Influence of solvent contribution on nonlinearities of near infra-red absorbing croconate and squaraine dyes with ultrafast laser excitation (original) (raw)

Temporal and polarization dependence of the nonlinear optical response of solvents

Optica

It has long been known that nonlinear refraction in solvents can depend on pulse width, and this along with experimental uncertainties has led to orders-of-magnitude disagreements in nonlinear refractive coefficients reported in the literature. To resolve this issue, we perform beam-deflection (BD) measurements of the rigorously defined nonlinear impulse response function for 24 commonly used solvents selected from various classes of molecules. Using this polarization-resolved BD, the bound-electronic and the three major nuclear contributions are separately measured by determining the magnitudes, symmetry, and temporal dynamics of each mechanism. This allows us to construct the response functions that we use to accurately establish self-consistent references for predicting and interpreting the outcomes of other experiments performed on these materials over the temporal range from 10 fs to 1 ns. The results also provide insight into relating solvent nonlinearities with their molecular structures and exploring the effects of the Lorentz-Lorenz local field. We find that nonconjugated molecules with small polarizability anisotropy exhibit negligible reorientational response, and hence the nonlinear refraction is almost independent of pulse width. Knowledge of the response functions also allows engineering the transient nonlinear refractive properties of solutions of organic dyes, for example, materials with effectively zero nonlinear refraction.

Ultrafast third order nonlinearities of organic solvents

Optics Express, 2015

The third order nonlinear optical parameters of a variety of organic solvents are determined under picosecond and femtosecond laser irradiation. Z-scan measurements have been carried out at 35 ps, 532 nm and at 40 fs, 800 nm, while Optical Kerr Effect studies were performed at 35 ps, 532 nm. The target of the present work is to provide a reference of the nonlinear optical response of various widely used organic solvents under the same experimental conditions and render feasible the direct comparison between their nonlinearities.

Dispersion of the complex cubic nonlinearity in two-photon absorbing organic and organometallic chromophores

Photonics: Design, Technology, and Packaging III, 2007

There is much interest in nonlinear absorbing chromophores for applications in photonics, nanophotonics and biophotonics. We have performed studies of dispersion of the nonlinear absorption cross sections and the refractive nonlinearities of organic and organometallic nonlinear chromophores using the technique of Z-scan, with a tunable amplified femtosecond laser system. Z-scan is less sensitive than the popular technique of two-photon induced fluorescence but has advantages of being suitable for non-fluorescent substances and providing information on both absorptive and refractive nonlinearities. We have analysed the experimental results in terms of simple models and using the Kramers-Kronig transformation as shown in this paper for Coumarine 307 and an organometallic dendrimer. The dispersion curves are often dominated by two-photon resonances but inclusion of other nonlinear mechanisms seems to be necessary for better understanding of their features.

Solvent Effects in the Determination of the Nonlinear Optical Properties

Journal of Nonlinear Optical Physics & Materials, 2008

The interaction between a two-level molecular system and a high intensity electric field under the influence of a solvent was analyzed through the OSBE. To solve these equations, the average of the coherence was performed, using a generalized Lorentzian approximation for the Voigt's function as a probability distribution. Applying the convolution theorem, we were able to find an analytical expression for the coherence, from which we calculate optical properties, such as the absorption coefficient, refractive index and emitted signal intensity. In this contribution, we show numerical results for these properties, calculated for a standard model of organic colorants, Green Malaquite.

Nonlinear Optical Properties of Water-Soluble Polymeric Dyes with Biological Applications

Macromolecules, 2000

The nonlinear optical properties of two water-soluble polymeric dyes, poly(R-478) (an anionic anthraquinone dye) and poly(S-119) (an anionic azo dye), are investigated utilizing nanosecond and femtosecond optical techniques such as z-scan, nonlinear transmission, and time-resolved luminescence. Poly(R-478) showed large nonlinear refraction when studied with femtosecond laser pulses at 800 nm, with a value for the intensity-dependent refractive index (n I) of 1.26 × 10-4 cm 2 /GW. The thin film result at 1064 nm indicated a large nonlinear absorption in both polymeric dyes. The origin of the large fast optical nonlinearities in the polymeric system S-119 was investigated by probing the different functional groups of the polymer. The chromophore group (Sunset Yellow) of the S-119 polymer showed a smaller nonlinear response when compared to the polymer result. Significant differences in the electronic dynamics between the parent poly(S-119) and the chromophore Sunset Yellow were observed by time-resolved luminescence spectroscopy. The applications of the NLO effects in these polymers are demonstrated for laser ablation of A549 lung carcinoma cells.

Single-beam Z-scan measurement of the third-order optical nonlinearities of triarylmethane dyes

Laser Physics, 2008

Solid-state dye-doped polymers are an attractive alternative to the conventional liquid-dye solutions. The search for new materials which have potential application in optoelectronic devices has lead us to probe the organic dyes. The solid state being a better medium when compared to a liquid medium has lead to the incorporation of dyes in the polymer matrix. The study of nonlinear characteristics of dyes in polymeric media is essential for developing such potential application devices. In this paper, the third-order nonlinear optical properties of three dyes from the Triarylmethane family were measured in 1-Butanol and in dye-doped polymer films by the Z-scan technique using a cw diode-pumped Nd:YAG laser at 532 nm. The Z-scan technique has also been used to present the observation of a nonlinear refractive index resulting from the photochromism of one of the dyes. These materials exhibit a large negative optical nonlinearity resulting due to the thermal effect. The relative contributions from the nonlinear absorption (NLA) and nonlinear refraction (NLR) are dependent on the chemical structure and linear absorption of the dyes. The dyes exhibited a nonlinear refractive coefficient n 2 , a nonlinear absorption coefficient β , and susceptibility χ (3) on the order of 10 -8 cm 2 /W, 10 -4 cm/W, and 10 − 6 esu, respectively, in both liquid and solid media. The results show that these dyes have potential applications in nonlinear optics.

Investigating the effects of intermolecular interactions on nonlinear optical properties of binary mixtures with high repetition rate femtosecond laser pulses

Peer J Physical Chemistry, 2022

Measurements of nonlinear optical (NLO) properties of different binary mixtures having carbon disulfide (CS 2) as the common component, namely CS 2-acetone, CS 2cyclopentanone, CS 2-toluene, and CS 2-carbon tetrachloride (CCl 4), are carried out by using the z-scan technique. Open-aperture z-scan (OAZS) and close-aperture z-scan (CAZS) experiments are performed to determine the nonlinear absorption coefficient (β) and nonlinear refractive index (n 2) of all binary liquid mixtures at various compositions of the components by employing a pulsed, high repetition rate (HRR) femtosecond laser. Also, we were able to use the flowing liquid to measure NLO properties in the CS 2-acetone binary mixture to remove the cumulative thermal effects produced due to the pulsed HRR laser light. Nonlinear refractive index (n 2) values are found to be influenced by the weak dipole-induced dipole intermolecular interactions between the nonpolar CS 2 and polar acetone as well as cyclopentanone of the respective binary mixtures. On the contrary n 2 values are not found to be affected by the intermolecular interactions in CS 2-toluene and CS 2-CCl 4 binary mixtures. In comparison, the nonlinear absorption coefficient (β) values are not found to be affected by the same in all different sets of binary mixtures.

Characterization of the ultrafast nonlinear response of new organic compounds

Organic Photonic Materials and Devices XXII, 2020

Here, we present our development of several experimental methods, which, when applied together, can provide a thorough characterization of the nonlinear refraction and absorption properties of materials. We focus mainly on time-resolved methods for studying both transient absorption and refraction that reveal molecular dynamics including excited-state absorption, singlet-triplet transfer, instantaneous electronic nonlinear refraction, and molecular reorientation. In particular, we will describe our recent studies of new materials including organometallic compounds and organic solvents such as Tetrachloroethylene (C2Cl4).

Z-scan studies and optical limiting of nanosecond laser pulses in neutral red dye

Optics and Laser Technology, 2008

The nonlinear optical absorption, refraction and optical limiting behaviour of an organic dye, neutral red, were investigated under excitation with nanosecond laser pulses at 532 nm. The nonlinear optical responses of the material were studied both in solution and solid film, made in methanol and polyvinyl alcohol, respectively, using single-beam Z-scan technique. The open aperture Z-scans of the solution samples displayed a switch over from saturable absorption to enhanced absorption with increase in input intensity. Theoretical fit to the experimental data indicated that the dominant mechanism of nonlinear absorption is two-photon absorption. The closed aperture Z-scans of both the samples denoted positive nonlinearity, which was three orders larger in magnitude in solid film, compared with that in solution. The results of optical limiting experiments revealed that neutral red exhibited strong optical limiting of nanosecond laser pulses with a threshold lower than that of C 60 in toluene. r