Investigation of Nonlinear Optical Processes in Mercury Sulfide Quantum Dots.

The authors report the third-harmonic generation, nonlinear refraction, and nonlinear absorption in HgS quantum dot (QD) suspensions and films using the nanosecond and femtosecond pulses. High conversion efficiency (7 × 10-4) towards the third harmonic (TH) of the 900-1700 nm, 150 fs laser in the thin (70 nm) films containing HgS QDs deposited on the glass substrates is obtained. The authors analyze spectral dependencies of the TH, nonlinear refractive indices, and nonlinear absorption coefficients of QDs in the 500-1700 nm range and discuss the relation between the TH process and the low-order nonlinear optical properties of these quantum dots.

Nonlinear Optical Characterization of InP@ZnS Core-Shell Colloidal Quantum Dots Using 532 nm, 10 ns Pulses.

InP@ZnS core-shell colloidal quantum dots (CQDs) were synthesized and characterized using the z-scan technique. The nonlinear refraction and nonlinear absorption coefficients (γ = -2 × 10-12 cm2 W-1, ß = 4 × 10-8 cm W-1) of these CQDs were determined using 10 ns, 532 nm pulses. The saturable absorption (ß = -1.4 × 10-9 cm W-1, Isat = 3.7 × 108 W cm-2) in the 3.5 nm CQDs dominated at small intensities of the probe pulses (I ≤ 7 × 107 W cm-2) followed by reverse saturable absorption at higher laser intensities. We report the optical limiting studies using these CQDs showing the suppression of propagated nanosecond radiation in the intensity range of 8 × 107-2 × 109 W cm-2. The role of nonlinear scattering is considered using off-axis z-scan scheme, which demonstrated the insignificant role of this process along the whole range of used intensities of 532 nm pulses. We discuss the thermal nature of the negative nonlinear refraction in the studied species.

Synthesis and low-order optical nonlinearities of colloidal HgSe quantum dots in the visible and near infrared ranges.

We synthesize colloidal HgSe quantum dots and characterize their nonlinear refraction and nonlinear absorption using a Nd:YAG laser and its second harmonic. The 7.5 nm quantum dots were synthesized using the hot-injection method. The nonlinear absorption (ß = 9×10-7 cm W-1) and negative nonlinear refraction (γ = -5×10-12 cm2 W-1) coefficients of colloidal quantum dots were determined using the 10 ns, 532 nm laser radiation. The joint influence of above processes was realized at a higher intensity of probe pulses. In the case of 10 ns, 1064 nm radiation, only negative nonlinear refraction dominated during z-scans of these quantum dots. The studies of optical limiting using two laser sources demonstrated the effectiveness of this process at 532 nm. The role of nonlinear scattering is analyzed. We discuss the mechanisms responsible for the nonlinear refraction processes in colloidal HgSe quantum dots.

Effective high-order harmonic generation from metal sulfide quantum dots.

In the past, common media for high-order harmonic generation (HHG) has been atoms and molecules. More recently, clusters, and nanoparticles have been introduced as HHG emitting media. Multi-particle media can enhance HHG yields but have more stringent requirements in determining the optimal parameters. Here, we demonstrate, for the first time, the effective application of 1-3 nm metal sulfide quantum dots (QDs) for harmonic generation in the 20 - 115 nm extreme ultraviolet range. We report on the syntheses, ablation of Ag2S, CdS, and ZnS QDs, and HHG from laser-produced plasmas by using single- and two-color pumps. We compare HHG efficiency from the ablated QDs to that of bulk metal sulfides and show a seven-fold increase in harmonic yields. Further, the study also allows us to understand the effects of QD-contained plasma spreading dynamics on HHG yield.