題である安定線から離れた原子核でも、大きなインパクトをもっている。現在、ベータ崩壊半減期と遅発中性子分岐比に関するいくつかの文献が利用可能であるが、測定と評価によって実施されるべき十分な考証は、それらの文献ではしばしば抜けている。この欠落部に注目し、遅発中性子の核データ評価とそれに関する新しい文献作成の作業が、国際原子力機関(IAEA)の援助の基に着手され、「ベータ遅発中性子用データベースの開発」に関するCoordinated Research Project (CRP)が結成された。本論文では、CRPで行われたこれまでの結果について報告をする。

論文

Suppressed lattice disorder for large emission enhancement and structural robustness in hybrid lead iodide perovskite discovered by high-pressure isotope effect

Kong, L.*; Gong, J.*; Hu, Q.*; Capitani, F.*; Celeste, A.*; 服部 高典; 佐野 亜沙美; Li, N.*; Yang, W.*; Liu, G.*; et al.

Advanced Functional Materials, 31(9), p.2009131_1 - 2009131_12, 2021/02

 被引用回数:29 パーセンタイル:83.84(Chemistry, Multidisciplinary)

有機-無機ハロゲン化物ペロブスカイトは非常に柔らかいために、圧力などの外部刺激により格子定数を容易に変化させることができ、有用な光電特性を引き出すのに有効である。一方でこの特性は、多少の加圧でも、格子を歪ませてしまい、光と物質の相互作用を弱め、それによる性能の低下を引き起こす。そこで本研究では、代表的な物質であるヨウ化メチルアンモニウム鉛に対して圧力効果および同位体効果を調べ、それらが格子歪を抑制することが分かった。このことは、それらが、これまで得られなかったような光学的,機械的特性を持つ物質を得る手段として有効であることを示している。

論文

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:244 パーセンタイル:99.77(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.

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