Temporal, spectral, and polarization dependence of the nonlinear optical response of carbon disulfide

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 CS 2 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 CS 2 , 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 CS 2 , 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 CS 2 .

Optical limiting properties and z-scan measurements of carbon disulfide at 205 μm wavelength

“…The nonlinear refractive index of CS 2 is measured at 2.05 µm using the z-scan technique [10], and the obtained value of (1.9±0.5)·10 −18 m 2 /W, i.e. (7.2±1.9)·10 −12 esu, for the nonlinear coefficient is in reasonable agreement with previous experiments using similar pulse duration at shorter wavelengths [11,12]. We show that the average nonlinear phase shift is a factor (2 − N −1 ) larger for a multiple-longitudinal mode (MLM) pulse, compared to a single-longitudinal mode (SLM) pulse, where N is the number of longitudinal modes.…”

“…At 2.05 µm wavelength, the refractive index of CS 2 is n 0 = 1.59 [17]. Ganeev et al and Reichert et al present measurements of the nonlinear coefficient of CS 2 for various pulse durations [11,12]. They find that it increases from γ = 3 · 10 −19 m 2 /W (1.1·10 −12 esu) for a pulse duration of 110 fs to 4 · 10 −18 m 2 /W (1.5·10 −11 esu) at a pulse duration of 75 ns.…”

“…The dependence of the nonlinear coefficient on the pulse duration is due to the contribution of different mechanisms on different time scales. For CS 2 these contributions come mainly from bound electrons (femtosecond time scale), molecular reorientation (picosecond time scale), electrostriction (nanosecond time scale), and thermal effects (> 10 ns time scale) [2,12,22].…”

Nondegenerate two- and three-photon nonlinearities in semiconductors

“…We apply our recently developed ultrafast beam deflection (BD) technique [19,29,30] to measure the ND-NLR of several direct-gap semiconductors. The experimental setup and beam geometries are shown in Figure 8(a).…”

Third-harmonic generation at interfaces with femtosecond pulses: self-focusing contribution and nonlinear microscopy

“…Orientational is only constant for pulses much longer than the orientation response time. 75 Hence, it is possible to change the effective nonlinearity of a solvent controlling the pulse duration (chirp) if the orientational response time is in the order of the pulse duration. Here, we propose a study of the self-focusing effect on the THG just changing the pulse duration of the excitation beam.…”