Manuel R. Ferdinandus

Dual-arm Z-scan technique to extract dilute solute nonlinearities from solution measurements

We present a technique in which small solute nonlinearities may be extracted from large solvent signals by performing simultaneous Z-scans on two samples (solvent and solution). By using a dual-arm Z-scan apparatus with identical arms, fitting error in determining the solute nonlinearity is reduced because the irradiance fluctuations are correlated for both the solvent and solution measurements. To verify the sensitivity of this technique, the dispersion of nonlinear refraction of a squaraine molecule is measured. Utilizing this technique allows for the effects of the solvent n2 to be effectively eliminated, thus overcoming a longstanding problem in nonlinear optical characterization of organic dyes.

Beam deflection measurement of time and polarization resolved ultrafast nonlinear refraction

We modify the well-known photothermal beam deflection technique to study ultrafast nonlinearities. Using phase-sensitive detection we directly measure the temporal and polarization dynamics of nonlinear refraction (NLR) with sensitivity to optically induced phase changes of approximately λ/20,000. We use the relative polarization dependence of excitation and probe to separate the isotropic and reorientational components of the NLR.

Quasi-three-level model applied to measured spectra of nonlinear absorption and refraction in organic molecules

Materials with a large nonlinear refractive index (n2) and relatively small linear and nonlinear absorption losses, namely, two-photon absorption (2PA, of coefficient α2), have long been sought after for applications such as all-optical switching (AOS). Here we experimentally determine the linear and 2PA properties of several organic molecules, which we approximate as centrosymmetric, and use a simplified essential-state model (quasi-three-level model) to predict the dispersion of n2. We then compare these predictions with experimental measurements of n2 and find good agreement. Here “quasi”-three-level means using a single one-photon allowed intermediate state and multiple (here two) two-photon allowed states. This also allows predictions of the figure-of-merit (FOM), defined as the ratio of nonlinear refractive phase shift to the 2PA fractional loss, that determines the viability for such molecules to be used in device applications. The model predicts that the optimized wavelength range for a large FOM lies near the short wavelength linear absorption edge for cyanine-like dyes where the magnitude of n2 is quite large. However, 2PA bands lying close to the linear absorption edge in certain classes of molecules can greatly reduce this FOM. We identify two molecules having a large FOM for AOS. We note that the FOM is often defined as the ratio of real to imaginary parts of the third-order susceptibility (χ(3)) with multiple processes leading to both components. As explained later in this paper, such definitions require care to only include the 2PA contribution to the imaginary part of χ(3) in regions of transparency.

Analysis of beam deflection measurements in the presence of linear absorption

We develop a series of analytical approximations allowing for rapid extraction of the nonlinear parameters from beam deflection measurements. We then apply these approximations to the analysis of cadmium silicon phosphide and compare the results against previously published parameter extraction methods and find good agreement for typical experimental conditions.

Quasi-three-level model applied to measured spectra of nonlinear absorption and refraction in organic molecules: publisher’s note

This note corrects author affiliations, errors in one equation, and two equation callouts of J. Opt. Soc. Am. B33, 780 (2016)10.1364/JOSAB.33.000780JOBPDE0740-3224.

Optimization of the Electronic Third-order Nonlinearity of Cyanine- like Molecules for All Optical Switching

All optical switching (AOS) applications require materials with a large nonlinear refractive index (n2) but relatively small linear and nonlinear absorption loss. The figure-of-merit (FOM), defined as the ratio between the real and imaginary parts of the second hyperpolarizability (γ), is widely used to evaluate the operating efficiency of AOS materials. By using an essential-state model, we describe the general dispersion behavior of γ of symmetric organic molecules and predict that the optimized wavelength range for a large FOM is near its linear absorption edge for cyanine-like dyes. Experimental studies are normally performed on organic solutes in solution which becomes problematic when the solvent nonlinearity dominates the total signal. This has been overcome using a Dual-arm Z-scan methodology to measure the solution and solvent simultaneously on two identical Z-scan arms and discriminating their small nonlinear signal difference. This technique significantly reduces the measurement uncertainty by correlating the excitation noise in both arms, leading to nearly an order-of-magnitude increase in sensitivity. Here we investigate the n2 and two-photon absorption (2PA) spectra of several classes of cyanine-like organic molecules and find that the results for most molecules agree qualitatively and quantitatively with the essential-state model. Many cyanine-like molecules show a relatively small FOM due to the presence of large 2PA bands near the linear absorption edge; however, an exception is found for a thiopyrylium polymethine molecule of which the maximum FOM can be < 400, making it an excellent candidate for AOS.

Dispersion of the electronic third-order nonlinearity of symmetric molecules

Using a dual-arm Z-scan to increase the signal-to-noise, we measure the dispersion of the electronic third-order nonlinearity of symmetric polymethines and squaraines and find good agreement with the essential-state model including CS2.

Measuring small solute nonlinearities in solution by dual-arm Z-Scan technique

An ongoing problem in characterizing organic nonlinearities in the presence of large solvent backgrounds can be eradicated by performing identical and simultaneous Z-scans on two samples (solvent and solvent plus solute).