Energy and spectral enhancement of femtosecond supercontinuum in a noble gas using a weak seed

We experimentally demonstrate that the use of a weak seed pulse of energy less than 0.4% of the pump results in a spectral energy enhancement that spans over 2 octaves and a total energy enhancement of more than 3 times for supercontinua generated by millijoule level femtosecond pulses in Krypton gas. Strong four-wave mixing of the pump-seed pulse interacting in the gas is observed. The spectral irradiance generated from the seeding process is sufficiently high to use white-light continuum as an alternative to conventional tunable sources of radiation for applications such as nonlinear optical spectroscopy

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

Generation of broad spectral components from midwave infrared ultrashort pulse laser propagation through ZnSe and ZnS

We investigate the nonlinear optical properties of ZnSe and ZnS using ultrashort (pulse duration approximately 200 fs) midwave infrared laser pulses between 3 and 4 mu m. Multiple harmonic generation in both materials was observed, as well as significant spectral modification of the fundamental pulse. Simulations using a nonlinear polarization model enhanced with ionization compared favorably with experimental data. Random quasi phase matching in the materials is the likely generator of the observed harmonics.SURVICE [S17-095008/DOTC-17-01-INIT0086]; Air Force Office of Scientific Research (AFOSR) [FA9550-16-1-0069]; AFOSR multidisciplinary research program of the university research initiative (MURI) [FA9550-16-1-0013]; AFOSR [FA9550-16-1-0121]This item from the UA Faculty Publications collection is made available by the University of Arizona with support from the University of Arizona Libraries. If you have questions, please contact us at [email protected]

Temporal, Spectral, and Polarization Dependence of the Nonlinear Optical Response of Carbon Disulfide

Carbon disulfide is the most popular material for applications of nonlinear optical (NLO) liquids, and is frequently used as a reference standard for NLO measurements. Although it has been the subject of many investigations, determination of the third-order optical nonlinearity of CS2 has been incomplete. This is in part because of several strong mechanisms for nonlinear refraction (NLR), leading to a complex pulse width dependence. We expand upon the recently developed beam deflection technique, which we apply, along with degenerate four-wave mixing and Z-scan, to quantitatively characterize (in detail) the NLO response of CS2, over a broad temporal range, spanning 6 orders of magnitude (∼32 fs to 17 ns). The third-order response function, consisting of both nearly instantaneous bound-electronic and noninstantaneous nuclear contributions, along with the polarization and wavelength dependence from 390 to 1550 nm, is extracted from these measurements. This paper provides a self-consistent, quantitative picture of the third-order NLO response of liquid CS2, establishing it as an accurate reference material over this broad temporal and spectral range. These results allow prediction of the outcome of any NLR experiment on CS2

Quasi-three-level Model Applied to Measured Spectra of Nonlinear Absorption and Refraction in Organic Molecules

Materials with a large nonlinear refractive index (2) and relatively small linear and nonlinear absorption losses, namely, two-photon absorption (2PA, of coefficient 2), 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 2. We then compare these predictions with experimental measurements of 2 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 2 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 ((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 (3) in regions of transparency.Abstract © 2016 Optical Society of Americ

Engineered nonlinear materials using gold nanoantenna array

Gold dipole nanoantennas embedded in an organic molecular film provide strong local electromagnetic fields to enhance both the nonlinear refractive index (n(2)) and two-photon absorption (2PA) of the molecules. An enhancement of 53x for 2PA and 140x for nonlinear refraction is observed for BDPAS (4,4'-bis(diphenylamino) stilbene) at 600 nm with only 3.7% of gold volume fraction. The complex value of the third-order susceptibility enhancement results in a sign change of n(2) for the effective composite material relative to the pure BDPAS film. This complex nature of the enhancement and the tunability of the nanoantenna resonance allow for engineering the effective nonlinear response of the composite film8119Agências de fomento estrangeiras apoiaram essa pesquisa, mais informações acesse artig

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. © 2013 The Optical Society

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 \u3c 400, making it an excellent candidate for AOS. © 2014 SPIE

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. © OSA 2013