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

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

Three-Photon Absorption Spectra and Bandgap Scaling In Direct-Gap Semiconductors

This paper presents three-photon absorption (3PA) measurement results for nine direct-gap semiconductors, including full 3PA spectra for ZnSe, ZnS, and GaAs. These results, along with our theory of 3PA using an eight-band Kane model (four bands with double spin degeneracy), help to explain the significant disagreements between experiments and theory in the literature to date. 3PA in the eight-band model exhibits quantum interference between the various possible pathways that is not observed in previous two-band theories. We present measurements of degenerate 3PA coefficients in InSb, GaAs, CdTe, CdSe, ZnTe, CdS, ZnSe, ZnO, and ZnS. We examine bandgap, Eg, scaling using -band tunneling and perturbation theories that show agreement with the predicted Eg−7 dependence; however, for those semiconductors for which we measured full 3PA spectra, we observe significant discrepancies with both two-band theories. On the other hand, our eight-band model shows excellent agreement with the spectral data. We then use our eight-band theory to predict the 3PA spectra for 15 different semiconductors in their zinc-blende form. These results allow prediction and interpretation of the 3PA coefficients for various narrow to wide bandgap semiconductors

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

Beam Deflection Measurements Of Nondegenerate Nonlinear Refractive Indices In Direct-Gap Semiconductors

We use the beam-deflection method to measure nondegenerate nonlinear refractive indices of ZnO and ZnSe and show, in agreement with theory, extremely nondegenerate nonlinear refraction is significantly larger than in the degenerate or near-degenerate case

Seeded Supercontinuum Generation In Gases And Condensed Matter

We measure a fourfold increase in femtosecond supercontinuum integrated spectral irradiance using extremely weak seeding (95010-3) in Kr gas. We present data on the effect of seeding on supercontinuum in other gases, liquids, and solids. © 2011 OSA

Seeded Femtosecond Supercontinua In Various Media

We investigate enhancement of femtosecond supercontinua (SC) in various nonlinear media including solvents by seeding the SC with nanojoule to microjoule visible pulses. Increasing enhancement for decreasing nonlinear refraction is observed. © 2011 OSA

Temporal Dynamics Of Nonlinear Absorption And Refraction In Crystalline And Hydrogenated Amorphous Silicon

We measure the temporal dynamics of nonlinear absorption (NLA) and refraction (NLR) in crystalline and hydrogenated-amorphous silicon at 1550 nm. The effect of relative polarization on NLA and NLR are also reported