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Organopalladium(II) boronates represent fundamental pretransmetalation intermediates in Suzuki–Miyaura cross-couplings. These species are typically kinetically unstable, making them particularly elusive. In this study, a range of unprecedented, kinetically stable alkyl-, alkenyl-, allenyl-, and alkynylpalladium(II) boronates were prepared from various Csp3, Csp2, and Cspelectrophiles via a simple, general method. The structures of these complexes were secured by X-ray crystallography, and the chemical competence of a number of these intermediates in transmetalation was demonstrated.

The methyl-migrated bicyclic skeleton of the halimane diterpenes has been found in a wide range of organisms, including flowering plants, liverworts, marine animals, and bacteria. The discovery of halima-1(10),14-dien-13-ol (3) from the Aotearoa New Zealand endemic alpine daisy Celmisia viscosais now reported. The full configuration was assigned for the first time by X-ray crystallography, enantiomeric to that of a liverwort isolate. The absolute configuration at C-5 of the halimane is opposite to that at C-5 of the labdane epimanool (1) found in some C. viscosaspecimens. Two new 2,6-dideoxyhexopyran-3-uloside halimane derivatives (4and 5) were also found, and the absolute configuration of 5was determined by 1H NMR analysis of the Mosher esters. Line broadening in the 13C NMR spectra of these halim-1(10)-enes was due to conformational exchange in the decalin ring A, as shown by molecular modeling and DFT calculations. 1H NMR and GC analyses of leaf extracts of individual plants from across the full geographic range of C. viscosarevealed intraspecific variation of diterpenes: 37 samples had halimadienol as the main diterpene in large amounts and 2 specimens had predominantly epimanool, again in large amounts. Three other viscid (sticky leaved) Celmisiaspecies also contained diterpenes, but none was detectable in four nonviscid Celmisiaspecies.

This report investigates the fundamental basis for rather surprising patterns of reactivity in Brønsted acid-mediated cyclizations of pyrrole substrates bearing pendant Michael acceptors that were identified during syntheses of Stemonaalkaloids. Integrated experimental and theoretical studies reveal the profound influence that substituent effects have on the viability of these transformations. Additionally, we identify that electronic effects, in addition to barrier-lowering secondary orbital interactions within transition states, account for the exclusive preference for 7-endo-trig cyclizations over 6-exo-trig cyclizations.

A rapid and facile method of accessing 4‐phenyl‐β‐keto‐α‐tetralones is reported. The key homo‐Nazarov cyclization was achieved via treatment of the preceding phenylcyclopropane with TiCl4at below ambient temperatures. In contrast to previous work, which was limited to electron‐rich substrates, the present transformations proceeded without heating and were applicable to an electronically broad range of substrates. Furthermore, a mechanistically novel reaction afforded an unexpected γ‐diarylketone as well as a rearranged regioisomer of the expected α‐tetralone. The rapid synthesis ofa series of structurally diverse 2‐acyl‐4‐phenyltetralones is reported. In addition an interesting reaction to produce a γ‐diarylketone was discovered.

This study investigates the mechanism of Suzuki–Miyaura Csp2–Csp2cross-couplings facilitated by PCP-type nickel(II) pincer complexes. By employing a combination of standard experimental and theoretical methods, it is proposed that a nickel(I)/(III) cycle is involved in this reaction and single-electron pathways likely operate in this transformation.

We have identified and extensively investigated the photochemical activation and reaction of a hydroxyquinone-derived phenyliodonium ylide in the presence of visible light using experiment and theory. These studies revealed that in its photoexcited state this iodonium is capable of facilitating a range of single-electron transfer (SET) processes, including hydrogen atom transfer (HAT), a Povarov-type reaction, and atom-transfer radical addition chemistry. Where possible, we have employed density functional theory (DFT) to develop a more complete understanding of these photoinduced synthetic transformations.

A series of electron donor–acceptor compounds are reported in which both the donor and acceptor strengths are systematically altered using mono-, bi-, and terthiophene as donors and benzo[c][1,2,5]thiadiazole (btd), dipyrido[3,2-a:2′,3′-c]phenazine (dppz), and the corresponding rhenium(I) complex, [ReCl(CO)3(dppz)], as acceptors. The electronic properties of the compounds are characterized using electrochemistry, electronic absorbance and emission spectroscopies, and transient absorption spectroscopy. The effect of donor and acceptor strengths on frontier molecular orbital localization and on the charge-transfer (CT) character of optical transitions is modeled using density functional theory (DFT) calculations. The electronic absorption spectra of the compounds investigated are dominated by intraligand charge-transfer (ILCT) transitions, where the CT character is shown to increase across the series from mono- to bi- to terthiophene but not significantly across the acceptor series. Emission is shown to originate from the absorbing state. Long-lived nonemissive states have been observed using transient absorption spectroscopy and assigned using triplet-state DFT calculations, which indicate that the lowest energy excited state has more thiophene-localized π,π* character with an increasing number of appended thiophenes.

The three-component reaction between a resorcinol, 1,3-dimethoxybenzene, and an alkyl aldehyde (R = C1–C11) along with BF3·OEt2affords a C2v-symmetric resorcin[4]arene tetraether in one step; in most cases, the single isomer can be precipitated from the reaction mixture in moderate to excellent yields (up to 89%). The reaction is tolerant of 2-substituted resorcinols (R′ = OH, Cl, Br, Me), allowing a third type of functionality to be regioselectively incorporated during the macrocyclization.

The ground- and excited-state properties of a series of [ReCl(CO)3(dppz)] complexes with substituted donor groups were investigated. Alteration of donor–acceptor communication through modulation of torsional angle and the number and nature of the donor substituents allowed the effects on the photophysical properties to be characterized though both computational and spectroscopic techniques, including time-dependent density functional theory and resonance Raman and time-resolved infrared spectroscopy. The ground-state optical properties show significant variation as a result of donor group modulation, with an increased angle between the donor and acceptor blue-shifting and depleting the intensity of the lowest-energy transition, which is consistently intraligand charge transfer (ILCT) in nature. However, across all complexes studied there was minimal perturbation to the excited-state properties and dynamics. Three excited states on the picosecond, nanosecond, and microsecond time scales were observed in all cases, corresponding to 1ILCT, 3ππ*, and 3ILCT, respectively.

A transition-metal-based donor-(linker)-acceptor system can produce long-lived charge transfer excited states using visible excitation wavelengths. The ground- and excited-state photophysical properties of a series of [ReCl(CO)3(dppz-(linker)-TPA)] complexes, with varying donor and acceptor energies, have been systematically studied using spectroscopic techniques (both vibrational and electronic) supported by computational chemistry. The long-lived excited state is 3ILCT in nature for all complexes studied, characterized through transient absorption and emission, transient resonance Raman (TR2), and time-resolved infrared (TRIR) spectroscopy and TDDFT calculations. Modulation of the donor and acceptor energies results in changes of the 3ILCT lifetime by 1 order of magnitude, ranging from 6.1(±1) μs when a diphenylamine donor is used to 0.6(±0.2) μs when a triazole linker and triphenylamine donor is used. The excited-state lifetime may be rationalized by consideration of the driving force within the framework of Marcus theory and appears insensitive to the nature of the linker.

A rapid and facile synthesis of benzannulated 6,5-spiroketals from vinyl 1,1-diacylcyclopropanes is reported. The method utilizes mild reaction conditions with good to excellent yields and high diastereoselectivity. This methodology was then used to construct the core of berkelic acid.

The synthesis, spectroscopic characterization, and computational modeling of seven benzo[c][2,1,3]thiadiazole-based donor–acceptor dyes is reported. Using a range of linker units, it is possible to alter the lowest energy transition in terms of intensity (from 8000 to 25000 L mol–1cm–1) and wavelength (from 350 to 430 nm). Resonance Raman spectroscopy was used in concert with DFT calculations to indicate that the linker unit participates in charge transfer processes. In each compound the excited state behavior appears to be primarily described by a BTD●–-Linker-TPA●+state. Stokes shift versus solvent parameter gradients are on the order of 15000 cm–1, indicating Δμ values are large. Dual emission is observed in six of the seven compounds and it can be modulated as a function of solvent. TD-DFT calculations, including excited state optimizations (linear response and state specific), indicate that the lowest energy emission is charge transfer in character. The high energy emissive state is assigned as n−π*. In nonpolar solvents, only the low energy charge transfer emission band is observed and this band generally has a high quantum yield (Φ ≈ 0.9). For compounds with phenyl and triazolyl linkers, in polar solvents only the high energy n−π* emission is observed. The high energy n−π* emission has a low quantum yield regardless of solvent.

Various strategies toward the synthesis of the marine natural product (−)-spiroleucettadine are described. In the original strategy, a biomimetic inspired oxidation of a 2-imidazoline scaffold uncovered unexpected reactivity, where benzylic oxidation followed by a Baeyer–Villiger reaction was observed. The second generation approach examined oxidative dearomatization of the phenol ring system first, where a competing spirocyclization process was uncovered. Efforts to forge the scaffold via a carbocation mediated benzyl migration were unsuccessful. Highlights of the successful synthesis include two consecutive hypervalent iodine reactions: the first formed the spirocyclic center and the second facilitated installation of an acetate group at the C-5 position to allow for subsequent introduction of the methyl amine side chain.

A hexa-peri-hexabenzocoronene (HBC)-substituted dipyridophenazine (dppz) ligand (dppz-HBC) and its corresponding rhenium [Re(CO)3Cl] and ruthenium [Ru(bpy)2]2+complexes were synthesized and characterized. The interplay of their various excited states was investigated using spectroscopic and computational techniques. Perturbation of the HBC was seen through a broadening and decreased intensity of the HBC absorption bands that dominate the absorption spectra. A delocalized, partial charge transfer state was shown through emission (520 nm) in the ligand and rhenium complex and is supported by time-dependent density functional theory calculations. Transient absorption measurements revealed the presence of dark states with a triplet delocalized state populated in the ligand, while in the complexes, longer-lived (2.3–2.5 μs) triplet HBC states could be accessed. The properties of the studied ligand and complexes provide insight into the future design of polyaromatic systems and add to the rich history of dppz systems.

A series of Ru(II) 2,2′-bipyridine (bpy) complexes with an electron-accepting dipyrido[3,2-a:2′,3′-c]phenazine (dppz) ligand coupled to an electron-donating triarylamine (TAA) group have been investigated. Systematic alteration of a bridging unit between the dppz and TAA allowed exploration into how communication between the donor and acceptor is perturbed by distance, as well as by steric and electronic effects. The effect of the bridging group on the electronic properties of the systems was characterized using a variety of spectroscopic methods, including Fourier transform–Raman (FT-Raman) spectroscopy, resonance Raman spectroscopy, and transient resonance Raman (TR2) spectroscopy. These methods were used in conjunction with ground- and excited-state absorption spectroscopy, electrochemical studies, and DFT calculations. The ground-state electronic absorption spectra show distinct variation with the bridging group, with the wavelength observed for the lowest energy electronic transition ranging from 449 nm to 522 nm, accompanied by large changes in the molar absorptivity. The lowest-energy Franck–Condon state was determined to be intra-ligand charge transfer (ILCT) in nature for most compounds. The presence of higher-energy metal-to-ligand charge transfer (MLCT) Ru(II) → bpy and Ru(II) → dppz transitions was also confirmed via resonance Raman spectroscopy. The TR2spectra showed characteristic dppz• –and TAA• +vibrations, indicating that the THEXI state formed was also ILCT in nature. Excited-state lifetime measurements reveal that the rate of decay is in accordance with the energy gap law and is not otherwise affected by the nature of the bridging unit.

A series of donor–acceptor compounds is reported in which the energy of the triarylamine donor is systematically tuned through para substitution with electron-donating methoxy and electron-withdrawing cyano groups. The acceptor units investigated are benzothiadiazole (btd), dipyridophenazine (dppz), and its [ReCl(CO)3(dppz)] complex. The effect of modulating donor energy on the electronic and photophysical properties is investigated using 1H NMR spectroscopy, DFT calculations, electrochemistry, electronic absorption and emission spectroscopies, ground state and resonance Raman spectroscopy, and transient absorption spectroscopy. Qualitative correlations between the donor energy and the properties of interest are obtained using Hammett σ+constants. Methoxy and cyano groups are shown to destabilize and stabilize, respectively, the frontier molecular orbitals, with the HOMO affected more significantly than the LUMO, narrowing the HOMO–LUMO band gap as the substituent becomes more electron-donatingobservable as a bathochromic shift in low-energy charge-transfer absorption bands. Charge-transfer emission bands are also dependent on the electron-donating/withdrawing nature of the substituent, and in combination with the highly solvatochromic nature of charge-transfer states, emission can be tuned to span the entire visible region.

The synthesis of two bipyridine-hexa-peri-hexabenzocoronene (bpy-HBC) ligands functionalized with either tBu or C12H25and their Re(I) tricarbonyl chloride complexes are reported and their electronic properties investigated using spectroscopic and computational methods. The metal complexes show unusual properties, and we observed the formation of a long-lived excited state using time-resolved infrared spectroscopy. Depending on the solvent, this appears to be of the form Rebpy•HBC•+or a bpy-centered π,π* state. TD-DFT calculations support the donor–acceptor charge transfer character of these systems, in which HBC is the donor and bpy is the acceptor. The ground state optical properties are dominated by the HBC chromophore with additional distinct transitions of the complexes, one associated with MLCT 450 nm (ε > 17 000 L mol–1cm–1) and another with a HBC/metal to bpy charge transfer, termed the MLLCT band (373 nm, ε = 66 000 L mol–1cm–1). These assignments are also supported by resonance Raman spectroscopy.

Flavonoids acylated on their core phenolic groups are rare. The Aotearoa New Zealand endemic alpine daisy Celmisia viscosais widespread, but its flavonoids have not previously been identified. Leaf extracts yielded a series of 8-O-acylated flavones with combinations of 3-methylbutanoate, 2-methylbutanoate, and 2-methylpropanoate groups and one, two, or three O-methyls, all previously unreported. Regiochemistries of 8-(3″-methylbutanoyl)-5-hydroxy-6,7,4′-trimethoxyflavone (5) and 8-(2″-methylbutanoyl)-5,7,4′-trihydroxy-6-methoxyflavone (10) were defined by X-ray crystallography. LC analyses of leaf extracts from the full geographic range of C. viscosashowed intraspecific variation of these flavones: most had high concentrations of trimethoxy 8-O-acylated flavones, but dimethoxy 8-O-acylated flavones were the most abundant flavonoids in two individuals. Three other viscid (sticky leaved) Celmisaspecies also contained these rare flavones, but four nonviscid Celmisahad none detectable.

A new coordination complex that incorporates discotic ligands oriented orthogonally to a central discotic unit has been synthesized, and images of self-organized structures on highly oriented pyrolytic graphite have been obtained. Scanning tunneling microscopy images show that the combination of the orthogonally disposed discotic components results in significantly different self-organized structures compared to those of the ligand, which contains a single discotic unit.

Palladium and tungsten complexes containing the bifunctional ligand 4-diphenylphosphanylcatechol (L1) have been synthesized. The catecholate functionality strongly binds to titanium dioxide nanoparticles, effectively anchoring the complexes to the TiO2 surface. Solid-state 31P NMR spectroscopy was used to probe the surface-bound compounds. Diffuse reflectance infrared spectroscopy also provided data on surface-bound tungsten carbonyl complexes. Preliminary experiments show that the palladium phosphane complex [PdBr2(L1)2] supported on TiO2 catalyzes the Sonogashira coupling of phenylacetylene with 4-iodonitrobenzene. (© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2005)

The crystallisation and crystal structures of three new crystal forms of MePh₃P+I₃− are described, bringing to four the number of polymorphs of this compound. Crystallisations were from alcohols, mixed alcohols, and dichloromethane, and are reproducible. There are strong similarities between all four of the crystal packing arrangements, which are solvent-free. In all structures the MePh₃P+ cations associate in two-dimensional nets using edge-to-face, offset-face-to-face, and methyl-to-face motifs, and the I₃− ions lie between these nets, with subtle variations in structure caused by sliding displacements of relatively constant cation-anion assemblies. The related compound EtPh₃P+I₃− has very similar crystal packing. The interactions between the I₃− and MePh₃P+ are mainly C–H⋯I, with some phenyl faces parallel to I₃−. The major electrostatic component of the lattice energy is associated with the occurrence of I₃− ions against the faces of nets of cations, consistent with this structural feature being the most invariant aspect of the crystal packing, while the structural variability is associated with the less stabilising cation⋯cation motifs. It appears that these crystals provide a good example of a system where shape is not a dominant feature in crystal packing, and that the tetramorphs represent almost equi-ergic local minima in a relatively deep section of the lattice energy hypersurface. The crystal packing of (MePh₃P+)₂I₈2− is similar.

Substitution of the bromine ligands in [(n-Bu)₄N]₂[Mo₃S₇Br₆] (1) by bidentate ligands such as maleonitriledithiolate (mnt) or oxalate (ox) affords the trinuclear clusters [Mo₃S₇(mnt)₃]2− ([2]2−) and [Mo₃S₇(ox)₃]2− ([3]2−) in moderate yields. The structures of clusters [2]2− and [3]2− have been determined by single-crystal X-ray diffraction as their tetrabutylammonium salts. Cluster 2 forms dimers by interaction of one sulfur atom of the mnt ligand with the anionic binding site of the cluster anion. The structure of 3 reveals the presence of aggregates between the anionic cluster and a Br− ion. The ESI-MS indicate that these cluster–bromine adducts are also present in solution. Electrochemical studies on complexes 1–3 show two irreversible waves associated with reductive cleavage of the disulfido bridges and one or two quasi-reversible oxidation processes for [Mo₃S₇(ox)₃]2− or [Mo₃S₇(mnt)₃]2−, respectively. No oxidation waves have been observed for compound 1 or for its thiocyanate derivative [(n-Bu)₄N]₂[Mo₃S₇(SCN)₆] (4) within the acetonitrile solvent window. The optical limiting properties of the complexes 1–4 have been measured by the Z-scan technique employing 40 ns pulses at 523 nm. Power limiting was observed for clusters 1, 2 and 4, whereas the oxalate derivative 3 was photochemically unstable under our experimental conditions.

Substitution of the bromine ligands in n-Bu4N2Mo3S7Br61 by bidentate ligands such as maleonitriledithiolate mnt or oxalate (ox) affords the trinuclear clusters Mo3S7mnt32−22− and Mo3S7ox32−32− in moderate yields. The structures of clusters 22−and 32−have been determined by single-crystal X-ray diffraction as their tetrabutylammonium salts. Cluster 2forms dimers by interaction of one sulfur atom of the mnt ligand with the anionic binding site of the cluster anion. The structure of 3reveals the presence of aggregates between the anionic cluster and a Br−ion. The ESI-MS indicate that these cluster–bromine adducts are also present in solution. Electrochemical studies on complexes 1–3show two irreversible waves associated with reductive cleavage of the disulfido bridges and one or two quasi-reversible oxidation processes for Mo3S7ox32−or Mo3S7mnt32−, respectively. No oxidation waves have been observed for compound 1or for its thiocyanate derivative n-Bu4N2Mo3S7SCN64 within the acetonitrile solvent window. The optical limiting properties of the complexes 1–4have been measured by the Z-scan technique employing 40 ns pulses at 523 nm. Power limiting was observed for clusters 1, 2and 4, whereas the oxalate derivative 3was photochemically unstable under our experimental conditions.

The complexes [Au(4-CÅflCC6F4OMe)(L)] [L = PMe3 (1), PPh3 (2)],trans-[Ru(4-C=CHC6F4OMe)Cl(dppm)2]PF6(3) and trans-[Ru(4-CÅflCC6F4OMe)Cl(dppm)2](4) have been prepared and the identity of (2) was confirmed by a structural study. Electrochemical data for (3) and (4) suggest that the 4-C6F4OMe group lies midway between Ph and 4-C6H4NO2in electron-withdrawing strength. Quadratic non-linearities at 1064 nm, determined by the hyper-Rayleigh scattering technique, increase for co-ligand variation, in the order PPh3 < PMe3, in proceeding from (2) to (1), whereas data for the vinylidene/alkynyl complexes (3) and (4) are experimentally indistinguishable. The quadratic non-linear optical data for (1) and (2) are comparable to those of their 4-nitrophenylalkynyl analogues, however, (1) and (2) are more optically transparent.

The new phosphines Ph2PC6H4-4-C≡CR [R=SiMe3(1), H (2)] have been used to prepare Ru3(CO)9(Ph2PC6H4-4-C≡CSiMe3)3(4) and Ru(C≡CC6H4-4-PPh2)(PPh3)2(η-C5H5) (3), respectively, the latter with a pendent phosphine. Reaction of 4 with carbonate or fluoride affords Ru3(CO)9(Ph2PC6H4-4-C≡CH)3(5) with pendent terminal alkynyl groups, the identity of which was confirmed by a structural study. Reaction of 5 with [Ru(NCMe)(PPh3)2(η-C5H5)]PF6or reaction of Ru3(CO)12with 3 gives Ru3(CO)9{(Ph2PC6H4-4-C≡C)Ru(PPh3)2(η-C5H5)}3(6). Complexes 3–6 have been studied by cyclic voltammetry. Proceeding from Ru3(CO)12to 4 or 5 shifts the cluster-centred reduction to more negative potential and affords facile cluster-centred oxidation. Proceeding from 4/5 and 3 to 6 results in similarly-located cluster-centred reduction and peripheral ruthenium-centred oxidation, but results in a lack of observable cluster-centred oxidation. Crystal data for 5·C6H14: space group P¯1, a=12.760(1) Å, b=17.077(1) Å, c=17.924(2) Å, α=108.656(5)°, β=96.344(5)°, γ=93.523(5)°, V=3658.4(6) Å3, Z=2, R=0.078, Rw=0.105 for 5008 reflections [I>2.00σ(I)].

Presents the author's views on the utilization of energy resources in Europe. Former Secretary of State Nigel Lawson's opinion on energy resources as a tradable good; Effect of gas, electricity and coal privatization on research and development; Energy as the cornerstone of continuing economic development; Fiscal incentives; Discussions on energy policy.

The three title compounds tri‐μ‐carbonyl‐1:2κ2C;1:3κ2C;2:3κ2C‐octacarbonyl‐1κC,2κ2C,3κ2C,4κ3C‐η5‐methylcyclopentadienyl‐tetrahedro‐triiridiummolybdenum(3 Ir—Ir)(3 Ir—Mo), tri‐μ‐carbonyl‐1:2κ2C;1:3κ2C;2:3κ2C‐octacarbonyl‐1κC,2κ2C,3κ2C,4κ3C‐η5‐tetramethylcyclopentadienyl‐tetrahedro‐triiridiummolybdenum(3 Ir—Ir)(3 Ir—Mo) and tri‐μ‐carbonyl‐1:2κ2C;1:3κ2C;2:3κ2C‐octacarbonyl‐1κC,2κ2C,3κ2C,4κ3C‐η5‐pentamethylcyclopentadienyl‐tetrahedro‐triiridiummolybdenum(3 Ir—Ir)(3 Ir—Mo), [MoIr3(η5‐C5H5−nMen)(μ‐CO)3(CO)8], where n= 1, 4 or 5, have a pseudo­tetrahedral MoIr3core geometry, with a η5‐C5H5−nMengroup ligating the Mo atom, bridging carbonyls spanning the edges of an MoIr2face, and eight terminally bound carbonyls.

The two title compounds, [Mo2Ir2(C6H7)2(CO)10] and [Mo2Ir2(C9H13)2(CO)10]·0.5CH2Cl2, respectively, or collectively [Mo2Ir2(μ‐CO)3(CO)7(η5‐C5H5−nMen)2] (n= 1 or 4), have a pseudo‐tetrahedral Mo2Ir2core geometry, an η5‐­C5H5−nMengroup ligating each Mo atom, bridging carbonyls spanning the edges of an MoIr2face and seven terminally bound carbonyl groups.

In the cation of the title complex, cis,cis,cis‐[Ru(η2‐O2CMe)(dppe)2]PF6·2MeOH [dppe is 1,2‐bis­(di­phenyl­phosphino)­ethane, C26H24P2], the Ru atom is in a pseudo‐octahedral coordination environment with two chelating dppe ligands and one chelating acetate ligand. Intra‐phosphine and intra‐acetate bond lengths and angles are unexceptional. Deviations from idealized octahedral coordination angles at ruthenium [O—Ru—O 59.43 (8)° and P—Ru—P 103.19 (2)°] presumably derive from constraints imposed by the chelate rings. The Ru—P distances for the mutually transP‐donor atoms [2.3785 (6) Å] are significantly longer than those for the Ru—P linkages transto the acetate ligand [2.3074 (6) Å]. The Ru1, C1 and C2 atoms lie on a twofold axis, and atom P3 of the anion lies on an inversion centre.

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