Abstract
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.
Highlights
Carbon disulfide (CS2) is a widely used nonlinear optical (NLO) liquid owing to its large third-order nonlinear refraction (NLR)
It has been subject to many experimental studies utilizing time-resolved techniques such as optical Kerr effect (OKE) [1,2,3,4,5,6,7,8], degenerate four-wave mixing (DFWM) [9,10], and nonlinear interferometry [11], as well as frequency domain light scattering [12,13,14], third-harmonic generation [15], and Z-scan [16,17,18,19,20,21]
By the application of several measurement techniques, we have experimentally investigated the third-order NLO response of CS2 to give a complete picture of its temporal, polarization, and spectral dependence
Summary
Reports of quantitative measurements of NLR, using absolutely calibrated techniques (such as Z-scan), only pertain to specific pulse widths and wavelengths, and are limited in applicability. By applying our newly developed beam deflection (BD) technique [35], we measure the third-order temporal response function, including the absolute magnitude and symmetry of each component, without a need to scale to a reference material. We determine the dispersion of NLR, including both bound-electronic and nuclear contributions, and the spectrum of 2PA from 390 to 1550 nm. These data give a self-consistent, quantitative picture of the third-order nonlinear dynamics of liquid CS2, making possible a prediction of the outcome of any measurement of 2PA or NLR
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