Time-resolved hyper-Rayleigh scattering: measuring first hyperpolarizabilities β of fluorescent molecules

Noordman, O.F.J.; Hulst, Niek F. van

doi:10.1016/0009-2614(96)00218-7

Cited by 113 publications

(71 citation statements)

References 13 publications

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“…These dipoles sustain the initial anisotropy of the photoexcitation, thus allowing for the polarization rotation. For instance, long-living pump-induced dipole moments excited via the electrostrictive mechanism [34,35] were found to govern the transient nonlinear-optical response in various dielectric media on the sub-and nanosecond timescale [36][37][38]. This suggestion is further confirmed by the fact that for some measurements the initial offset of the rotation ψ remains for delay times of 1 ns and even longer, see for instance Fig.…”

Section: (B) Illustrates the 180supporting

confidence: 59%

Femtosecond laser-induced optical anisotropy in a two-dimensional lattice of magnetic dots

et al. 2014

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Using pump-probe optical polarimetry we demonstrate that femtosecond laser excitation of a 2D regular lattice of magnetic nanodots effectively changes the optical anisotropy of the array. Study of the dynamics of the femtosecond laser-induced anisotropy reveals four main mechanisms occurring in the electronic, spin, and lattice subsystems. Below 1 ps, a strong Kerr-like nonlinearity causes linear birefringence, with its axis directed along the electric field of the linearly polarized femtosecond laser pump pulse. In addition, a long-living linear birefringence is also induced due to slowly relaxing excitations. Also below 1 ps, ultrafast laser-induced demagnetization of Co leads to a partial breakdown of the circular birefringence of the magnetic nanodots. On the timescale up to 300 ps, optically triggered acoustic modes of the dots drive oscillations of the linear optical birefringence. During this process, the oscillations damp while transferring their energy into acoustic modes of the substrate. On the nanosecond timescale, the signal is dominated by acoustic oscillations at the surface of the substrate.

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Section: (B) Illustrates the 180supporting

confidence: 59%

Femtosecond laser-induced optical anisotropy in a two-dimensional lattice of magnetic dots

et al. 2014

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“…[32] If no attention is devoted to the potential multiphoton fluorescence contribution to the HRS signal, a systematic overestimation of b can result. [33] This systematic error can be avoided by making the distinction between immediate scattering and time-delayed fluorescence in the spectral domain (spectrally broad fluorescence versus sharp scattering at the second-harmonic of the laser line only), in the time domain (a nanosecond fluorescence tail following the femtosecond laser pulse excitation), [34] or in the frequency domain. In the latter approach, the fluorescence is demodulated (diminished in amplitude) and acquires a phase shift with respect to scattering only.…”

Section: Second-order Nonlinear Optical (Hrs) Measurementsmentioning

confidence: 99%

Alkynyl Expanded Donor–Acceptor Calixarenes: Geometry and Second‐Order Nonlinear Optical Properties

Hennrich

Murillo

Prados

et al. 2007

Chemistry A European J

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A number of wide- and narrow-rimmed functionalized alkynylcalix[4]arenes have been synthesized by Sonogashira coupling. With respect to their optical properties, these donor-acceptor systems are treated as ensembles of covalently linked, electronically independent tolane subchromophores. Linear UV/visible and fluorescence spectroscopic investigations revealed that the charge-transfer character of the electronic transitions in calixarenes, and also the second-order nonlinear optical (NLO) properties depend on the electron-withdrawing nature of the terminal ethynylphenyl substituent (NO(2), CF(3), H). The nitro derivatives display high values of the quadratic hyperpolarizability beta. Not only do the (nonlinear) optical properties of the target compounds depend on the number and relative disposition of the subchromophores, but also on the geometry of the calixarenes. In particular, the opening angle of the calixarene cavity can be determined by the substitution pattern of the calixarene scaffold (wide- versus narrow-rim substitution) and the number of the acetylene functions introduced. Both the NLO properties and the conformational issues are conveniently assessed by using hyper-Rayleigh scattering (HRS) in solution, and supported by X-ray crystallography in the solid state.

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“…the use of bandpass filters [12,22] or a scanning monochromator. [62] Also, numerous techniques have been developed to avoid or abstract the TPAF contribution to β: long wavelength measurement, [63Ϫ65] time-resolved HRS, [66] high-frequency demodulation [67] and the measurement of the TPAF spectrum to abstract the fluorescence contribution to the HRS signal. [68,69] The HRS experiments were carried out in CH 2 Cl 2 solution at 1064 nm fundamental wavelength using p-nitroaniline (pNA) as an external reference.…”

Section: Hyperpolarisability Measurementsmentioning

confidence: 99%

Structure−Property Dependence of the First Hyperpolarisabilities of Organometallic Merocyanines Based on the μ-Vinylcarbynediiron Acceptor and Ferrocene Donor

Farrell

Manning

Murphy

et al. 2001

Eur. J. Inorg. Chem.

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In order to investigate the structure−property relationship of nonlinear optical materials, a series of organometallic chromophores were synthesised utilising the [Fe 2 (η-C 5 H 5 ) 2 (CO) 2 (µ-CO)(µ-C−)] + electron-accepting moiety and the ferrocenyl group, Fc, as the electron donor. The π-linker between these two termini was systematically modified and the mutual electronic communication between them was determined using IR, NMR, and electronic absorption spectroscopy. An X-ray structure determination of [Fe 2 (η-C 5 H 5 ) 2 (CO) 2 (µ-CO)(µ-C−CH=CH−CH=C(Cl)−Fc)][BF 4 ] confirmed the strong electronic interaction between the donor and the acceptor with reduced π-bridge bond-length alternation. The nonlinear optical properties of these complexes were examined using the hyper Rayleigh scattering technique. The experimental first hyperpolarisabilities are some of the highest obtained for ferrocenyl chromophores and, significantly, no enhancement

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Time-resolved hyper-Rayleigh scattering: measuring first hyperpolarizabilities β of fluorescent molecules

Cited by 113 publications

References 13 publications

Femtosecond laser-induced optical anisotropy in a two-dimensional lattice of magnetic dots

Femtosecond laser-induced optical anisotropy in a two-dimensional lattice of magnetic dots

Alkynyl Expanded Donor–Acceptor Calixarenes: Geometry and Second‐Order Nonlinear Optical Properties

Structure−Property Dependence of the First Hyperpolarisabilities of Organometallic Merocyanines Based on the μ-Vinylcarbynediiron Acceptor and Ferrocene Donor

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