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61.
Rodriguez KR Tian H Heer JM Teeters-Kennedy S Coe JV 《The Journal of chemical physics》2007,126(15):151101
The interaction of an infrared surface plasmon and an excited molecular vibration was investigated by using a square array of subwavelength holes in a Ni film which supports propagating, surface-plasmon-mediated, transmission resonances. The largest transmission resonance [the (1,0)(-)] was tuned through the rocking vibration of the hexadecane molecule (at 721 cm(-1)) in a hexadecane film on the mesh by varying the thickness of the film. The interaction of the rocking vibration and surface plasmon is characterized spectroscopically by an increase in the intensity of the vibrational band by more than a factor of 2, variation of the vibrational line shape relative to the spectrum on a nonmetallic surface, and shifts in vibrational peak position by as much as 3.0 cm(-1). Relationships are developed between the transmission resonance position and the thickness and dielectric properties of the coating. 相似文献
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Benjamin J. Coe Stephan Houbrechts Inge Asselberghs Andr Persoons 《Angewandte Chemie (International ed. in English)》1999,38(3):366-369
Low‐energy metal‐to‐ligand charge‐transfer (MLCT) excitations are associated with the very large molecular nonlinear optical (NLO) coefficients, β, of the complexes [RuII(NH3)5(N‐R‐4,4′‐bipyridinium)]3+ (R=methyl, phenyl, or 4‐acetylphenyl). Chemical oxidation to the RuIII forms causes bleaching of the MLCT absorptions and marked attenuation of the NLO responses. Both effects are completely reversed upon re‐reduction, and the extent of the β switching is about 10‐ to 20‐fold. 相似文献
64.
Coe BJ Chamberlain MC Essex-Lopresti JP Gaines S Jeffery JC Houbrechts S Persoons A 《Inorganic chemistry》1997,36(15):3284-3292
A series of new Ru(II) complex salts trans-[Ru(NH(3))(4)(L(1))(L(2))](PF(6))(n) [n = 2, L(1) = 4-acetylpyridine (4-acpy) and L(2) = 4-(dimethylamino)pyridine (dmap) (1), 4-(dimethylamino)benzonitrile (dmabn) (2), 4-picoline (4-pic) (3), or 1-methylimidazole (1-MeIm) (4); n = 3, L(1) = N-methyl-4,4'-bipyridinium (MeQ(+)) and L(2) = dmap (6), dmabn (7), 1-MeIm (8), 4-acpy (9), or phenothiazine (PTZ) (10); n = 2, L(1) = dmap and L(2) = 4-pyridinecarboxaldehyde (pyca) (12) or ethyl isonicotinate (isne) (13)] have been synthesized and fully characterized. These complexes display intense, visible metal-to-ligand charge-transfer (MLCT) absorptions which are highly solvatochromic. An X-ray crystal structure determination has been carried out for trans-[Ru(NH(3))(4)(MeQ(+))(PTZ)](PF(6))(3).Me(2)CO (10.Me(2)CO). This salt, empirical formula C(26)H(38)F(18)N(7)OP(3)RuS, crystallizes in the hexagonal system, space group P6(3), with a = b = 17.853(4) ?, c = 21.514(6) ?, and Z = 6. The MeQ(+) ligand adopts an almost planar conformation, with a torsion angle of 9.6 degrees between the two pyridyl rings. The dipolar cations exhibit a strong projected component along the z axis, but crystal twinning precludes second-harmonic generation. Measurements of the first hyperpolarizability beta by using the hyper-Rayleigh scattering technique at 1064 nm yield very large values in the range (232-621) x 10(-30) esu, the largest being for trans-[Ru(NH(3))(4)(MeQ(+))(dmabn)](PF(6))(3) (7). These beta values are resonance enhanced via the MLCT excitations. A correlation between beta and the MLCT absorption energy confirms that this excitation is the primary contributor to beta. The two-level model yields static hyperpolarizabilities beta(0) in the range (10-130) x 10(-30) esu, with trans-[Ru(NH(3))(4)(MeQ(+))(dmap)](PF(6))(3) (6) having the largest. The beta(0) values of the complexes of the bipyridyl ligand MeQ(+) are larger than those of their analogues containing monopyridyl ligands because of extended conjugation. beta(0) correlates with the MLCT energy only when the MLCT absorption is sufficiently far from the second harmonic at 532 nm. 相似文献
65.
An experimental modification has improved dehydrofluorinations of undeca- deca- and nona- fluoroeyclohexanes, and enhanced the proportions of dienes and aromatics formed. 相似文献
66.
The use of NbCl5, MoCl5, TaCl5 and WCl6 as reagents to effect the replacement by chlorine of the hydroxyl group in cyclohexanol has been investigated. Selective and almost complete conversion of cyclohexanol to cyclohexyl chloride was achieved using WCl6 or TaCl5. The chlorination reactions of cyclohexylmethanol, tetrahydrofurfuryl alcohol, tetrahydropyran-2-methanol and tetrahydro-4H-pyran-4-ol were also investigated. 相似文献
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Coe BJ Jones LA Harris JA Brunschwig BS Asselberghs I Clays K Persoons A 《Journal of the American Chemical Society》2003,125(4):862-863
We have used several techniques, including hyper-Rayleigh scattering and Stark spectroscopy, to investigate the effects of polyene chain length on the optical properties of complexes containing ruthenium(II) electron donor groups and pyridinium electron acceptors. In marked contrast with all other known donor-acceptor polyenes, conjugation extension beyond a single double bond in the dipolar complexes studied leads to blue-shifting of the intramolecular charge-transfer absorptions. Furthermore, the static first hyperpolarizabilities beta0 become maximized with trans-1,3-butadienyl linkages and then decrease in complexes with three CH=CH bonds. Our results clearly demonstrate that the molecular engineering criteria for metal-containing nonlinear optical chromophores can differ dramatically from those for purely organic compounds. 相似文献