Hyper-Rayleigh Scattering in Isotropic Solution

Hendrickx, Eric; Clays, Koen; Persoons, André

doi:10.1021/ar960233o

Cited by 228 publications

(230 citation statements)

References 48 publications

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“…While the linear optical properties of metal nanoparticles have been extensively investigated, the potential of these materials for second-order nonlinear optical applications -including secondorder photonics applications ('hyperphotonics') -has been relatively untapped. Second-order molecular nonlinear optical behavior is commonly quantified by reporting components of the first hyperpolarizability tensor b. Hyper-Rayleigh scattering (HRS), or incoherent second harmonic generation (SHG), has emerged over the last decade as a powerful technique to measure b values of species in solution [1]. In isotropic media, conventional coherent SHG is forbidden in the electric dipole approximation [2].…”

Section: Introductionmentioning

confidence: 99%

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Johnson

Hupp

et al. 2002

Chemical Physics Letters

142

109

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The optical frequency doubling properties of silver, copper, and platinum nanoparticles in aqueous solution are studied via hyper-Rayleigh scattering (HRS) spectroscopy. Substantial HRS responses are observed for silver and copper particles. The response is attributed to enhancement due to resonance of the nonlinearly scattered light with the particles' surface plasmon absorption band. Platinum particles, which lack visible-region plasmon absorption, do not display detectable HRS signals. The largest signals from silver particles are observed under conditions of two-photon resonance, qualitatively consistent with the predictions of available theory; smaller yet still impressive signals are observed under pre-and post-resonant conditions. Ó

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Section: Introductionmentioning

confidence: 99%

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Johnson

Hupp

et al. 2002

Chemical Physics Letters

142

109

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“…47,48 Accurate zzz values could be determined by measuring the individual samples in dichloromethane, at five different concentrations and different modulation frequencies, in order to exclude contributions of multiphoton fluorescence from the nonlinear scattering signal. 49,50 The obtained zzz values are listed in Table 8.…”

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confidence: 99%

Substituted 4,4′-Stilbenoid NCN-Pincer Platinum(II) Complexes. Luminescence and Tuning of the Electronic and NLO Properties and the Application in an OLED

et al. 2008

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A series of 4,4′-disubstituted organic-organometallic stilbenes, i.e., the 4′-substituted stilbenoid-NCN-pincer platinum(II) complexes [PtCl(NCN-R-4)] (NCN-R-4 ) [C 6 H 2 (CH 2 NMe 2 ) 2 -2,6-R-4] -in which R ) C 2 H 2 C 6 H 4 -R′-4′ with R′ ) NPh 2 , NMe 2 , OMe, SiMe 3 H, I, CN, NO 2 ) (1-8), were studied for their electronic, electrochemical, and NLO properties. Complex 7 was also chemically oxidized using Cu(II)Cl 2 , yielding the [Pt(IV)Cl 3 (NCN(C 2 H 2 C 6 H 4 -CN-4′)-4)] complex 11. In contrast to 1 and 7, 11 did not show luminescent properties in solution at room temperature. In the solid state (X-ray crystallography) 11 has an overall bent structure, with the pincer moiety and the cyano group beneath the plane of the central double bond. Stilbenoid pincer complex 1 (R′ ) NPh 2 ) was also studied with UV/vis spectroscopy in a series of different solvents. The compound shows an intense low-energy transition band, appearing at a lower energy (λ max ) 374-379 nm) than 2 (R′ ) NMe 2 ), which contains a stronger donor group. The UV/vis absorption data of a selected series of stilbenoid pincer platinum complexes were interpreted in terms of a qualitative orbital model based on DFT and TD-DFT calculations. The trends observed in the transition energies correlate well with the donor/acceptor properties of the substituents. It was shown that the HOMO-LUMO gap of the stilbenoid pincer platinum compounds decreases when going from an electron-neutral group (R′ ) H) toward an electron-donating (R′ ) NMe 2 ) or -accepting (R′ ) NO 2 ) group. The fluorescence properties of 1 were also investigated using fluorescence and laser spectroscopy, showing that the metal center favors nonradiative decay from the excited state to the ground state. For 7 (R′ ) CN), solid-state 13 C CP/MAS NMR measurements were performed, and a value of 1 J( 13 C, 195 Pt) ) 1003 ( 15 Hz was obtained for the C ipso carbon, reflecting π-contributions in the carbon-metal bond. The cyclic voltammetry study on the complexes revealed an irreversible oxidation from Pt(II) to Pt(IV). In general the oxidation potential is influenced by the electronic character of the R′ substituent. The influence of the para R′ substituent on the hyperpolarizability of the compound was investigated using the femtosecond (frequencyresolved) HRS technique. For 1-7 good zzz values were measured ( zzz ranging from (164-1324) × 10 -30 esu) with the highest value for 6 (R′ ) I). The higher zzz values were found for the compounds that contain a low-energy UV/vis absorption band and/or a large absorption coefficient. Donor-acceptor complexes 7 and 8 were successfully applied in an organic light-emitting diode (OLED). In the electroluminescence spectrum of 7 (R′ ) CN) a low-energy emission band was observed at 643 nm. This band also appeared in the solid-state luminescence spectra of 7, however, only at low temperatures (298-15 K). The emission band was assigned to result from a triplet excited state. The present study shows that the introduction of a NCN-pincer platinum fragment ...

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“…The only second harmonic signal from an isotropic fluid (in the absence of any static field) is the much weaker form known as hyper-Rayleigh scattering, involving the sixth rank average [123]; chiral behavior can only arise through the involvement of an M1 or E2 interaction. However, with sum-frequency generation, in which conversion of two dissimilar photons into another occurs,  symmetry can be broken at the E1 3 level, and it is possible to observe not only local molecular ordering [124] but also chiral discrimination [125].…”

Section: Multipole Interference Tensor πmentioning

confidence: 99%

Quantum formulation for nanoscale optical and material chirality: symmetry issues, space and time parity, and observables

Andrews

2018

J. Opt.

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To properly represent the interplay and coupling of optical and material chirality at the photonmolecule or photon-nanoparticle level invites a recognition of quantum facets in the fundamental aspects and mechanisms of light-matter interaction. It is therefore appropriate to cast theory in a general quantum form, one that is applicable to both linear and nonlinear optics as well as various forms of chiroptical interaction including chiral optomechanics. Such a framework, fully accounting for both radiation and matter in quantum terms, facilitates the scrutiny and identification of key issues concerning spatial and temporal parity, scale, dissipation and measurement. Furthermore it fully provides for describing the interactions of structured or twisted light beams with a vortex character, and it leads to the complete identification of symmetry conditions for materials to provide for chiral discrimination. Quantum considerations also lend a distinctive perspective to the very different senses in which other aspects of chirality are recognized in metamaterials. Duly attending to the symmetry principles governing allowed or disallowed forms of chiral discrimination supports an objective appraisal of the experimental possibilities and developing applications.

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Hyper-Rayleigh Scattering in Isotropic Solution

Cited by 228 publications

References 48 publications

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Substituted 4,4′-Stilbenoid NCN-Pincer Platinum(II) Complexes. Luminescence and Tuning of the Electronic and NLO Properties and the Application in an OLED

Quantum formulation for nanoscale optical and material chirality: symmetry issues, space and time parity, and observables

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