Article
Biochemistry & Molecular Biology
Pei Xie, Jin-Yun Wang, Ya-Zi Huang, Xue-Meng Wu, Zhong-Ning Chen
Summary: Two heteroctanuclear Au4Ag4 cluster complexes with a twisted paper clip structure have been prepared through self-assembly reactions. These complexes exhibit ligand fluorescence and phosphorescence in solutions, and display bright yellow-green phosphorescence in crystalline form. Mechanical grinding causes a dramatic shift from yellow-green emission to red luminescence.
Article
Materials Science, Multidisciplinary
Raquel Utrera-Melero, Brendan Huitorel, Marie Cordier, Florian Massuyeau, Jean-Yves Mevellec, Nicolas Stephant, Philippe Deniard, Camille Latouche, Charlotte Martineau-Corcos, Sandrine Perruchas
Summary: This article presents an original mechanochromic luminescent copper iodide cluster and its application in the synthesis of mechanically responsive films. The mechanochromic mechanism is attributed to the structural changes of the molecular cluster at defects created locally in the crystalline structure, leading to intense room temperature emission in response to mechanical forces. The mechanically responsive films based on the studied cluster exhibit high contrasted luminescence mechanochromic properties with writing and erasing activating and deactivating the emission of the photoactive component.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Engineering, Electrical & Electronic
Sehoon Park, Dae-Woong Park, Kristof Vaesen, Anirudh Kankuppe, Siddhartha Sinha, Barend van Liempd, Piet Wambacq, Jan Craninckx
Summary: This article presents the design method of a low-power, high-efficiency, x9 frequency-modulated continuous-wave (FMCW) radar transmitter operating in the 135-155 GHz frequency range. The transmitter uses cascaded frequency triplers to bring the signal to the desired frequency band and employs phase-controlled frequency tripling to boost the output power and RF conversion efficiency. Experimental results demonstrate that this transmitter achieves high output power and efficiency in a 28nm CMOS process.
IEEE JOURNAL OF SOLID-STATE CIRCUITS
(2022)
Article
Chemistry, Physical
Hao Yan, Tzu-Wei Tseng, Shun Omagari, Iain Hamilton, Tomonori Nakamura, Martin Vacha, Ji-Seon Kim
Summary: In this study, the role of the beta-phase in polyfluorene-based copolymers on energy transfer (ET) was investigated. The results showed that the beta-phase can significantly improve the performance and color purity of polymer light-emitting devices. By conducting single-molecule spectroscopy, it was found that efficient ET occurs from the glassy phase to the beta-phase. Density functional theory calculations and temperature-dependent spectroscopy confirmed the mechanism of ET from the glassy phase to the CT state.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Masato Kobayashi, Yuta Oba, Tomoko Akama, Tetsuya Taketsugu
Summary: This paper proposes a practical electronic calculation method for lanthanide complexes, which introduces the frozen core potential approximation and relaxation of rotational degrees of freedom to improve the accuracy and convergence of the calculations.
JOURNAL OF MATHEMATICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Hiroaki Iwamoto, Yu Ozawa, Yuta Hayashi, Tsuneo Imamoto, Hajime Ito
Summary: A new series of C-1-symmetric P-chirogenic bisphosphine ligands have been developed, which showed high performance in a copper(I)-catalyzed asymmetric borylation reaction. Computational studies highlighted the importance of the highly rigid phosphine conformation in achieving high stereo- and product-selectivities.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Takao Tsuneda, Hiroki Sumitomo, Masatoshi Hasebe, Takuro Tsutsumi, Tetsuya Taketsugu
Summary: It has been established that the reactive orbital energy theory (ROET) can theoretically reproduce the rule-based electronic theory diagrams of organic chemistry. By studying the charge transfer natures of typical organic carbon-carbon and carbon-heteroatom bond formation reactions, the ROET provides insights into the reactive orbitals and charge transferability indices. The ROET analyses also reveal the detailed orbital-based mechanisms for these reactions, explaining the pi-bond formations in acidic conditions and sigma-bond formations at alpha-carbons in basic conditions. Moreover, it is suggested that the methyl group plays a role in accepting and donating electrons in these reactions.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tomonori Nakamura, Shun Omagari, Xiaobin Liang, Qiwen Tan, Ken Nakajima, Martin Vacha
Summary: Using atomic force microscopy and fluorescence microscopy, we studied the single-chain structure of conjugated polymer polyfluorene (PFO). We found that mechanical stretching of the chain causes disappearance of the green emission band, indicating that the green emission originates from an intrachain aggregated state on the self-folded chain. Additionally, stretching upon laser irradiation leads to the appearance of additional features in the force spectra, small force peales in the initial stages of the unfolding, which are attributed to a combination of excitonic and van der Waals coupling of a ground-state intrachain aggregate.
Article
Chemistry, Physical
Masatsugu Nishida, Tomoko Akama, Masato Kobayashi, Tetsuya Taketsugu
Summary: In this study, a time-dependent Hartree-Fock-Bogoliubov (HFB) method is proposed for treating the excited states of molecules with static correlations at a reasonable computational cost. The canonical basis variant of the TDHFB method proposed by Ebata et al. is also considered to avoid electron number violations. Calculation results for the elongated hydrogen molecule show that the TDHFB method can partially incorporate two-electron excited determinants.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Hung Cuong Dinh, Ganesan Elumalai, Hidenori Noguchi, Andrey Lyalin, Tetsuya Taketsugu, Kohei Uosaki
Summary: In this study, the electrocatalytic activities of gold (Au) electrodes for the oxygen reduction reaction (ORR) were enhanced by modifying the Au surface with size-selected hexagonal boron nitride nanosheets (BNNS). The smaller the size of the BNNS, the lower the overpotential for ORR and the higher the ORR activity. The smallest BNNS size range (0.1-0.22 μm) reduced the overpotential by as much as 330 mV compared to a bare Au electrode, and it exhibited an ORR activity only 80 mV higher than that of a platinum (Pt) electrode.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
Takayuki Nakanishi, Yuichi Hirai, Jian Xu, Takashi Takeda, Shunsuke Watanabe, Atsuo Yasumori, Shou Hakamada, Yuichi Kitagawa, Yasuchika Hasegawa
Summary: Luminescent lanthanide coordination polymer crystals (LCPCs) are of great interest in materials chemistry due to their unique and customizable functional properties. These crystals offer a high degree of structural tunability, including size- and morphology-dependent properties, making them promising materials for various applications such as light emitting diodes.
SCIENCE AND TECHNOLOGY OF ADVANCED MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Yuichi Hirai, Stann Van Baaren, Takahito Ohmura, Takayuki Nakanishi, Takashi Takeda, Yuichi Kitagawa, Yasuchika Hasegawa, Remi Metivier, Clemence Allain
Summary: In pursuit of new mechanically responsive luminescent materials, the study aims to differentiate triboluminescence (TL) from photoluminescence (PL). A beta-diketonate ligand with tert-butyl groups is used to quench Eu-III-centered PL and provide efficient photosensitization of Tb-III ions. Nanomechanical tests reveal the ductility of the crystals, making them ideal for accumulating deformation energy before breakage. Additionally, the study investigates the TL/PL color difference and mechanochromic luminescence (MCL) in a Tb-III/Eu-III heterodinuclear complex.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Masatoshi Hasebe, Takuro Tsutsumi, Tetsuya Taketsugu, Takao Tsuneda
Summary: This study compares the effects of the long-range correction (LC) and CCSD method on the total and orbital electron densities of molecules. The LC stabilizes electrons in the long-range interaction regions of kinetic energy density, while the CCSD method stabilizes electrons in the long-range interaction regions in the vertical molecular planes. The LC has a similar effect to the CCSD method on unoccupied orbitals, but differs for occupied orbitals.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Toranosuke Takagi, Shun Omagari, Martin Vacha
Summary: In this study, ligand exchange on the CsPbBr3 perovskite nanocrystal surface was performed and its effect on photoluminescence blinking was investigated. By replacing oleic acid and oleylamine ligands with quaternary amine ligands used in the synthesis process, a substantial increase in photoluminescence quantum yield and improved blinking characteristics were achieved. Statistical analysis showed longer duration of ON-times, shorter OFF-times, and a higher fraction of ON-time intervals after the ligand exchange.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Anubha Agarwal, Shun Omagari, Martin Vacha
Summary: We prepared and characterized mixed cation perovskite films of MA(1-x)FA(x)PbI(3) composition with x = 0, 0.3, and 0.5 at the nanoscale level. Films with x = 0.5 and 0.3, prepared using ethyl acetate as an antisolvent in a one-step spin-coating process, showed compositionally stability in ambient air for over a year, unlike films prepared with chlorobenzene antisolvent. In situ photoluminescence spectroscopy was used to monitor the degradation onset near the film edges, with degradation products exhibiting similar photoluminescence spectra to 2D perovskite sheets. Morphologically, aging of the films resulted in the coalescence of film grain structure into larger crystal grains. Additionally, aging did not affect dynamic photoluminescence quenching or long-range charge diffusion on the order of micrometers.
Article
Chemistry, Multidisciplinary
Keisuke Tashiro, Masato Kobayashi, Kiyotaka Nakajima, Tetsuya Taketsugu
Summary: A comprehensive reaction-path search using quantum chemical calculations was conducted to understand the mechanism of humin formation in the oxidation of HMF to FDCA. The study identified multiple reaction paths with low barriers for the reaction of HMF with OH-. It was also confirmed computationally that acetal protection of HMF could suppress humin formation.
Article
Chemistry, Multidisciplinary
Kewei Sun, Kazuma Sugawara, Andrey Lyalin, Yusuke Ishigaki, Kohei Uosaki, Oscar Custance, Tetsuya Taketsugu, Takanori Suzuki, Shigeki Kawai
Summary: In this study, complex organometallic oligomers were systematically synthesized on Cu(111) through sequential ring opening and bonding of phenanthroline derivatives by multiple Cu atoms. Characterization using scanning tunneling microscopy and density functional theory calculations revealed the role of Cu adatoms in the chiral oligomers. Furthermore, the strength of the bonds against sliding friction was found to be sufficient.
Article
Chemistry, Multidisciplinary
Satoi Wada, Takuro Tsutsumi, Kenichiro Saita, Tetsuya Taketsugu
Summary: Recently, surface-hopping ab initio molecular dynamics (SH-AIMD) simulations have been used to study the mechanisms and dynamics of excited-state chemical reactions. In this study, the authors investigate the effects of spin-orbit coupling (SOC) on the results of dynamics simulations using spin-pure and spin-mixed states for the hydride MH2 (M = Si, Ge, Sn, Pb). The results show that spin-mixed state potential energy surfaces are essential for simulating intersystem crossing in systems containing Sn and Pb elements.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)