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.

[1]  William T. Lotshaw,et al.  Femtosecond laser-induced optical kerr dynamics in CS2/alkane binary solutions , 1988 .

[2]  Dirk,et al.  Effects of centrosymmetry on the nonresonant electronic third-order nonlinear optical susceptibility. , 1990, Physical review. A, Atomic, molecular, and optical physics.

[3]  Matthew Reichert,et al.  Beam deflection measurement of time and polarization resolved ultrafast nonlinear refraction. , 2013, Optics letters.

[4]  Hervé Leblond,et al.  Robust two-dimensional spatial solitons in liquid carbon disulfide. , 2013, Physical review letters.

[5]  Brian J. Orr,et al.  Perturbation theory of the non-linear optical polarization of an isolated system , 1971 .

[6]  M. Baba,et al.  Nonlinear refraction in CS2 , 2004 .

[7]  N. Peyghambarian,et al.  Integrated liquid-core optical fibers for ultra-efficient nonlinear liquid photonics , 2012, 2012 Conference on Lasers and Electro-Optics (CLEO).

[8]  Reginald C. Farrow,et al.  Microscopic dynamics in simple liquids by subpicosecond birefringences , 1984 .

[9]  Xiao-Liang Zhang,et al.  Third-order nonlinear susceptibility tensor elements of CS2 at femtosecond time scale. , 2011, Optics express.

[10]  Jonathan S. Friedman,et al.  The effects of molecular geometry on the depolarized stimulated gain spectra of simple liquids , 1993 .

[11]  A Novel Technique for the Measurement of Polarization-Specific Ultrafast Raman Responses , 2001 .

[12]  Effect of two-beam coupling in strong-field optical pump-probe experiments , 2013, 1302.3208.

[13]  A. Smirl,et al.  Weak-Wave Retardation and Phase-Conjugate Self-Defousing in Si , 1982 .

[14]  M. Falconieri,et al.  Simultaneous measurement of pure-optical and thermo-optical nonlinearities induced by high-repetition-rate, femtosecond laser pulses: application to CS2 , 1999 .

[15]  Govind P. Agrawal,et al.  Nonlinear Fiber Optics , 1989 .

[16]  C. Kuo,et al.  The transient optical Kerr effect of simple liquids studied with an ultrashort laser with variable pulsewidth , 1996 .

[17]  Ryuji Morita,et al.  Study on Ultrafast Dynamic Behaviors of Different Nonlinear Refractive Index Components in CS 2 Using a Femtosecond Interferometer , 1997 .

[18]  Robert A Norwood,et al.  Mid-IR supercontinuum generation in an integrated liquid-core optical fiber filled with CS 2 , 2014 .

[19]  E. V. Van Stryland,et al.  Numerical modeling of thermal refraction inliquids in the transient regime. , 1999, Optics express.

[20]  Francois Kajzar,et al.  Comparison of Z-scan and THG derived nonlinear index of refraction in selected organic solvents , 2008 .

[21]  D. Milam.  Review and assessment of measured values of the nonlinear refractive-index coefficient of fused silica. , 1998, Applied optics.

[22]  D. J. Hagan,et al.  Kramers-Krönig relations in nonlinear optics , 1992 .

[23]  David J. Hagan,et al.  Purely refractive transient energy transfer by stimulated Rayleigh-wing scattering , 1997 .

[24]  K. Kamada,et al.  Orientational and collision-induced contribution to third-order nonlinear optical response of liquid CS2 , 2000 .

[25]  J. Perry,et al.  Quasi-three-level model applied to measured spectra of nonlinear absorption and refraction in organic molecules , 2016 .

[26]  H. Giessen,et al.  Generalized retarded response of nonlinear media and its influence on soliton dynamics. , 2011, Optics express.

[27]  A. Major,et al.  Broadband characterization of the nonlinear optical properties of common reference materials , 2004, IEEE Journal of Selected Topics in Quantum Electronics.

[28]  H. Purwar,et al.  Collinear, two-color optical Kerr effect shutter for ultrafast time-resolved imaging. , 2014, Optics express.

[29]  E. W. Stryland,et al.  Measurement of nondegenerate nonlinearities using a two-color Z scan. , 1992, Optics letters.

[30]  Theodore A. Litovitz,et al.  Erratum: Rayleigh Scattering: Collisional Motions in Liquids , 1971 .

[31]  Joseph S. Melinger,et al.  Analysis of Intermolecular Coordinate Contributions to Third-Order Ultrafast Spectroscopy of Liquids in the Harmonic Oscillator Limit , 2001 .

[32]  N. T. Hunt,et al.  Polarisation-resolved ultrafast Raman responses of carbon disulfide in solution and microemulsion environments , 2003 .

[33]  C. J. Fecko,et al.  Isotropic and anisotropic Raman scattering from molecular liquids measured by spatially masked optical Kerr effect spectroscopy , 2002 .

[34]  David J. Hagan,et al.  Dual-arm Z-scan technique to extract dilute solute nonlinearities from solution measurements , 2012 .

[35]  E. V. Van Stryland,et al.  Nonlinear optical beam propagation for optical limiting. , 1999, Applied optics.

[36]  Influence of the retarded response on an ultrafast nonlinear optofluidic fiber coupler. , 2011, Optics express.

[37]  N. Bloembergen,et al.  Complex Intensity-Dependent Index of Refraction, Frequency Broadening of Stimulated Raman Lines, and Stimulated Rayleigh Scattering , 1966 .

[38]  Robert L. Carman,et al.  Interferometric Measurements of the Nonlinear Refractive-Index Coefficient Relative to CS, in Laser-System-Related Materials , 1975 .

[39]  William T. Lotshaw,et al.  Femtosecond optical Kerr studies on the origin of the nonlinear responses in simple liquids , 1988 .

[40]  Robert A. Norwood,et al.  Mid-IR supercontinuum generation in an integrated liquid-core optical fiber filled with CS_2 , 2013 .

[41]  Graham R. Fleming,et al.  Heterodyne detected transient grating spectroscopy in resonant and non-resonant systems using a simplified diffractive optics method , 2001 .

[42]  David J. Hagan,et al.  Experiment and analysis of two-photon absorption spectroscopy using a white-light continuum probe , 2002 .

[43]  Samir Sahu,et al.  Nonlinear Material Based All-Optical Parallel Subtraction Scheme: an Implementation , 2012 .

[44]  Mansoor Sheik-Bahae,et al.  Dispersion of bound electron nonlinear refraction in solids , 1991 .

[45]  A. Samoc,et al.  Dispersion of refractive properties of solvents: Chloroform, toluene, benzene, and carbon disulfide in ultraviolet, visible, and near-infrared , 2003 .

[46]  Tan Min Pau,et al.  Genetic structure of the snakehead murrel, Channa striata (channidae) based on the cytochrome c oxidase subunit I gene: Influence of historical and geomorphological factors , 2011, Genetics and molecular biology.

[47]  E. W. Stryland,et al.  Sensitive Measurement of Optical Nonlinearities Using a Single Beam Special 30th Anniversary Feature , 1990 .

[48]  Xueru Zhang,et al.  Nonlinear absorption of CS2 at the wavelength of 400 nm with femtosecond pulses , 2012 .

[49]  Kenji Kamada,et al.  Mechanisms of ultrafast refractive index change in organic system , 2003, SPIE Optics + Photonics.

[50]  S. Shapiro,et al.  Light Scattering from Fluctuations in Orientations of CS 2 in Liquids , 1967 .

[51]  A. Kaplan.  “External” self-focusing of light by a nonlinear layer , 1969 .

[52]  Microscopic origin of the optical Kerr effect response of CS2- pentane binary mixtures , 1998 .

[53]  M. Ziółek,et al.  Determination of the temporal response function in femtosecond pump-probe systems , 2001 .

[54]  K. Duppen,et al.  Time resolved four- and six-wave mixing in liquids. II. Experiments , 1997 .

[55]  Emmanuel Koudoumas,et al.  An experimental investigation of the nonlinear refractive index (n2) of carbon disulfide and toluene by spectral shearing interferometry and z-scan techniques , 2003 .

[56]  Robert R. Alfano,et al.  Optical Kerr effect in liquids , 1979 .

[57]  P. Madden,et al.  LIGHT SCATTERING STUDIES OF MOLECULAR LIQUIDS , 1980 .

[58]  R. Norwood,et al.  Slow light based on stimulated Raman scattering in an integrated liquid-core optical fiber filled with CS2. , 2013, Optics express.

[59]  Honghua Hu.  Third Order Nonlinearity Of Organic Molecules , 2012 .