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Journal Articles

Ordered graphane nanoribbons synthesized via high-pressure diels-alder polymerization of 2,2'-bipyrazine

Li, F.*; Tang, X.*; Fei, Y.*; Zhang, J.*; Liu, J.*; Lang, P.*; Che, G.*; Zhao, Z.*; Zheng, Y.*; Fang, Y.*; et al.

Journal of the American Chemical Society, 147(17), p.14054 - 14059, 2025/04

 Times Cited Count:0 Percentile:0.00(Chemistry, Multidisciplinary)

We synthesized a crystalline graphane nanoribbon (GANR) via pressure-induced polymerization of 2,2'-bipyrazine (BPZ). By performing Rietveld refinement of in situ neutron diffraction data, nuclear magnetic resonance spectroscopy, infrared spectra, and theoretical calculation, we found that BPZ experienced Diels-Alder polymerization between the $$pi$$ $$cdots$$ $$pi$$ stacked aromatic rings, and formed extended boat-GANR structures with exceptional long-range order. The unreacted -C=N- groups bridge the two ends of the boat, and ready for further functionalization. The GANR has a bandgap of 2.25 eV, with booming photoelectric response ($$I_{rm on}$$/$$I_{rm off}$$ =18.8). Our work highlights that the high-pressure topochemical polymerization is a promising method for the precise synthesis of graphane with specific structure and desired properties.

Journal Articles

High-pressure polymerization of phenol toward degree-4 carbon nanothread

Yang, X.*; Che, G.*; Wang, Y.*; Zhang, P.*; Tang, X.*; Lang, P.*; Gao, D.*; Wang, X.*; Wang, Y.*; Hattori, Takanori; et al.

Nano Letters, 25(3), p.1028 - 1035, 2025/01

 Times Cited Count:1 Percentile:0.00(Chemistry, Multidisciplinary)

Saturated sp$$^3$$-carbon nanothreads (CNTh) have garnered significant interest due to their predicted high Young's modulus and thermal conductivity. While the incorporation of heteroatoms into the central ring has been shown to influence the formation of CNTh and yield chemically homogeneous products, the impact of pendant groups on the polymerization process remains underexplored. In this study, we investigate the pressure-induced polymerization of phenol, revealing two phase transitions occurring below 0.5 and 4 GPa. Above 20 GPa, phenol polymerizes into degree-4 CNThs featuring hydroxyl and carbonyl groups. Hydrogen transfer of hydroxyl groups was found to hinder the formation of degree-6 nanothreads. Our findings highlight the crucial role of the hydroxyl group in halting further intracolumn polymerization and offer valuable insights for future mechanism research and nanomaterial synthesis.

Journal Articles

Pressure-induced polymerization of 1,4-difluorobenzene towards fluorinated diamond nanothreads

Che, G.*; Fei, Y.*; Tang, X.*; Zhao, Z.*; Hattori, Takanori; Abe, Jun*; Wang, X.*; Ju, J.*; Dong, X.*; Wang, Y.*; et al.

Physical Chemistry Chemical Physics, 27(2), p.1112 - 1118, 2025/01

 Times Cited Count:3 Percentile:65.57(Chemistry, Physical)

Pressure-induced polymerization (PIP) of aromatic molecules has emerged as an effective method for synthesizing various carbon-based materials. In this work, PIP of 1,4-difluorobenzene (1,4-DFB) was investigated. ${it In situ}$ high-pressure investigations of 1,4-DFB reveal a phase transition at approximately 12.0 GPa and an irreversible chemical reaction at 18.7 GPa. Structural analysis of the product and the kinetics of the reaction uncovered the formation of pseudohexagonal stacked fluoro-diamond nanothreads with linear growth. Compared to the crystal structures of benzene under high pressure, 1,4-DFB exhibits higher compression along the [001] axis. The anisotropic compression is attributed to the stronger H$$cdot cdot cdot pi$$ interaction along the [01$$overline{1}$$] axis and the potential compression-inhibiting H$$cdot cdot cdot$$F interactions along the [100] and [010] axes, and it facilitates a possible reaction pathway along the [01$$overline{1}$$] axis. This work emphasizes the crucial role of functionalization in modulating molecular stacking and influencing the reaction pathway.

Journal Articles

Solid-state Alder-ene reaction of 1-hexene under high pressure

Xu, J.*; Lang, P.*; Liang, S.*; Zhang, J.*; Fei, Y.*; Wang, Y.*; Gao, D.*; Hattori, Takanori; Abe, Jun*; Dong, X.*; et al.

Journal of Physical Chemistry Letters (Internet), p.2445 - 2451, 2025/00

 Times Cited Count:0 Percentile:0.00(Chemistry, Physical)

The Alder-ene reaction is a chemical reaction between an alkene with an allylic hydrogen, and it provides an efficient method to construct the C-C bond. Traditionally, this reaction requires catalysts, high temperatures, or photocatalysis. In this study, we reported a high-pressure-induced solid-state Alder-ene reaction of 1-hexene at room temperature without a catalyst. 1-Hexene crystallizes at 4.3 GPa and polymerizes at 18 GPa, forming olefins. By exploring gas chromatography-mass spectrometry, we discovered that 1-hexene generates dimeric products through the Alder-ene reaction under high pressures. The in situ neutron diffraction shows that the reaction process did not obey the topochemical rule. A six-membered ring transition state including one C-H $$sigma$$ bond and two alkene $$pi$$ bonds was evidenced by the theoretical calculation, whose energy obviously decreased when compressed to 20 GPa. Our work offers a novel and promising method to realize the Alder-ene reaction at room temperature without a catalyst, expanding the application of this important reaction.

Journal Articles

Strong low-energy rattling modes enabled liquid-like ultralow thermal conductivity in a well-ordered solid

Liu, P.-F.*; Li, X.*; Li, J.*; Zhu, J.*; Tong, Z.*; Kofu, Maiko*; Nirei, Masami; Xu, J.*; Yin, W.*; Wang, F.*; et al.

National Science Review, 11(12), p.nwae216_1 - nwae216_10, 2024/12

 Times Cited Count:12 Percentile:91.22(Multidisciplinary Sciences)

Journal Articles

Brightening triplet excitons enable high-performance white-light emission in organic small molecules via integrating n-$$pi^*/pi$$-$$pi^*$$ transitions

Yang, Q.*; Yang, X.*; Wang, Y.*; Fei, Y.*; Li, F.*; Zheng, H.*; Li, K.*; Han, Y.*; Hattori, Takanori; Zhu, P.*; et al.

Nature Communications (Internet), 15, p.7778_1 - 7778_9, 2024/09

 Times Cited Count:9 Percentile:88.46(Multidisciplinary Sciences)

Luminescent materials that simultaneously embody bright singlet and triplet excitons hold great potential in optoelectronics, signage, and information encryption. However, achieving high-performance white-light emission is severely hampered by their inherent unbalanced contribution of fluorescence and phosphorescence. Herein, we address this challenge by pressure treatment engineering via hydrogen bonding cooperativity effect to realize the mixture of n-$$pi^*/pi$$-$$pi^*$$ transitions, where the triplet state emission was boosted from 7% to 40% in isophthalic acid (IPA). A superior white-light emission based on hybrid fluorescence and phosphorescence was harvested in pressure-treated IPA, and the photoluminescence quantum yield was increased to 75% from the initial 19% (blue-light emission). In-situ high-pressure IR spectra, X ray diffraction, and neutron diffraction reveal continuous strengthening of the hydrogen bonds with the increase of pressure. Furthermore, this enhanced hydrogen bond is retained down to the ambient conditions after pressure treatment, awarding the targeted IPA efficient intersystem crossing for balanced singlet/triplet excitons population and resulting in efficient white-light emission. This work not only proposes a route for brightening triplet states in organic small molecule, but also regulates the ratio of singlet and triplet excitons to construct high-performance white-light emission.

Journal Articles

Antiferromagnetism and phase stability of CrMnFeCoNi high-entropy alloy

Zhu, L.*; He, H.*; Naeem, M.*; Sun, X.*; Qi, J.*; Liu, P.*; Harjo, S.; Nakajima, Kenji; Li, B.*; Wang, X.-L.*

Physical Review Letters, 133(12), p.126701_1 - 126701_6, 2024/09

 Times Cited Count:1 Percentile:48.32(Physics, Multidisciplinary)

Journal Articles

Gradient residual strain measurement procedure in surface impacted railway steel axles by using neutron scattering

Zhou, L.*; Zhang, H.*; Qin, T. Y.*; Hu, F. F.*; Xu, P. G.; Ao, N.*; Su, Y. H.; He, L. H.*; Li, X. H.*; Zhang, J. R.*; et al.

Metallurgical and Materials Transactions A, 55(7), p.2175 - 2185, 2024/07

 Times Cited Count:3 Percentile:75.40(Materials Science, Multidisciplinary)

Journal Articles

Crystal-liquid duality driven ultralow two-channel thermal conductivity in $$alpha$$-MgAgSb

Li, J.*; Li, X.*; Zhang, Y.*; Zhu, J.*; Zhao, E.*; Kofu, Maiko; Nakajima, Kenji; Avdeev, M.*; Liu, P.-F.*; Sui, J.*; et al.

Applied Physics Reviews (Internet), 11(1), p.011406_1 - 011406_8, 2024/03

 Times Cited Count:7 Percentile:91.57(Physics, Applied)

Journal Articles

Onset of collectivity for argon isotopes close to $$N=32$$

Linh, B. D.*; Corsi, A.*; Gillibert, A.*; Obertelli, A.*; Doornenbal, P.*; Barbieri, C.*; Duguet, T.*; G$'o$mez-Ramos, M.*; Holt, J. D.*; Hu, B. S.*; et al.

Physical Review C, 109(3), p.034312_1 - 034312_15, 2024/03

 Times Cited Count:2 Percentile:58.81(Physics, Nuclear)

no abstracts in English

Journal Articles

The BCC $$rightarrow$$ FCC hierarchical martensite transformation under dynamic impact in FeMnAlNiTi alloy

Li, C.*; Fang, W.*; Yu, H. Y.*; Peng, T.*; Yao, Z. T.*; Liu, W. G.*; Zhang, X.*; Xu, P. G.; Yin, F.*

Materials Science & Engineering A, 892, p.146096_1 - 146096_11, 2024/02

 Times Cited Count:4 Percentile:82.70(Nanoscience & Nanotechnology)

Journal Articles

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.*; Kajimoto, Ryoichi; Ikeuchi, Kazuhiko*; Deng, G.*; et al.

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

 Times Cited Count:2 Percentile:62.71(Materials Science, Multidisciplinary)

Journal Articles

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.*; Kanada-En'yo, Yoshiko*; et al.

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

 Times Cited Count:21 Percentile:93.59(Physics, Multidisciplinary)

The cluster structure of the neutron-rich isotope $$^{10}$$Be has been probed via the ($$p,palpha$$) reaction. The triple differential cross-section was extracted and compared to distorted-wave impulse approximation reaction calculations performed in a microscopic framework using the Tohsaki-Horiuchi-Schuck-R$"o$pke wave function and the wave function deduced from Antisymmetrized Molecular Dynamics calculations. The remarkable agreement between calculated and measured cross-sections in both shape and magnitude validates the description of the $$^{10}$$Be ground-state as a rather compact nuclear molecule.

Journal Articles

A One-third magnetization plateau phase as evidence for the Kitaev interaction in a honeycomb-lattice antiferromagnet

Shangguan, Y.*; Bao, S.*; Dong, Z.-Y.*; Xi, N.*; Gao, Y.-P.*; Ma, Z.*; Wang, W.*; Qi, Z.*; Zhang, S.*; Huang, Z.*; et al.

Nature Physics, 19(12), p.1883 - 1889, 2023/09

 Times Cited Count:19 Percentile:94.19(Physics, Multidisciplinary)

Journal Articles

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

Chen, S.*; Browne, F.*; Doornenbal, P.*; Lee, J.*; Obertelli, A.*; Tsunoda, Yusuke*; Otsuka, Takaharu*; Chazono, Yoshiki*; Hagen, G.*; Holt, J. D.*; et al.

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

 Times Cited Count:9 Percentile:85.35(Astronomy & Astrophysics)

Gamma decays were observed in $$^{56}$$Ca and $$^{58}$$Ca following quasi-free one-proton knockout reactions from $$^{57,59}$$Sc. For $$^{56}$$Ca, a $$gamma$$ ray transition was measured to be 1456(12) keV, while for $$^{58}$$Ca an indication for a transition was observed at 1115(34) keV. Both transitions were tentatively assigned as the $$2^{+}_{1} rightarrow 0^{+}_{gs}$$ decays. A shell-model calculation in a wide model space with a marginally modified effective nucleon-nucleon interaction depicts excellent agreement with experiment for $$2^{+}_{1}$$ level energies, two-neutron separation energies, and reaction cross sections, corroborating the formation of a new nuclear shell above the N = 34 shell. Its constituents, the $$0_{f5/2}$$ and $$0_{g9/2}$$ orbitals, are almost degenerate. This degeneracy precludes the possibility for a doubly magic $$^{60}$$Ca and potentially drives the dripline of Ca isotopes to $$^{70}$$Ca or even beyond.

Journal Articles

Pressure-modulated magnetism and negative thermal expansion in the Ho$$_2$$Fe$$_{17}$$ intermetallic compound

Cao, Y.*; Zhou, H.*; Khmelevskyi, S.*; Lin, K.*; Avdeev, M.*; Wang, C.-W.*; Wang, B.*; Hu, F.*; Kato, Kenichi*; Hattori, Takanori; et al.

Chemistry of Materials, 35(8), p.3249 - 3255, 2023/04

 Times Cited Count:2 Percentile:21.90(Chemistry, Physical)

Hydrostatic and chemical pressure are efficient stimuli to alter the crystal structure and are commonly used for tuning electronic and magnetic properties in materials science. However, chemical pressure is difficult to quantify and a clear correspondence between these two types of pressure is still lacking. Here, we study intermetallic candidates for a permanent magnet with a negative thermal expansion (NTE). Based on in situ synchrotron X-ray diffraction, negative chemical pressure is revealed in Ho$$_2$$Fe$$_{17}$$ on Al doping and quantitatively evaluated by using temperature and pressure dependence of unit cell volume. A combination of magnetization and neutron diffraction measurements also allowed one to compare the effect of chemical pressure on magnetic ordering with that of hydrostatic pressure. Intriguingly, pressure can be used to control suppression and enhancement of NTE. Electronic structure calculations indicate that pressure affected the top of the majority band with respect to the Fermi level, which has implications for the magnetic stability, which in turn plays a critical role in modulating magnetism and NTE. This work presents a good example of understanding the effect of pressure and utilizing it to control properties of functional materials.

Journal Articles

Multiple mechanisms in proton-induced nucleon removal at $$sim$$100 MeV/nucleon

Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; G$'o$mez-Ramos, M.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Cai, B. S.*; Yuan, C. X.*; Brown, B. A.*; et al.

Physical Review Letters, 130(17), p.172501_1 - 172501_8, 2023/04

 Times Cited Count:12 Percentile:88.25(Physics, Multidisciplinary)

We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient $$^{14}$$O nucleus with large Fermi-surface asymmetry at $$sim$$100 MeV/nucleon. Our results provide the first quantitative contributions of multiple reaction mechanisms including the quasifree knockout, inelastic scattering, and nucleon transfer processes. It is shown that the inelastic scattering and nucleon transfer, usually neglected at such energy regime, contribute about 50% and 30% to the loosely bound proton and deeply bound neutron removal, respectively.

Journal Articles

Mg-Zn-Mn oxide systems for a rechargeable Mg-battery cathode

Ye, X.*; Shimokawa, Kohei*; Kezuka, Yuto*; Hatakeyama, Takuya*; Li, H.*; Ichitsubo, Tetsu

Journal of Physical Chemistry C, 127(11), p.5210 - 5218, 2023/03

 Times Cited Count:2 Percentile:10.57(Chemistry, Physical)

Journal Articles

A Colossal barocaloric effect induced by the creation of a high-pressure phase

Jiang, X.*; Hattori, Takanori; Xu, X.*; Li, M.*; Yu, C.*; Yu, D.*; Mole, R.*; Yano, Shinichiro*; Chen, J.*; He, L.*; et al.

Materials Horizons, 10(3), p.977 - 982, 2023/03

 Times Cited Count:26 Percentile:93.43(Chemistry, Multidisciplinary)

As a promising environment-friendly alternative to current vapor-compression refrigeration, solid-state refrigeration based on the barocaloric effect has been attracting world wide attention. Generally, both phases in which a barocaloric effect occurs are present at ambient pressure. Here, instead, we demonstrate that KPF$$_{6}$$ exhibits a colossal barocaloric effect due to the creation of a high-pressure rhombohedral phase. The phase diagram is constructed based on pressure-dependent calorimetric, Raman scattering, and neutron diffraction measurements. The present study is expected to provide an alternative routine to colossal barocaloric effects through the creation of a high-pressure phase.

Journal Articles

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

Wei, D.*; Gong, W.; Tsuru, Tomohito; Lobzenko, I.; Li, X.*; Harjo, S.; Kawasaki, Takuro; Do, H.-S.*; Bae, J. W.*; Wagner, C.*; et al.

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

 Times Cited Count:105 Percentile:99.79(Engineering, Mechanical)

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