Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

We report an unprecedented result of self‐aggregation of [Pt(L1)Cl] (HL1 = 1,3‐di(5‐carboxy‐2‐pyridyl)benzene) triggered by CO2 in basic aqueous solution. The color of basic aqueous solution containing [Pt(L1)Cl] changes from yellow to blue‐green during the aggregation resulted from a reaction with CO2 in air. Upon CO2 gas bubbling, strong and broad absorption bands of aggregate assigned to the metal‐metal‐to‐ligand charge transfer transition appeared at 701 and 1152 nm. Recrystallization of [Pt(L1)Cl] from Na2CO3 aqueous solution afforded polymorphic crystals of red and blue‐green forms. A single X‐ray crystallography revealed that the red form of crystal consists of a Pt–Pt stacked dimer bridged by CO32– ion and one of the carboxy groups of L1 is deprotonated. An elemental analysis provided evidence that the blue‐green crystal is constructed by linear array consisting of the [Pt(L2)(CO3)]3– (HL2 = 1,3‐di(5‐carboxylate‐2‐pyridyl)benzene) units. The formation process of blue‐green aggregate in aqueous solution was monitored through a transient absorption spectrum, and the absorption of aggregates involved in the spectral change were examined by a global analysis. A singular value decomposition and kinetic analysis provide that there are four species resulted from the self‐assembling reaction in the solution and the maximal degree of aggregation is at least 32‐mer.

DOI： 10.1002/cssc.202301174

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DOI： 10.1021/acs.inorgchem.3c00820

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We report colour/luminescence colour changes of M[Ru(bpy)(CN)₄] crystal (M²⁺ = Ca²⁺, Sr²⁺, and Ba²⁺; bpy = 2,2’-bipyridine). An X-ray crystallographic study reveals the crystals are constructed by linear-chains of {[Ru(bpy)(CN)₄][Ca(H₂O)₅]}_n,...

DOI： 10.1039/d1dt03666a

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DOI： 10.1039/D2DT00368F

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A newly designed Pt(ii) complex showing a variety of emission colors depending on the degree of stacking is capable of sensing chloroform vapor.

DOI： 10.1039/d2dt02360a

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsanm.1c02977

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DOI： 10.1021/acs.jpcb.1c03753

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Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.jpcb.0c09733

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<p>[Ir(tpy)2](PF6)3 (tpy = 2,2’:6’,2’’-terpyridine) dissolved in CH3CN was found to exhibit dual color luminescent emission depending on the excitation wavelength. Specifically, blue and green emissions were obtained with excitation at...</p>

DOI： 10.1039/d1dt00021g

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<p>This work assessed solvent isotope effects on the photoracemization rate and emission lifetime for [Ru(bpy)₃]²⁺ (bpy = 2,2′-bipyridine) in water.</p>

DOI： 10.1039/c9cp06758b

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DOI： 10.1016/j.jlumin.2018.11.042

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DOI： 10.1021/acs.inorgchem.9b00373

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DOI： 10.1039/C9DT00565J

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We found a pseudo-polymorphic crystal of fac-tris(2-phenyl pyridinato-C-2,N)iridium(III) (fac-Ir(ppy)(3)) and hydration of fac-Ir(ppy)(3) in dichloromethane. Slow evaporation of solvent from dichloromethane solution containing fac-Ir(ppy)(3) gave a dark yellow crystal having six waters of crystallization, which were confirmed by FTIR and thermogravimetric analysis (TGA). The hydration of fac-Ir(ppy)(3) was found to proceed slowly in Wet dichloromethane containing similar to 1 x 10(-2) M. With increasing the water content in dichloromethane, the signal at similar to 1.5 ppm in H-1 NMR was split into two peaks, which were assigned to water molecules in bulk solvent and that in hydrated fac-Ir(ppy)(3), respectively, from the measurement of diffusion coefficient (D) using the DOSY technique. Two water molecules were determined to attach to fac-h(PpY)(3) in Wet CH2CI2. (C) 2016 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.poly.2016.12.007

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We synthesized neutral Ru(II) complexes cis-Ru(bpy)(2)(CN)(2) (bpy = 2,2'-bipyridine), cis-Ru(dmb)(2)(CN)(2) (dmb = 4,4'-dimethyl-2,2'-bipyridine), cis-Ru(dbb)(2)(CN)(2) (dbb = 4,4'-di-tertbutyl-2,2'-bipyridine), and cis-Ru(phen)(2)(CN)(2) (phen = 1,10-phenanthroline) and optically resolved them into respective enantiomers using high-performance liquid chromatography with a chiral column. The absolute configuration of enantiomer of cis-Ru(dbb)(2)(CN)(2) was determined by an X-ray crystallography. Upon photoirradiation, the entire enantiomers of the complexes underwent the racemization with considerably slow rates (k = 1 x 10(-6) to 1 x 10(-5) s(-1)) and small quantum yields (phi = 1 x 10(-6) to 1 x 10(-5)). The photoracemization was concluded to proceed via a five-coordinate pyramidal intermediate with the base plane composed of Ru, bidentate polypyridine, and two cyanides and the axial ligand of mono dentate polypyridine. We derived the equations for photoracemization rate and quantum yield by a kinetics analysis of the photoracemization reaction that depended on polypyridine ligand, solvent, temperature, wavelength and intensity of irradiation light, and emission lifetime. From the temperature-dependent photoracemization reaction, the energy gap between (MLCT)-M-3 (metal-to-ligand charge transfer) and (3)d-d* states was estimated as Delta E = 4000-5000 cm(-1), and the energy of invisible (3)d-d* state was estimated to be ca. 20 500 cm(-1), which was in good agreement with that of [Ru(bpy)(3)](2+).

DOI： 10.1021/acs.inorgchem.6b00772

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We prepared enantiomers of chiral Pt-II complexes, Pt(pppb)Cl and Pt(pppb)CN (pppbH=1-pyridyl-3-(4,5-pinenopyridyl)benzene), and measured their CPL (circularly polarized luminescence) spectra for excimer and trimer emission. The contribution of the pinene moiety to CPL was considerably low for the -* emission of the monomer but large for MMLCT (metal-metal-to-ligand charge-transfer) of the excimer and trimer which had a helical structure induced in a face-to-face stacking fashion. The trimer CPL for (+)-Pt(pppb)Cl was larger in intensity than that of excimer CPL; on the other hand, that for (+)-Pt(pppb)CN was opposite in sign compared with that of excimer CPL. We conclude that differences in the excited-state structure of the aggregate between Pt(pppb)Cl and Pt(pppb)CN account for the variation in the CPL spectra. By the aid of TD-DFT calculations it was predicted that the dihedral angle (Cl-Pt-Pt-Cl) was 50-60 degrees or 110-140 degrees for Pt(pppb)Cl aggregates and 160 degrees for Pt(pppb)CN aggregates.

DOI： 10.1002/asia.201500985

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We investigated the luminescence properties and color tuning of [Pt(dpb)Cl] (dpbH = 1,3-di(2-pyridyl) benzene) and its analogues. An almost blue emission was obtained for the complex [Pt(Fmdpb)CN] (FmdpbH = 4-fluoro-1,3-di(4-methyl-2-pyridyl) benzene), modified by the introduction of -F and -CH3 groups to the dpb ligand and the substitution of -Cl by -CN. As the concentration of the solution was increased, the color of the emission varied from blue to white to orange. The color change resulted from a monomer-excimer equilibrium in the excited state. A broad emission spectrum around 620 nm was clearly detected along with a structured monomer emission around 500 nm. Upon further increases in concentration, another broad peak appeared in the longer wavelength region of the spectrum. We assigned the near-infrared band to the emission from an excited trimer generated by the reaction of the excimer with the ground-state monomer. The emission lifetimes of the monomer, dimer, and trimer were evaluated as tau(M) = 12.8 mu s, tau(D) = 2.13 mu s, and tau(T) = 0.68 mu s, respectively, which were sufficiently long to allow association with another Pt-II complex and dissociation into a lower order aggregate. Based on equilibrium constants determined from a kinetic study, the formation of the excimer and the excited trimer were concluded to be exothermic processes, with Delta G(D)* = -24.5 kJ mol(-1) and Delta G(T)* = -20.4 kJ mol(-1) respectively, at 300 K.

DOI： 10.1002/chem.201403789

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The intermolecular interaction and aggregation of the neutral complex fac-tris(2-phenylpyridinato-C-2,N)iridium(III) (fac-Ir(ppy)(3)) in solution was investigated. Intermolecular interactions were found to effectively decrease the luminescence lifetime via self-quenching with increasing fac-Ir(ppy)3 concentrations. A Stern-Vohner plot for quenching in acetonitrile was linear, due to bimolecular self-quenching, but curved in toluene as the result of excimer formation. H-1 NMR spectra demonstrated a monomer-aggregate equilibrium which resulted in spectral shifts depending on solvent polarity. X-ray crystallography provided structural information concerning the aggregate, which is based on a tetramer consisting of two Delta-fac-Ir(ppy)(3)-Lambda-fac-Ir(ppy)(3) pairs. Offset pi-pi stacking of ppy ligands and electrostatic dipole-dipole interactions between complex molecules play an important role in the formation of these molecular pairs.

DOI： 10.1021/jp403974h

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We studied the isotope effect of crystal water on the emission lifetime of Ru(dbb)(2)(CN)(2)center dot 2H(2)O in the solid state. The emission lifetime ratio of Ru(dbb)(2)(CN)(2)center dot 2D(2)O (dbb = 4,4'-di-tert-butyl-2,2'-bipyridine) and Ru(dbb)(2)(CN)(2)center dot 2H(2)O was determined to be tau(D)/tau(H) = 1.14 +/- 0.05 at 298 K. From a crystal structural analysis, it was concluded that hydrogen bonding between crystal water and the 5,5'-and/or 3,3'-H atoms of the dbb ligands contributed more effectively to the isotope effect of crystal water on emission lifetime than that between water and the CN ligands. With increasing temperature, two water molecules were released at 310-345 K and over 385 K stepwise from hydrophobic channels constructed from dbb moieties. Exposure of the non-hydrated crystal, Ru(dbb)(2)(CN)(2), to H2O or D2O vapor at 298 K gave Ru(dbb)(2)(CN)(2)center dot 2H(2)O or Ru(dbb)(2)(CN)(2)center dot 2D(2)O, respectively. Under a H2O-D2O mixed atmosphere, there was no correlation between the ratio of H2O and D2O in crystal water and the statistical distribution of H2O and D2O in the mixed atmosphere. Even under a 70% D2O atmosphere, selective sorption of H2O in the crystal of Ru(dbb)(2)(CN)(2) was observed.

DOI： 10.1039/c3ra23362f

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We investigated polymorphism in [Pt(fdpb) Cl] [Hfdpb = 1,3-bis(5-trifluoromethyl-2-pyridyl)benzene]. The following polymorphs of the complex were crystallized: yellow [Form Y; orthorhombic, Pca2(1), a = 23.4336(14) angstrom, b = 4.6377(2) angstrom, c = 15.7845(9) angstrom, Z = 4], red [Form R; monoclinic, C2/c, a = 21.3619(12) angstrom, b = 13.5629(7) angstrom, c = 13.6974(6) angstrom, beta = 122.301(2)degrees, Z = 8], and dark green [Form G; monoclinic, P2(1)/a, a = 6.7953(4) angstrom, b = 18.2519(12) angstrom, c = 13.5199(8) angstrom, beta = 96.039(2)degrees, Z = 4]. The yellow color of Form Y was due to the influence of stacking on the pi,pi* absorption of the Pt molecule; the red color of Form R originated from a MMLCT absorption due to Pt-Pt interactions in a closely stacked dimer; and the dark green of Form G was attributed to the absorption of a linear array of Pt-II complexes. The polymorphs emitted luminescence at around 550 (Form Y), 670 (Form R), and 750 nm (Form G). Mechanical grinding of the crystals changed the polymorphs from the crystalline to the amorphous phase; the emission spectra of ground samples of Forms Y and R, observed at 750 nm, were identical. When the amorphous solid was heated to around 500 K, the emission spectrum was blueshifted to 670 nm due to a phase transition from amorphous to crystalline. Heating also caused a crystal-crystal transformation; phase transitions from Form G to Form R and Form R to Form Y proceeded at 430-470 and 540-560 K, respectively.

DOI： 10.1002/ejic.201001359

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Adsorption and diffusion behavior of dipolar Ir(ppy)(3) molecules on Cu(111) has been investigated by low-temperature scanning tunneling microscopy (STM). At low coverages, highly dispersed structures of Ir(ppy)(3) are formed on the Cu(111) surface, which result from the repulsive dipole-dipole interactions. The two-dimensional surface diffusion of single Ir(ppy)(3) molecules is directly observed in a temperature range from 65 to 94 K, the hopping rate of which is systematically derived from STM images. We also extract the corresponding activation energy, pre-exponential factor, and jump length for the diffusion of Ir(ppy)(3) on Cu(111).

DOI： 10.1103/PhysRevB.82.155414

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The "solvent effect" on the solid-state luminescence of a neutral complex, [Ru(dbb)(2)(CN)(2)] (dbb = 4,4'-di-tert-butyl-2,2'-bipyridine), was presented. The crystals of this complex showed a variety of luminescence color from orange to dark-red, depending on the acceptor number of the solvent included in the crystal as a solvent of crystallization. The luminescence change was very similar to the solvatochromism in solution, which was attributed to the local donor-acceptor interaction between the CN group and the solvent molecules. The dynamic shift observed in the transient emission spectrum of the crystalline powder was accounted for by the solvent molecule reorganization. X-ray crystallography of [Ru(dbb)(2)(CN)(2)]center dot 3(CH3)(2)CO showed the complex molecule having an approximate C-2 symmetry and very weak interactions between the acetone molecules and the CN groups. A three-dimensional network constructed by acetone molecules was observed in the hydrophobic space consisting of t-butyl groups in dbb ligands. A thin film of the complex showed vapochromic behavior such that the luminescence changed depending on the solvent of crystallization. This suggests a capability for organic molecule discrimination using the complex in the solid state.

DOI： 10.1021/ic9021596

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By using low-temperature scanning tunneling microscopy, we show that long linear chains of Alq(3) are formed on a Cu(111) surface at a temperature of less than 250 K. The linear chains include an identical width, composed of double rows separated by about 0.75 nm, and are enlarged in the [112] direction and its equivalent directions of Cu(111). Above this critical deposition temperature, isolated single molecules are randomly distributed and are very mobile on the surface even at 78 K. The formation of the linear chains should be associated with the metastable adsorption structures of Alq(3) existing only at low temperature.

DOI： 10.1021/jp811454t

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The mechanochemical behavior of Pt(5dpb)Cl (5dpbH = 1,3-di(5-methyl-2-pyridyl)benzene) was investigated in terms of solid-state luminescence. The yellow luminescence of the crystalline complex changed to orange when grinding into. ne powder on a glass substrate with a spatula. A broad emission band, which was not detected for the crystal, was observed at around 670 nm for the powder. The powder X-ray diffraction (XRD) pattern was the same as that calculated from X-ray crystallographic data of the single crystal. A broad band appeared within 100 ns after laser excitation accompanied by quenching of the (3)(pi, pi*) emission of Pt(5dpb)Cl, which was then weakened with decreasing temperature and disappeared below 120 K. The phenomenon was very similar to the excimer formation observed in solution. A related complex, Pt(dpb)Cl (dpbH = 1,3-di(2-pyridyl)benzene), also exhibited luminescent mechanochromism. However, the broad emission that appeared upon grinding still remained at 77 K, and XRD showed that the ground sample of Pt(dpb)Cl was amorphous.

DOI： 10.1039/b811107c

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In the title compound, [ Pt( C18H15N2) Cl], the Pt-II centre adopts a distorted square- planar coordination geometry due to the pincer- type monoanionic N - C - N tridentate ligand. The planar complexes stack via pi - pi interactions to form twodimensional accumulated sheets. This packing pattern is in contrast to that in related pincer- type N - C - N complexes, which exhibit a one- dimensional columnar stacking.

DOI： 10.1107/S0108270107044009

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Highly dispersed superstructures of a dipolar iridium complex are formed on a Cu(111) surface. We show that the dilute superstructures with density-controlled intermolecular separations are stabilized by the strong and long-range repulsive intermolecular interactions. The repulsive intermolecular interactions are quantitatively evaluated by using low-temperature scanning tunneling microscopy, which are characterized by the surface-enhanced dipole-dipole interactions.

DOI： 10.1103/PhysRevLett.98.206102

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：VSP BV  

Transient FT-IR spectra of fac-Re(dmb)(CO)(3)(Et) after laser excitation (355 nm) were investigated in THF under Ar and CO2 atmospheres. The CO stretching bands of Re(dmb(center dot))(CO)(3) (THF) grow (2008 and 1897 cm(-1)) and those of Re(dmb)(CO)(3)(Et) bleach (1987 and 1875 cm(-1)) at times &lt;1 mu s, consistent with clean cleavage of the Re-Et bond. Under a CO2 atmosphere, the long-lived radical (tau &gt;100 ms) converts slowly to the formato complex, Re(dmb)(CO)(3)(OC(O)H) (2020. 1916, 1873 and 1630 cm(-1)). When the solvent is slightly wet, the bicarbonato complex, Re(dmb)(CO)(3)(OC(O)OH), is also observed after photolysis under CO2.

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The radiationless transition rates from metal-to-ligand charge-transfer excited states of [Ru(phen)(3)](2+) (phen = 1,10-phnanthroline) and its analogues were investigated in terms of the Huang-Rhys factors (S) using luminescence measurements and quantum chemical calculations. From the luminescence spectral fitting, it was found that not only S-M for medium frequency mode but also S-L for low frequency mode was significant for the nonradiative process. Huang-Rhys factors predicted by the conventional quantum chemical method were in agreement with the experimental values, S-M and S-L. (c) 2005 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.cplett.2005.10.015

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Neutral ruthenium(II) complexes [RuLL'(CN)(2)] (L, L' = bpy, dmb, dbb; bpy = 2,2'-bipyridine, dmb = 4,4'-dimethyl-2,2'-bipyridine, dbb = 4,4'-tert-butyl-2,2'-bipyridine) were prepared, and the luminescence characteristics of the complexes in the solid state were measured. The luminescence was tuned by crystal waters included in the crystals; for example, [Ru(dbb)(2)(CN)(2)].2H(2)O, [Ru(dbb)(2)(CN)(2)]-H2O, and [Ru(dbb)(2)(CN)(2)] emit luminescence at 640, 685, and 740 nm, respectively.

DOI： 10.1021/ic049169u

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER INST PHYSICS  

A radial pattern is found to form in the polycarbonate (PC) substratum of a recordable compact disk. Characteristic features of the pattern axe that it is composed of about 80 needle-like regions, the shape of which closely resembles a thin film. In addition, white light is found to scatter at the needle-like region/matrix boundaries. This suggests that the PC substratum may have inferior transparency due to the formation of this pattern. Thus, it is important to understand the bifurcation of the radial-pattern formation from the viewpoint of materials science and engineering. Based on the mechanics of the PC viscous fluid, it has been found that the bifurcation of the pattern formation has a Reynolds number of about 10(-3). (C) 2001 American Institute of Physics.

DOI： 10.1063/1.1400778

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Language：English   Publisher：The Chemical Society of Japan  

Photolyses of <i>μ</i>-amido-<i>μ</i>-hyperoxo-dicobalt(III) complexes, [LCo(NH₂,O₂⁻)CoL]⁴⁺ (L = 4NH₃ (<b>1</b>), en + 2NH₃ (<b>2</b>), 2en (<b>3</b>), tren (<b>4</b>)), (tren: 2,2′,2″-triaminotriethylamine, en: ethylenediamine) were investigated. The photolysis of complex <b>4</b> in a neutral aqueous solution produced a <i>μ</i>-hydroxo-<i>μ</i>-peroxo-dicobalt(III) complex, [(tren)Co(OH,O₂²⁻)Co(tren)]³⁺, together with a mononuclear cobalt(III) complex, [Co(NH₃)(tren)(H₂O)]³⁺. A mononuclear complex and Co²⁺ were produced in the photolyses of <i>μ</i>-hyperoxo complexes <b>1</b> and <b>2</b> containing NH₃ ligand in neutral aqueous solutions. In acidic media, only mononuclear complex and Co²⁺ were produced in the photolysis of all <i>μ</i>-hyperoxo complexes examined. Quantum yields of the complexes with NH₃ increased with increasing the number of coordinated NH₃ (<i>φ</i> = 0.25, 0.11, 0.023, and 0.028 for complexes <b>1</b>, <b>2</b>, <b>3</b>, and <b>4</b>, respectively, at 365 nm irradiation in neutral region). The quantum yields obtained in acidic solutions were similar in magnitude to those obtained in neutral solutions.

DOI： 10.1246/bcsj.68.178

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