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Tachikawa Yasuto,Shiiba Michiharu 한국수자원학회 2000 한국수자원학회논문집 Vol.33 No.S
A TIN, Triagulated Irregular Network, based topographic modeling method and a distributed rainfall-runoff model using the topographic representation is presented. In the TIN based topographic representation, a watershed basin is modeled as a set of contig
Tachikawa, Takashi,Yamashita, Soichiro,Majima, Tetsuro American Chemical Society 2011 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.133 No.18
<P>According to the concept of active sites, the activity of heterogeneous catalysts correlates with the number of available catalytic sites and the binding affinity of the substrates. Herein, we report a single-molecule, single-particle fluorescence approach to elucidate the inherent photocatalytic activity of exposed surfaces of anatase TiO<SUB>2</SUB>, a promising photocatalyst, using redox-responsive fluorogenic dyes. A single-molecule imaging and kinetic analysis of the fluorescence from the products shows that reaction sites for the effective reduction of the probe molecules are preferentially located on the {101} facets of the crystal rather than the {001} facets with a higher surface energy. This surprising discrepancy can be explained in terms of face-specific electron-trapping probability. In situ observation of the catalytic events occurring at the solid/solution interfaces reveals the hidden role of the crystal facets in chemical reactions and their impact on the efficiency and selectivity of heterogeneous (photo)catalysts.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2011/jacsat.2011.133.issue-18/ja201415j/production/images/medium/ja-2011-01415j_0009.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja201415j'>ACS Electronic Supporting Info</A></P>
Tachikawa, Takashi,Cui, Shi-Cong,Fujitsuka, Mamoru,Majima, Tetsuro The Royal Society of Chemistry 2012 Physical chemistry chemical physics Vol.14 No.12
<P>Graphene oxide (GO) nanosheets have received a great deal of attention for a wide range of applications from optoelectronic devices to biological sensors. We now report a mechanistic study of the interfacial electron transfer (ET) processes between organic dye molecule, 9-phenyl-2,3,7-trihydroxy-6-fluorone (PF), and nanometre-sized GO sheets using ensemble-averaged and single-molecule spectroscopies. The ET dynamics was characterized by the direct observation of the PF radical cation during the laser flash photolysis, and its reaction rate was determined to be ∼10<SUP>11</SUP> s<SUP>−1</SUP>. The single-molecule fluorescence spectroscopy was utilized to clarify the heterogeneous nature of the interfacial ET within individual composites. Their fluorescence lifetimes and spectra were found to vary from composite to composite, possibly due to the different local structures and molecular interactions. The autocorrelation analysis of fluorescence intensity trajectories also revealed the temporal fluctuation of the ET reactivity.</P> <P>Graphic Abstract</P><P>Single-molecule spectroscopy revealed the heterogeneous nature of the electron transfer dynamics in individual dye-modified graphene oxide nanosheets. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c2cp23317g'> </P>
Tachikawa, Takashi,Majima, Tetsuro Royal Society of Chemistry 2010 Chemical Society reviews Vol.39 No.12
<P>Nanostructured metal oxide semiconductors, such as TiO<SUB>2</SUB> and ZnO, have attracted great attention as the promising material for photovoltaic devices, photocatalysts for water splitting and environmental purification, sensors, batteries, <I>etc</I>. In this <I>critical review</I>, we have focused on the on-site observation of interfacial chemical reactions involving charge carriers and reactive oxygen species (ROS), such as singlet oxygen and the hydroxyl radical, generated by the photoexcitation of TiO<SUB>2</SUB> nanoparticles using single-molecule, single-particle fluorescence spectroscopy. Advanced fluorescence imaging techniques enable us to determine the location of the photocatalytically active sites that are closely related to the defects heterogeneously distributed on the surface. Consequently, this review provides a great opportunity to understand the temporal and spatial heterogeneities within an individual catalyst particle, allowing for the potential use of single-molecule, single-particle approaches in the analysis of photocatalytic reactions (189 references).</P> <P>Graphic Abstract</P><P>This critical review describes the progress in the single-molecule, single-particle fluorescence imaging techniques for exploring TiO<SUB>2</SUB> photocatalytic reactions. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=b919698f'> </P>
Tachikawa, Yasuto,Shiiba, Michiharu Korea Water Resources Association 2000 한국수자원학회논문집 Vol.33 No.1
A TIN, Triagulated Irregular Network, based topographic modeling method and a distributed rainfall-runoff model using the topographic representation is presented. In the TIN based topographic representation, a watershed basin is modeled as a set of contiguous non-overlapping triagular facets : the watershed basin is subdivided according to streamlines to deal with water movement one-dimensionally ; and each partitioned catchment is approximated to a slope element having a quasi-three-dimensional shape by using cubic spline functions. On an approximated slope element, water movement is represented by combined surface-subsurface kinematic wave equations considering a change of slope gradient and slope width. By using the distributed rainfall-runoff model, the effects of spatial variability of soil properties on runoff response are examined.
Tachikawa, Takashi,Majima, Tetsuro American Chemical Society 2012 Langmuir Vol.28 No.24
<P>In this Article, we focus on the in situ observation of photochemical reactions on individual nanoobjects of solid catalysts using single-molecule, single-particle fluorescence spectroscopy. The use of high-resolution imaging techniques with suitable fluorogenic probes enables us to determine the location of the catalytically active sites that are related to the structural heterogeneities on the surface of the solid catalyst and the temporal fluctuation of photochemical reactivity. Furthermore, we present the real-time observation of metastable gold nanoclusters in polymer matrices at the single-cluster level. This Article encourages readers to explore the nanoworld in terms of practical applications in many fields such as fundamental physics and chemistry.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/langd5/2012/langd5.2012.28.issue-24/la300177h/production/images/medium/la-2012-00177h_0009.gif'></P>
Tachikawa, Takashi,Wang ,, Nan,Yamashita, Soichiro,Cui, Shi‐,Cong,Majima, Tetsuro WILEY‐VCH Verlag 2010 Angewandte Chemie Vol.122 No.46
<P><B>Einzelmolekül‐Fluoreszenzsonde</B>: Über die Bildung der stark fluoreszierenden 4‐NHOH‐Form eines 3,4‐dinitrophenylsubstituierten Bor‐Dipyrromethan‐Farbstoff wird der Elektronentransfer an einzelnen TiO<SUB>2</SUB>‐Partikeln untersucht (siehe Bild; B gelb, C grau, F grün, H weiß, O rot). Kinetische und optische Analysen der Fluoreszenzereignisse geben Aufschluss über die Dynamik der molekularen Wechselwirkungen und die Verteilung der reaktiven Zentren.</P>