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Che, G.*; Tang, X.*; Liu, J.*; Lang, P.*; Fei, Y.*; Yang, X.*; Wang, Y.*; Gao, D.*; Wang, X.*; Ju, J.*; et al.
Nano Letters, 25(39), p.14467 - 14472, 2025/09
Mechanochemical radical polymerization has unique advantages in the synthesis of polymer due to its reduced solvent consumption and adaptability of insoluble monomers. However, it suffers from the uncontrollable degradation of the formed polymers during reaction and new synthetic strategy with precise controllability needs to be developed. Here, by employing high static pressure up to 30 GPa, we found 1,3,5-trifluorobenzene undergoes radical polymerization by breaking the conjugated
-bonds, and forms a carbon nanothread with high selectivity (Polymer-I polymorph). Based on the crystal structure at the threshold pressure and the calculated energy barriers for the bonding pathway, we concluded that the benzene-rings react via a 1-2 radical polymerization pathway. Our work highlights high pressure is a robust method to initiate the solid-state radical polymerization, even for very stable aromatics, and offers fresh insights for the synthesis of polymeric carbon-based materials with high selectivity.
Naeem, M.*; Rehman, A. U.*; Romero Resendiz, L.*; Salamci, E.*; Aydin, H.*; Ansari, P.*; Harjo, S.; Gong, W.; Wang, X.-L.*; 3 of others*
Communications Materials (Internet), 6, p.65_1 - 65_13, 2025/04
Naeem, M.*; Ma, Y.*; Tian, J.*; Kong, H.*; Romero-Resendiz, L.*; Fan, Z.*; Jiang, F.*; Gong, W.; Harjo, S.; Wu, Z.*; et al.
Materials Science & Engineering A, 924, p.147819_1 - 147819_10, 2025/02
Times Cited Count:1 Percentile:63.96(Nanoscience & Nanotechnology)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:2 Percentile:82.57(Chemistry, Multidisciplinary)Saturated sp
-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.
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:57.51(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.
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
interaction along the [01
] axis and the potential compression-inhibiting H
F interactions along the [100] and [010] axes, and it facilitates a possible reaction pathway along the [01
] axis. This work emphasizes the crucial role of functionalization in modulating molecular stacking and influencing the reaction pathway.
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:1 Percentile:69.06(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
bond and two alkene
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.
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:16 Percentile:91.80(Multidisciplinary Sciences)
-
transitionsYang, 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:16 Percentile:91.89(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-
-
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.
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:4 Percentile:70.50(Physics, Multidisciplinary)Ying, H.*; Yang, X.*; He, H.*; Yan, A.*; An, K.*; Ke, Y.*; Wu, Z.*; Tang, S.*; Zhang, Z.*; Dong, H.*; et al.
Scripta Materialia, 250, p.116181_1 - 116181_7, 2024/09
Times Cited Count:5 Percentile:75.30(Nanoscience & Nanotechnology)Wang, S.*; Wang, J.*; Zhang, S.*; Wei, D.*; Chen, Y.*; Rong, X.*; Gong, W.; Harjo, S.; Liu, X.*; Jiao, Z.*; et al.
Journal of Materials Science & Technology, 185, p.245 - 258, 2024/06
Times Cited Count:21 Percentile:97.66(Materials Science, Multidisciplinary)Ma, Y.*; Naeem, M.*; Zhu, L.*; He, H.*; Sun, X.*; Yang, Z.*; He, F.*; Harjo, S.; Kawasaki, Takuro; Wang, X.-L.*
Acta Materialia, 270, p.119822_1 - 119822_13, 2024/05
Times Cited Count:11 Percentile:91.62(Materials Science, Multidisciplinary)Yuan, X.*; Hu, Q. H.*; Fang, X.*; Wang, Q. M.*; Ma, Y.*; Tachi, Yukio
Sedimentary Geology, 465, p.106633_1 - 106633_14, 2024/05
Times Cited Count:0 Percentile:0.00(Geology)
-MgAgSbLi, 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:13 Percentile:91.92(Physics, Applied)
Linh, B. D.*; Corsi, A.*; Gillibert, A.*; Obertelli, A.*; Doornenbal, P.*; Barbieri, C.*; Duguet, T.*; G
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:3 Percentile:71.61(Physics, Nuclear)no abstracts in English
Sn
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:4 Percentile:69.82(Materials Science, Multidisciplinary)
Be ground-state molecular structure using
Be(
)
He triple differential reaction cross-section measurementsLi, P. J.*; Beaumel, D.*; Lee, J.*; Assi
, 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:25 Percentile:94.14(Physics, Multidisciplinary)The cluster structure of the neutron-rich isotope
Be has been probed via the (
) 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
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
Be ground-state as a rather compact nuclear molecule.
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:23 Percentile:93.71(Physics, Multidisciplinary)
Ca cast doubt on a doubly magic
CaChen, 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:84.70(Astronomy & Astrophysics)Gamma decays were observed in
Ca and
Ca following quasi-free one-proton knockout reactions from
Sc. For
Ca, a
ray transition was measured to be 1456(12) keV, while for
Ca an indication for a transition was observed at 1115(34) keV. Both transitions were tentatively assigned as the
decays. A shell-model calculation in a wide model space with a marginally modified effective nucleon-nucleon interaction depicts excellent agreement with experiment for
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
and
orbitals, are almost degenerate. This degeneracy precludes the possibility for a doubly magic
Ca and potentially drives the dripline of Ca isotopes to
Ca or even beyond.
Fe
intermetallic compoundCao, 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:5 Percentile:51.21(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
Fe
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.