Measurements of the first hyperpolarizabilities of thiophene-based charge-transfer chromophores with hyper-Rayleigh scattering at 1064 and 1907 nm

Wang, C. H.; Woodford, Jeffrey N.; Jen, Alex K.‐Y.

doi:10.1016/s0301-0104(00)00308-6

Cited by 20 publications

(15 citation statements)

References 48 publications

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“…A pronounced two-photon resonance with the charge-transfer (CT) excited state is clearly observed, and also the onset of a second resonance at higher energy is visible (most probably a two-photon resonance with the higher energy excited state also visible in the linear absorption spectrum), as well as a long-wavelength tail in the off-resonance region, converging towards the static value β 0 . Note also that the two-photon resonance is significantly redshifted compared to the linear absorption band, in line with previous observations [17,19,27,30,32,39]. The highest β values are obtained in the most polar solvent acetonitrile, as can be expected for a NLO chromophore at the left hand side in the Bond Length Alternation (BLA) diagram [80,81].…”

Section: Application To the Nonlinear Optical Dye Disperse Redsupporting

confidence: 89%

“…In pioneering papers by Wang and co-workers [14,17,19,27] and more recently also by Shoute et al [10,[20][21][22], the resonance effect on the first hyperpolarizability was observed by performing HRS measurements at a number of different wavelengths. However, these measurements are generally characterized by a very low signal-to-noise (S/N) ratio, which was attributed to the noise of the detector and to intensity fluctuations of the incoming laser pulses [19].…”

Section: Introductionmentioning

confidence: 99%

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Highly sensitive setup for tunable wavelength hyper-Rayleigh scattering with parallel detection and calibration data for various solvents

Campo¹,

Desmet²,

Wenseleers³

et al. 2009

Opt. Express

100

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A very sensitive experimental setup for accurate wavelength-dependent hyper-Rayleigh scattering (HRS) measurements of the molecular first hyperpolarizability beta in the broad fundamental wavelength range of 600 to 1800 nm is presented. The setup makes use of a stable continuously tunable picosecond optical parametric amplifier with kilohertz repetition rate. To correct for multi-photon fluorescence, a small spectral range around the second harmonic wavelength is detected in parallel using a spectrograph coupled to an intensified charge-coupled device. Reliable calibration against the pure solvent is possible over the full accessible spectral range. An extensive set of wavelength-dependent HRS calibration data for a wide range of solvents is presented, and very accurate measurements of the beta dispersion of the well-known nonlinear optical chromophore Disperse Red 1 are demonstrated.

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Section: Application To the Nonlinear Optical Dye Disperse Redsupporting

confidence: 89%

Section: Introductionmentioning

confidence: 99%

Highly sensitive setup for tunable wavelength hyper-Rayleigh scattering with parallel detection and calibration data for various solvents

Campo¹,

Desmet²,

Wenseleers³

et al. 2009

Opt. Express

100

View full text Add to dashboard Cite

show abstract

“…It is reasonable to suppose that such studies will result in optimized structures with responses comparable to the best figures of merit for the vector hyperpolarizability. Figures of merit exceeding 1000 have been observed [34]- [36] for the vector hyperpolarizability. Indeed, our results as indicated in Table I indicate that 2 and 3 figures of merit may be routinely comparable to the 1 component.…”

Section: Device Prospectsmentioning

confidence: 99%

Prospects for chiral nonlinear optical media

Ostroverkhov

Ostroverkhova

Petschek

et al. 2001

IEEE J. Select. Topics Quantum Electron.

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This paper describes the development and optimization of chiral, nonpolar media with large second-order nonlinear optical responses. We employ molecular engineering, quantum-mechanical sum-overstates theory, and measurements of molecular hyperpolarizability by means of Kleinman-disallowed hyper-Rayleigh scattering in order to understand molecular properties. Then we analyze the appropriate arrangement of the chromophores that produce an optimum axial nonlinear optical medium. Chromophores with large Kleinman disallowed traceless symmetric second-rank tensor hyperpolarizabilities can be aligned so as to result in large susceptibilities (2) in structures that lack polar order. We found that 3-shaped chromophores with 2 or similar symmetry are good candidates for these materials, as they can exhibit large second-rank components of the hyperpolarizability tensor. A wide variety of techniques can be used to fabricate bulk materials belonging to the chiral nonpolar symmetry groups and 2. The microscopic chromophore alignment schemes that optimize the nonlinear optical response in such materials are deduced from general symmetry consideration for both molecules and bulk. We also speculate on the possible application of such materials as high-bandwidth spatial light modulators.

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“…͑1͔͒ to decrease with decreasing excitation wavelength, 21 in contradiction to the result given here ͑see Table I͒ and results given elsewhere. [12][13][14][15]22 To account for the experimental observation concerning the change of ␤ 0 with the excitation wavelength, Wang has modified Eq. ͑1͒ by including the vibrational structure in the ground and excited electronic states in the damped TLM and obtained a ␤ dispersion relation as 21…”

Section: Resultsmentioning

confidence: 99%

Dispersion of the first hyperpolarizability of a strongly charge-transfer chromophore investigated by tunable wavelength hyper-Rayleigh scattering

Hsu

Liu

Wang

et al. 2001

The Journal of Chemical Physics

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Two-photon resonant hyperpolarizability of an H-shaped molecule studied by wavelength-tunable hyper-Rayleigh scattering J. Chem. Phys. 133, 244503 (2010); 10.1063/1.3506421Resonant Raman spectra and first molecular hyperpolarizabilities of strongly charge-transfer molecules Hyper-Rayleigh scattering and frequency dependence of the first molecular hyperpolarizability of a strong charge-transfer chromophoreThe first hyperpolarizability ͑␤͒ of a strongly charge-transfer ͑azulenic-barbituric͒ chromophore is measured by hyper-Rayleigh scattering ͑HRS͒ experiment using 11 excitation wavelengths, ranging from 900 nm to 1907 nm. The measured wavelength-dependence of the ␤ value is used to investigate the dispersion relation of the first hyperpolarizability of the charge-transfer chromophore. When excited by the 1064 nm wavelength laser radiation, the experimental HRS spectrum shows a two-photon resonance ͑TPR͒ peak, which does not coincide with the maximum of the linear absorption spectrum. The wavelength dependence of the first hyperpolarizability cannot be explained by an undamped or damped two level model. However, incorporating vibrational motion in the damped two-level model results in a good fit between theoretical and experimentally measured ␤, especially in the vicinity of TPR region.

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Measurements of the first hyperpolarizabilities of thiophene-based charge-transfer chromophores with hyper-Rayleigh scattering at 1064 and 1907 nm

Cited by 20 publications

References 48 publications

Highly sensitive setup for tunable wavelength hyper-Rayleigh scattering with parallel detection and calibration data for various solvents

Highly sensitive setup for tunable wavelength hyper-Rayleigh scattering with parallel detection and calibration data for various solvents

Prospects for chiral nonlinear optical media

Dispersion of the first hyperpolarizability of a strongly charge-transfer chromophore investigated by tunable wavelength hyper-Rayleigh scattering

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