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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:1 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
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 (
/
=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.
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:84.76(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.
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 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.
Li, 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:21 Percentile:94.59(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:19 Percentile:93.50(Physics, Multidisciplinary)Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; Gmez-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:13 Percentile:87.42(Physics, Multidisciplinary)We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient O nucleus with large Fermi-surface asymmetry at
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.
Chen, J.*; Yamamoto, Kei; Zhang, J.*; Ma, J.*; Wang, H.*; Sun, Y.*; Chen, M.*; Liu, S.*; Gao, P.*; Yu, D.*; et al.
Physical Review Applied (Internet), 19(2), p.024046_1 - 024046_9, 2023/02
Times Cited Count:6 Percentile:62.75(Physics, Applied)Orlandi, R.; Makii, Hiroyuki; Nishio, Katsuhisa; Hirose, Kentaro; Asai, Masato; Tsukada, Kazuaki; Sato, Tetsuya; Ito, Yuta; Suzaki, Fumi; Nagame, Yuichiro*; et al.
Physical Review C, 106(6), p.064301_1 - 064301_11, 2022/12
Times Cited Count:4 Percentile:52.14(Physics, Nuclear)Zheng, R.*; Gong, W.; Du, J.-P.*; Gao, S.*; Liu, M.*; Li, G.*; Kawasaki, Takuro; Harjo, S.; Ma, C.*; Ogata, Shigenobu*; et al.
Acta Materialia, 238, p.118243_1 - 118243_15, 2022/10
Times Cited Count:44 Percentile:97.03(Materials Science, Multidisciplinary)Chen, L.*; Mao, C.*; Chung, J.-H.*; Stone, M. B.*; Kolesnikov, A. I.*; Wang, X.*; Murai, Naoki; Gao, B.*; Delaire, O.*; Dai, P.*
Nature Communications (Internet), 13, p.4037_1 - 4037_7, 2022/07
Times Cited Count:22 Percentile:81.53(Multidisciplinary Sciences)Brumm, S.*; Gabrielli, F.*; Sanchez-Espinoza, V.*; Groudev, P.*; Ou, P.*; Zhang, W.*; Malkhasyan, A.*; Bocanegra, R.*; Herranz, L. E.*; Berda, M.*; et al.
Proceedings of 10th European Review Meeting on Severe Accident Research (ERMSAR 2022) (Internet), 13 Pages, 2022/05
Wang, X.*; Tang, X.*; Zhang, P.*; Wang, Y.*; Gao, D.*; Liu, J.*; Hui, K.*; Wang, Y.*; Dong, X.*; Hattori, Takanori; et al.
Journal of Physical Chemistry Letters (Internet), 12(50), p.12055 - 12061, 2021/12
Times Cited Count:15 Percentile:70.46(Chemistry, Physical)Substituted polyacetylene is expected to improve the chemical stability, physical properties, and additional functions of the polyacetylene backbones, but its diversity is very limited. Here, by applying external pressure on solid acetylenedicarboxylic acid, we report the first crystalline poly-dicarboxylacetylene with every carbon on the trans-polyacetylene backbone bonded to a carboxyl group, which is very hard to synthesize by traditional methods. This unique structure combines the extremely high content of carbonyl groups and high conductivity of a polyacetylene backbone, which exhibits a high specific capacity and excellent cycling/rate performance as a Li-ion battery (LIB) anode. We present a completely functionalized crystalline polyacetylene and provide a high-pressure solution for the synthesis of polymeric LIB materials and other polymeric materials with a high content of active groups.
Zhang, J.*; Chen, M.*; Chen, J.*; Yamamoto, Kei; Wang, H.*; Hamdi, M.*; Sun, Y.*; Wagner, K.*; He, W.*; Zhang, Y.*; et al.
Nature Communications (Internet), 12, p.7258_1 - 7258_8, 2021/12
Times Cited Count:21 Percentile:77.31(Multidisciplinary Sciences)Yan, S. Q.*; Li, X. Y.*; Nishio, Katsuhisa; Lugaro, M.*; Li, Z. H.*; Makii, Hiroyuki; Pignatari, M.*; Wang, Y. B.*; Orlandi, R.; Hirose, Kentaro; et al.
Astrophysical Journal, 919(2), p.84_1 - 84_7, 2021/10
Times Cited Count:5 Percentile:33.27(Astronomy & Astrophysics)Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; Hattori, Takanori; Wang, Y.*; Dong, X.*; et al.
Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09
Times Cited Count:7 Percentile:42.22(Chemistry, Physical)Pressure-induced phase transition and polymerization of nitrogen-rich molecules are widely focused due to its extreme importance for the development of green high energy density materials. Here, we present a study of the phase transition and chemical reaction of 1H-tetrazole up to 100 GPa by using Raman, IR, X-ray diffraction, neutron diffraction techniques and theoretical calculation. A phase transition above 2.6 GPa was identified and the high-pressure structure was determined with one molecule in a unit cell. The 1H-tetrazole polymerizes reversibly below 100 GPa, probably through a carbon-nitrogen bonding instead of nitrogen-nitrogen bonding. Our studies updated the structure model of the high pressure phase of 1H-tetrazole, and presented the possible intermolecular bonding route for the first time, which gives new insights to understand the phase transition and chemical reaction of nitrogen-rich compounds, and benefit for designing new high energy density materials.
Nagao, Michihiro*; Kelley, E. G.*; Faraone, A.*; Saito, Makina*; Yoda, Yoshitaka*; Kurokuzu, Masayuki*; Takata, Shinichi; Seto, Makoto*; Butler, P. D.*
Physical Review Letters, 127(7), p.078102_1 - 078102_7, 2021/08
Times Cited Count:27 Percentile:86.89(Physics, Multidisciplinary)Zhai, Y.*; Luo, P.*; Nagao, Michihiro*; Nakajima, Kenji; Kikuchi, Tatsuya*; Kawakita, Yukinobu; Kienzle, P. A.*; Z, Y.*; Faraone, A.*
Physical Chemistry Chemical Physics, 23(12), p.7220 - 7232, 2021/03
Times Cited Count:5 Percentile:30.29(Chemistry, Physical)Zhang, P.*; Tang, X.*; Wang, Y.*; Wang, X.*; Gao, D.*; Li, Y.*; Zheng, H.*; Wang, Y.*; Wang, X.*; Fu, R.*; et al.
Journal of the American Chemical Society, 142(41), p.17662 - 17669, 2020/10
Times Cited Count:34 Percentile:78.58(Chemistry, Multidisciplinary)Solid-state topochemical polymerization (SSTP) is a promising method to construct functional crystalline polymeric materials, but in contrast to various reactions that happen in solution, only very limited types of SSTP reactions are reported. Diels-Alder (DA) and dehydro-DA (DDA) reactions are textbook reactions for preparing six-membered rings in solution but are scarcely seen in solid-state synthesis. Here, using multiple cutting-edge techniques, we demonstrate that the solid 1,4-diphenylbutadiyne (DPB) undergoes a DDA reaction under 10-20 GPa with the phenyl as the dienophile. The crystal structure at the critical pressure shows that this reaction is "distance-selected". The distance of 3.2 between the phenyl and the phenylethynyl facilitates the DDA reaction, while the distances for other DDA and 1,4-addition reactions are too large to allow the bonding. The obtained products are crystalline armchair graphitic nanoribbons, and hence our studies open a new route to construct the crystalline carbon materials with atomic-scale control.
Schaffer, M. J.*; Snipes, J. A.*; Gohil, P.*; de Vries, P.*; Evans, T. E.*; Fenstermacher, M. E.*; Gao, X.*; Garofalo, A. M.*; Gates, D. A.*; Greenfield, C. M.*; et al.
Nuclear Fusion, 51(10), p.103028_1 - 103028_11, 2011/10
Times Cited Count:42 Percentile:82.79(Physics, Fluids & Plasmas)Experiments at DIII-D investigated the effects of ferromagnetic error fields similar to those expected from proposed ITER Test Blanket Modules (TBMs). Studied were effects on: plasma rotation and locking; confinement; L-H transition; edge localized mode (ELM) suppression by resonant magnetic perturbations; ELMs and the H-mode pedestal; energetic particle losses; and more. The experiments used a 3-coil mock-up of 2 magnetized ITER TBMs in one ITER equatorial port. The experiments did not reveal any effect likely to preclude ITER operations with a TBM-like error field. The largest effect was slowed plasma toroidal rotation v across the entire radial profile by as much as via non-resonant braking. Changes to global
,
and
were
3 times smaller. These effects are stronger at higher
and lower
. Other effects were smaller.
Hoesch, M.*; Fukuda, Tatsuo; Mizuki, Junichiro; Takenouchi, Tomohiro*; Kawarada, Hiroshi*; Sutter, J. P.*; Tsutsui, Satoshi*; Baron, A. Q. R.*; Nagao, Masanori*; Takano, Yoshihiko*
Physical Review B, 75(14), p.140508_1 - 140508_4, 2007/04
Times Cited Count:36 Percentile:77.16(Materials Science, Multidisciplinary)We observed phonon dispersions using inelastic X-ray scattering from CVD-grown high quality superconducting (=4.2 K) boron-doped and non-doped diamonds. By comparing these two, we found almost no change in the acoustic branch along both [111] and [001] directions. On the other hand, strong softening were observed in the optical branch of the boron-doped diamond in both directions: about 2 meV at Brillouin zone boundary and 8 meV at zone center (
point). From this result we estimated the electron-phonon coupling factor
=0.33, and this supports theoretical models suggesting a phonon-mediated pairing mechanism via coupling of optical phonon modes to Fermi surfaces around the
point.