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The mechanism of resonance enhancement of a single harmonic during high-order harmonic generation in indium-, zinc-, and chromium-contained atomic and molecular plasmas is reexamined using single-color and two-color pumps of ablated species. We demonstrate that oxides, selenides, and phosphides of these metals notably reduce the enhancement of a single harmonic compared with purely atomic plasma due to either a shift of the ionic transitions possessing strong oscillator strength out of the wavelength of those harmonics or a reduction of the oscillator strength of these transitions. The role of oscillator strength in harmonic enhancement is discussed and compared with improvements in phase-matching conditions for some harmonics in the region of anomalous dispersion of ionic transitions. The application of different wavelengths of driving pulses drastically changes the enhancement of a single harmonic in indium-contained plasmas. [ABSTRACT FROM AUTHOR]

As high-order harmonic emitters, quantum dots are produced through laser-induced plasmas. Subsequently, we generate high-order harmonics with 800-nm and 30-fs pulses from laser-produced plasmas containing quantum dots of different metal sulfides (Ag2S, CdS, and Cd0.5Zn0.5S). The high-order harmonic generation is analyzed using different approaches, including two-color (800 nm + 400 nm) pump, application of alloyed quantum dots, and quasiphase matching of interacting waves. We discuss the self-phase modulation induced splitting of harmonics, the difference in the application of thick and thin crystals for second harmonic (400 nm) emission during two-color pumping of the quantum dot plasma, the spatial modulation of the quantum dot plasma for quasiphase matching, and the comparison of harmonic yields from monomer and quantum dot plasmas. This study allows us to determine the mechanisms of coherent extreme ultraviolet radiation generation using a few nanometer-sized emitters as well as optimal methods for further enhancing the high-order harmonic generation efficiency. [ABSTRACT FROM AUTHOR]

High-order harmonics generation in the laser-induced plasmas produced on the surfaces of lead-free perovskites is studied. We analyze the harmonics generation in (CH3NH3)2CuCl4 and (CH3NH3)2CuBr4 plasmas during their ablation by the femtosecond, picosecond, and nanosecond pulses. The modifications of the high-order harmonics spectra are studied using the -color pump scheme (800 nm and 400 nm, 40 fs pulses). The influence of the variations of laser chirp and pulse duration on the dynamics of high-order harmonics generation is examined. The spectral shift, chirp-related harmonic cutoff scaling, and the role of the pulse duration of converting and heating laser radiation are examined at different conditions of plasma formation and harmonic generation. The dependencies of the pulse duration and the fluence of heating pulses on the harmonic's blue shift are found. The effect of harmonics broadening and splitting on the two red- and blue-shifted components is demonstrated. [ABSTRACT FROM AUTHOR]

Analysis and characterization of laser-produced plasmas (LPPs) require the advanced methods for determination of different multiparticle component formation and spreading. Time-resolved high-order harmonic generation (HHG) in spreading LPPs allows determining optimal conditions for this process. One of the most important parameters of HHG in LPP is the delay between the heating and driving pulses. We demonstrate that the optimization of delays allows achieving the maximal harmonic yields in LPP created on the surfaces of the solid targets possessing different molar masses (m). The optimal delays (t) for B4C, ZnO, GaP, GaAs, and Ag2S plasmas were determined to be approximately 200, 300, 350, 500, and 700 ns, respectively. These variations of delays correspond to the t∞(m)0.5 dependence for different materials. We demonstrate the applicability of the proposed method for analysis of the resonance-enhanced harmonics in atomic and molecular plasmas (Mo and MoS2) and for studies of large perovskite aggregates as potential emitters of harmonics. This diagnostic technique can also be applied to the analysis of the presence of different nanostructures in LPPs through HHG with a high spatiotemporal resolution. [ABSTRACT FROM AUTHOR]

Thin films containing small-sized quantum dots (QDs) and nanoparticles have shown strong optical nonlinearities caused by the confinement effect. Here, we report the study of third-order optical nonlinearities of silver sulfide (Ag2S) QD thin films using 800 and 400 nm, 30 fs pulses. The absorption spectrometry and transmission electron microscopy are used to characterize the synthesized 80 and 500 nm Ag2S QD films. The giant enhancement of nonlinearities is observed up to three to six orders of magnitude larger compared to those for the bulk and liquid Ag2S samples. We also demonstrate the efficient high-order harmonic generation in the plasmas produced during ablation of the Ag2S QD thin films. The analysis of the dynamics of the QD-containing plasma spreading allowed optimization of the delay between the heating and the driving pulses for an enhancement of harmonics conversion efficiency. [ABSTRACT FROM AUTHOR]

Mixed (FAPbI3)0.92(MAPbBr3)0.08 perovskite thin films exhibit strong nonlinear optical responses, rendering them promising candidates for applications in photonics and optical communications. In this work, we present a systematic study on the ultrafast third-order nonlinear optical processes in mixed perovskite nanocrystals (NCs) by exploring the generation of third harmonic radiation and giant two-photon absorption-based photoluminescence (PL) when excited by femtosecond laser pulses of a 1030 nm central wavelength. A comparative analysis of the coherent third harmonic generation in the thin-film-containing perovskite nanocrystals has shown a 40× enhancement of the third harmonic signal compared to the signal generated in the pure quartz substrate. The cubic dependence of the third-nonlinear optical response of the (FAPbI3)0.92(MAPbBr3)0.08 perovskites on the intensity of the driving radiation was identified using broadband 38 femtosecond driving pulses. The positive nonlinear refractive index (γ = +1.4 × 10−12 cm2·W−1) is found to play an important role in improving the phase-matching conditions of the interacting pulses by generating a strong third order harmonic. The giant two-photon absorption (TPA)-assisted PL peak was monitored and a blue shift of the PL was obtained in the higher intensity range of the laser pulses, with the absorption coefficient β estimated to be~+7.0 cm·MW−1 at a 1030 nm laser wavelength. [ABSTRACT FROM AUTHOR]

Resonance-enhanced harmonics from laser-produced plasma plumes are an interesting phenomenon, whose underlying mechanism is still under debate. In particular, it is unclear whether the macroscopic dispersion properties of the plasma are the key factors for the formation of the enhancement. To shed light on this problem, we perform experiments with two-component plasmas, in which one of the components (tin) is known to be able to generate enhanced harmonics and the other component (lead) is known for altering the overall dispersion properties of the plasma medium. We compare the harmonics spectra from the plasma of pure tin and the plasma of tin/lead alloy. Depending on the driving wavelength, we observe enhanced harmonics at around 47 or 44 nm in both types of plasmas. The two enhanced regions could be attributed to resonances in singly-charged and doubly-charged tin ions, respectively. Our results indicate that the co-existence of lead plasma does not destroy the presence of the enhanced harmonics of tin plasma, and it seems to suggest that the macroscopic properties of the plasma are not the origin of the resonance-enhanced harmonics in tin. [ABSTRACT FROM AUTHOR]

Application of high pulse repetition rate lasers opens the way for increasing the average flux of the high-order harmonics generating in the ions- and nanoparticles-containing plasmas ablated on the surfaces of various metal targets. We demonstrate the harmonic generation of 37 fs, 150 kHz, 1030 nm, 0.5 mJ pulses in different plasmas. The formation of plasma plumes on the surfaces of carbon, titanium, boron, zinc, and manganese targets was performed during laser ablation, using 250 fs pulses from the same laser. The ablation of the mixed powder of boron nanoparticles and silver microparticles was used for generation of harmonics with high yield. Harmonics up to the fortieth orders from the carbon plasma were obtained. The estimated conversion efficiencies in laser-produced plasmas were ≤10−5. The photon flux for a single harmonic generating in carbon plasma was estimated to be 8 × 1013 photons/s. [ABSTRACT FROM AUTHOR]

Gold nanoparticles (NPs) have a wide range of applications in various fields. Here, we present high-order nonlinear optical studies of the plasmas produced from ablation of Au bulk targets and Au NP films deposited on paper and glass substrates. Experimentally, we analyze high-order harmonic generation (HHG) from gold NPs-containing plasmas. The HHG is produced by 35-fs pulses at 800 and 400 nm, while the plasmas are produced by femtosecond (35 fs, 800 nm), picosecond (200 ps, 800 nm), and nanosecond (5 ns, 1064 nm) pulses, respectively. High-order harmonics produced from ablated Au NPs on paper were 40 times stronger than the HHG from that ablated from the Au bulk targets. Through molecular dynamic simulations, we investigate the formation of gold NPs during laser ablation of a metal surface under different conditions. [ABSTRACT FROM AUTHOR]

Gold films are widely used for different applications. We present the results of third- and high-order nonlinear optical studies of the thin films fabricated from Au nanoparticle solutions by spin-coating methods. These nanoparticles were synthesized by laser ablation of bulk gold in pure water using 200 ps, 800 nm pulses. The highest values of the nonlinear absorption coefficient (9 × 10−6 cm W−1), nonlinear refractive index (3 × 10−11 cm2 W−1), and saturation intensity (1.3 × 1010 W cm−2) were achieved using 35 fs, 400 nm pulses. We also determined the relaxation time constants for transient absorption (220 fs and 1.6 ps) at 400 nm. The high-order harmonic generation was studied during propagation of 35 fs, 800 nm pulses through the plasma during the ablation of gold nanoparticle film and bulk gold. The highest harmonic cutoff (29th order) was observed in the plasma containing gold nanoparticles. [ABSTRACT FROM AUTHOR]