Comparative study of electronic and orientational nonlinear refractive indices with nonlinear ellipse rotation measurements

Barbano, E. C.; Souza, Tiago Gualberto Bezerra de; Zílio, Sérgio Carlos; Misoguti, Lino

doi:10.1364/josab.33.000e40

Cited by 6 publications

(8 citation statements)

References 18 publications

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“…In a recent study, our NLO response functions have also been used to interpret the results of mid-infrared supercontinuum generation from CS 2 -core optical fibers, which helps us understand new hybrid soliton dynamics as a result of the noninstantaneous NLR of CS 2 [31,32]. Recently, seven solvents (also included in this work) were studied along with CS 2 using nonlinear ellipse rotation (NER) experiments [33,34] for a range of pulse widths, from which predictions of n 2,eff are given using an empirical model [29]. To open up more possibilities for other materials to be used in NLO applications, we follow the same BD methodology as [20,25] to perform extensive experimental characterizations on the third-order NLO response functions for 24 widely used organic solvents, as listed in Table 1.…”

Section: Introductionmentioning

confidence: 99%

Temporal and polarization dependence of the nonlinear optical response of solvents

Zhao

Reichert

Benis

et al. 2018

Optica

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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.

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Section: Introductionmentioning

confidence: 99%

Temporal and polarization dependence of the nonlinear optical response of solvents

Zhao

Reichert

Benis

et al. 2018

Optica

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“…While, NER signal depends only of B, the Z-scan one depends on both A and B coefficients, for instance. 23,31 As mentioned in previous references, 19,22,23 we have improved the measuring precision of the NER signals by using a phase-sensitive method and also extended the application to thick samples using a short focus lens. 22 For a short focal length, the sample can be probed more locally, and it is possible to measure simultaneously more than one sample in a single run.…”

Section: Nonlinear Ellipse Rotation (Ner) Ner Is a Nonlinear Optical ...mentioning

confidence: 93%

“…Equation considers a pulsed laser with a temporal Gaussian, whose time-averaged intensity is I = I 0 /√2 and a Gaussian beam transverse profile, with I ( z = 0 ) = I /2 . Here, we assume B to be of the pure electronic origin for rhodamine dyes such that the relation with n 2 is given by …”

Section: Methodsmentioning

confidence: 99%

Absolute Nonlinear Refractive Index Spectra Determination of Organic Molecules in Solutions

et al. 2019

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It has been a great challenge to measure the spectrum of pure bound-electronic third-order nonlinear refraction (n 2) of organic chromophores in solutions because of the spurious contribution from the solvent and cuvette walls. In order to circumvent this problem, we present here a new method to obtain a highly accurate absolute n 2 value of organic molecules in solutions with a self-referenced nonlinear ellipse rotation (NER) technique. As a proof of concept, we measured n 2 spectra of two well-known chromophores, rhodamines B and 6G dissolved in methanol, in the range from ∼600 to 1200 nm. Our results pointed out that these two dyes present similar dispersion curves with strong negative nonlinearities near the one-photon absorption band and small positive values at long wavelengths. Furthermore, the negative signal of the dyes can be strong enough to cancel and even invert the positive nonlinear refraction of the solvent (methanol) as the solution’s concentration increases. To understand the n 2 spectrum and its connection to molecular properties of organic chromophores, we employed the sum-over-states (SOS) approach within the few-energy-level model and observed an excellent agreement between the experimental and theoretical spectra. In this way, we believe that, employing our NER technique and the SOS model, it is possible to determine both experimentally and theoretically the absolute magnitude and spectra of pure electronic n 2 for a large variety of other organic molecules.

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“…We found out this proportional factor was already contemplated by the stablished theory, even though it was never highlighted before. 29 This study have opened the possibility to investigate the intricate relationship among the (3) components and how they are related with each physical mechanism that generate NLO phenomena.…”

Section: A New Way Of Evaluatementioning

confidence: 99%

“…28 Furthermore, a comparison of NER and the well-established Z-Scan technique for the study of we explore in deep relationship between the third order susceptibility ( (3) ) elements associated with each effect of those effects. 29 Motivated by the accomplishments obtained using NER to evaluate the solids and solvents 2 , we conjectured the possibility to extend it for gaseous media confined in hollow core fiber (HCF), which opens the opportunity to study NLO properties of this important state of matter, so far weakly explored due the restrictions imposed by their low density.…”

Section: Introductionmentioning

confidence: 99%

Characterization of gases nonlinear refractive index and energetic deep UV generation in hollow core fiber

Souza¹

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I thank the Photonic's group members, for every group meeting and interaction. I have definitely learned a lot. Special thanks goes to my colleague Emerson Cristiano Barbano. Our scientific and personal exchange were among the highest points of my graduation. A man to be remembered. My sincere gratitude to all IFSC-USP community, who has provided a very rich and pleasant environment along all my graduation. As much as I live, I would never forget those days. Standing out, I mention Evandro Ares, a true friend! I thank all my ICFO colleagues, highlighting my host Jens Biegert and my mentor Maurizio Reduzzi during my internship at Attosecond and Ultrafast Optics group. There, I matured my knowledge in nonlinear optics. I am aware my personal debt with my family will never be paid. I hope I can honor them. Fabiola Ferreira de Almeida, my best friend. We grew up together. During the writing of this Thesis, I had one target in mind, the forthcoming students. I wrote for them. I am going to feel realized if they use my accumulated experience to fly higher and further. My work is something to be overcome, it is a step into your Selbstüberwindung. I also thank CAPES for the scholarship, FAPESP and CNPq by financial support. This study was financed in part by the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior-Brasil (CAPES)-Finance Code 001. "The task is not so much to see what no one has seen yet; but to think what nobody has thought yet, about what everybody sees."

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Comparative study of electronic and orientational nonlinear refractive indices with nonlinear ellipse rotation measurements

Cited by 6 publications

References 18 publications

Temporal and polarization dependence of the nonlinear optical response of solvents

Temporal and polarization dependence of the nonlinear optical response of solvents

Absolute Nonlinear Refractive Index Spectra Determination of Organic Molecules in Solutions

Characterization of gases nonlinear refractive index and energetic deep UV generation in hollow core fiber

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