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41.
Dr. Takaaki Mitsuhashi Dr. Lena Barra Zachary Powers Volga Kojasoy Andrea Cheng Feng Yang Dr. Yoshimasa Taniguchi Dr. Takashi Kikuchi Prof. Dr. Makoto Fujita Prof. Dr. Dean J. Tantillo Prof. Dr. John A. Porco Jr Prof. Dr. Ikuro Abe 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):23980-23989
Fungal meroterpenoids are a diverse group of hybrid natural products with impressive structural complexity and high potential as drug candidates. In this work, we evaluate the promiscuity of the early structure diversity-generating step in fungal meroterpenoid biosynthetic pathways: the multibond-forming polyene cyclizations catalyzed by the yet poorly understood family of fungal meroterpenoid cyclases. In total, 12 unnatural meroterpenoids were accessed chemoenzymatically using synthetic substrates. Their complex structures were determined by 2D NMR studies as well as crystalline-sponge-based X-ray diffraction analyses. The results obtained revealed a high degree of enzyme promiscuity and experimental results which together with quantum chemical calculations provided a deeper insight into the catalytic activity of this new family of non-canonical, terpene cyclases. The knowledge obtained paves the way to design and engineer artificial pathways towards second generation meroterpenoids with valuable bioactivities based on combinatorial biosynthetic strategies. 相似文献
42.
Munetaka Iwamura Airi Fukui Koichi Nozaki Hikaru Kuramochi Satoshi Takeuchi Tahei Tahara 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(51):23354-23361
Femtosecond time-resolved absorption and picosecond time-resolved emission measurements were carried out for highly concentrated aqueous solutions of K2[Pt(CN)4] to investigate excited-state dynamics of the [Pt(CN)42−] oligomers formed with metallophilic interactions. Time-resolved absorption spectra exhibit complicated dynamics that are represented with five time constants. Among them, the 90-ps and 400-ps dynamics were assigned to the S1 → T1 intersystem crossing of the trimer and tetramer coexisting in the solution by comparison with the fluorescence decays. Clear oscillations of transient absorption were observed in the first few picoseconds, and the frequency-detected-wavelength 2D analysis revealed that the 135-cm−1 and 65-cm−1 oscillations arise from the Pt–Pt stretch motions of the S1 trimer and S1 tetramer, respectively. The obtained time-resolved spectroscopic data provide a clear view of the excited-state dynamics of the [Pt(CN)42−] oligomers in the femto-/picosecond time region. 相似文献
43.
Ryo Kimura Hikaru Kuramochi Pengpeng Liu Takuya Yamakado Atsuhiro Osuka Tahei Tahara Shohei Saito 《Angewandte Chemie (International ed. in English)》2020,59(38):16430-16435
Flapping fluorophores (FLAP) with a flexible 8π ring are rapidly gaining attention as a versatile photofunctional system. Here we report a highly photostable “flapping peryleneimide” with an unprecedented fluorogenic mechanism based on a bent‐to‐planar conformational change in the S1 excited state. The S1 planarization induces an electronic configurational switch, almost quenching the inherent fluorescence (FL) of the peryleneimide moieties. However, the FL quantum yield is remarkably improved with a prolonged lifetime upon a slight environmental change. This fluorogenic function is realized by sensitive π‐conjugation design, as a more π‐expanded analogue does not show the planarization dynamics. With strong visible‐light absorption, the FL lifetime response synchronized with the flexible flapping motion is useful for the latest optical techniques such as FL lifetime imaging microscopy (FLIM). 相似文献
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The spin torque and zeta force, which govern spin dynamics, are studied by using monoatoms in their steady states. We find nonzero local spin torque in transition metal atoms, which is in balance with the counter torque, the zeta force. We show that d-orbital electrons have a crucial effect on these torques. Nonzero local chirality density in transition metal atoms is also found, though the electron mass has the effect to wash out nonzero chirality density. Distribution patterns of the chirality density are the same for Sc–Ni atoms, though the electron density distributions are different. 相似文献
50.
We have investigated the values of the Rashba spin-orbit coupling constant alpha in In(0.52)Al(0.48)As/In(0.53)Ga(0.47)As/In(0.52)Al(0.48)As quantum wells using the weak antilocalization (WAL) analysis as a function of the structural inversion asymmetry (SIA) of the quantum wells. We have found that the deduced alpha values have a strong correlation with the degree of SIA of the quantum wells as predicted theoretically. The good agreement between the theoretical and experimental values of alpha suggests that our WAL approach for deducing alpha values provides a useful tool in designing future spintronics devices that utilize the Rashba spin-orbit coupling. 相似文献