scispace - formally typeset
Search or ask a question
Author

Takashi Kubo

Other affiliations: University of Hyogo, Université de Namur, Ehime University  ...read more
Bio: Takashi Kubo is an academic researcher from Osaka University. The author has contributed to research in topics: Diradical & Singlet state. The author has an hindex of 50, co-authored 286 publications receiving 8642 citations. Previous affiliations of Takashi Kubo include University of Hyogo & Université de Namur.


Papers
More filters
Journal ArticleDOI
TL;DR: In this paper, the second hyperpolarizability of singlet diradical systems is investigated using a model compound, the p-quinodimethane (PQM) molecule with different both-end carbon−carbon (C−C) bond lengths, by several ab initio molecular orbital and density functional theory methods.
Abstract: The dependence of the second hyperpolarizability (γ) on the diradical character (y) for singlet diradical systems is investigated using a model compound, the p-quinodimethane (PQM) molecule with different both-end carbon−carbon (C−C) bond lengths, by several ab initio molecular orbital and density functional theory methods. The diradical character based on UHF calculations indicates that at equilibrium geometry PQM is in a singlet ground state and primarily exhibits a quinoid structure, whereas the diradical character increases when increasing both-end C−C bond lengths. At the highest level of approximation, that is, using the UCCSD(T) method with the 6-31G*+diffuse p (ζ = 0.0523) basis set, the longitudinal static γ of PQM presents a maximum value for intermediate diradical character (y ≈ 0.5) while the γ values are larger for intermediate and large diradical character (y ≈ 0.5−0.7) than for small diradical character (y < 0.2). This feature suggests that the γ values of singlet diradical systems in the i...

282 citations

Journal ArticleDOI
TL;DR: This Letter theoretically shows that the third-order NLO properties are drastically enhanced in symmetric open-shell diradical systems with intermediate Diradical character and further reveals that this enhancement is associated with the ferromagnetic and antiferromagnetic interactions.
Abstract: Although most third-order nonlinear optical (NLO) materials are closed-shell singlet systems, this Letter theoretically shows that the third-order NLO properties are drastically enhanced in symmetric open-shell diradical systems with intermediate diradical character and further reveals that this enhancement is associated with the ferromagnetic and antiferromagnetic interactions. This new paradigm opens up a promising area for designing new third-order NLO materials.

244 citations


Cited by
More filters
Journal Article
TL;DR: In this article, a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators were developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of 3D micro-optical and micromechanical structures, including photonic-bandgap-type structures.
Abstract: Two-photon excitation provides a means of activating chemical or physical processes with high spatial resolution in three dimensions and has made possible the development of three-dimensional fluorescence imaging, optical data storage, and lithographic microfabrication. These applications take advantage of the fact that the two-photon absorption probability depends quadratically on intensity, so under tight-focusing conditions, the absorption is confined at the focus to a volume of order λ3 (where λ is the laser wavelength). Any subsequent process, such as fluorescence or a photoinduced chemical reaction, is also localized in this small volume. Although three-dimensional data storage and microfabrication have been illustrated using two-photon-initiated polymerization of resins incorporating conventional ultraviolet-absorbing initiators, such photopolymer systems exhibit low photosensitivity as the initiators have small two-photon absorption cross-sections (δ). Consequently, this approach requires high laser power, and its widespread use remains impractical. Here we report on a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators. Two-photon excitable resins based on these new initiators have been developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of three-dimensional micro-optical and micromechanical structures, including photonic-bandgap-type structures.

1,833 citations

Journal ArticleDOI
TL;DR: In this article, a review of the recent progress in fabricating metal-organic frameworks (MOFs) and MOF-derived nanostructures for electrochemical applications is presented.
Abstract: Metal–organic frameworks (MOFs) have received a lot of attention because of their diverse structures, tunable properties and multiple applications such as gas storage, catalysis and magnetism. Recently, there has been a rapidly growing interest in developing MOF-based materials for electrochemical energy storage. MOFs have proved to be particularly suitable for electrochemical applications because of their tunable chemical composition that can be designed at the molecular level and their highly porous framework in which fast mass transportation of the related species is favorable. In this review, the recent progress in fabricating MOFs and MOF-derived nanostructures for electrochemical applications is presented. The review starts with an introduction of the principles and strategies for designing targeted MOFs followed by a discussion of some novel MOF-derived structures and their potential applications in electrochemical energy storage and conversion. Finally, major challenges in electrochemical energy storage are highlighted and prospective solutions from current progress in MOF-based nanostructure research are given.

1,250 citations

Journal ArticleDOI
TL;DR: Recent progress in the "bottom-up" chemical syntheses of structurally well-defined nanographenes, namely graphene molecules and GNRs are described.
Abstract: Nanographenes, or extended polycyclic aromatic hydrocarbons, have been attracting renewed and more widespread attention since the first experimental demonstration of graphene in 2004. However, the atomically precise fabrication of nanographenes has thus far been achieved only through synthetic organic chemistry. The precise synthesis of quasi-zero-dimensional nanographenes, i.e. graphene molecules, has witnessed rapid developments over the past few years, and these developments can be summarized in four categories: (1) non-conventional methods, (2) structures incorporating seven- or eight-membered rings, (3) selective heteroatom doping, and (4) direct edge functionalization. On the other hand, one-dimensional extension of the graphene molecules leads to the formation of graphene nanoribbons (GNRs) with high aspect ratios. The synthesis of structurally well-defined GNRs has been achieved by extending nanographene synthesis to longitudinally extended polymeric systems. Access to GNRs thus becomes possible through the solution-mediated or surface-assisted cyclodehydrogenation, or “graphitization,” of tailor-made polyphenylene precursors. In this review, we describe recent progress in the “bottom-up” chemical syntheses of structurally well-defined nanographenes, namely graphene molecules and GNRs.

1,031 citations

Journal ArticleDOI
TL;DR: In this paper, a review of magnetic properties of spintronic devices based on carbon nanofragments and graphite is presented, with the help of computational examples based on simple model Hamiltonians.
Abstract: Magnetic materials and nanostructures based on carbon offer unique opportunities for future technological applications such as spintronics. This paper reviews graphene-derived systems in which magnetic correlations emerge as a result of reduced dimensions, disorder and other possible scenarios. In particular, zero-dimensional graphene nanofragments, one-dimensional graphene nanoribbons and defect-induced magnetism in graphene and graphite are covered. Possible physical mechanisms of the emergence of magnetism in these systems are illustrated with the help of computational examples based on simple model Hamiltonians. In addition, this review covers spin-transport properties, proposed designs of graphene-based spintronic devices, magnetic ordering at finite temperatures as well as the most recent experimental achievements.

981 citations