Determination of resonant and nonresonant third-order nonlinearities of organic molecules by phase-conjugate interferometry

Abstract

We have used a phase-conjugate interferometer to determine the real and imaginary parts of the third-order hyperpolarizability of 3,3'-diethyloxadicarbocyanine iodide (DODCI) and 4-methoxy-4'-nitrostilbene (MONS) at 1064 nm. For DODCI the values are enhanced by a two-photon resonance, and the two-photon extinction coefficient is determined. However, the nonlinear loss of DODCI is dominated by linear absorption from the two-photon excited state. We could not observe linear or nonlinear absorption for the MONS solutions, and we have determined the nonresonant third-order hyperpolarizability for this molecule.

Third-Harmonic Scattering for Fast and Sensitive Screening of the Second Hyperpolarizability in Solution

“… a All values are converted to B-convention, and rescaled with the most recent calibration factor for χ (2) and χ (3) of α-quartz b Phase-conjugate interferometry c Reference determined in this manuscript which can ultimately be traced back to χ (3) of α-quartz (see text). …”

All-optical switching by means of an interferometer with nonlinear frequency doubling mirrors

“…In addition to alloptical switching, a modification of this new nonlinear optical interferometer can be used for measurement of the value of (2) of the media used for frequency doubling, as for the Twyman-Green interferometer with phase conjugation mirrors used for measurement of (3) . [25][26][27]…”

On the third-order nonlinear optical responses of cis and trans stilbenes – a quantum chemistry investigation

“…This technique also probes γ (− ω ; ω , − ω , ω ). 16 When the polarizations of the probe and the pump are parallel, the probed second hyperpolarizability is identical to DFWM:…”

“…Experimentally, recent papers have reported the measurement of the second hyperpolarizabilities using the third-harmonic scattering (THS) technique, 14,15 which has provided a new impetus in calculating these g responses. In addition to THS, other experimental characterization techniques to determine g encompass phase-conjugate interferometry (PCI), 11,16,17 degenerate four-wave mixing (DFWM), electric field-induced second harmonic generation (EFISHG), [18][19][20] and third harmonic generation (THG). 21,22 However, the results obtained with different techniques can be difficult to compare.…”