ABSTRACT
In this work, we systematically explore the third-order nonlinear optical properties of all-inorganic CsPbX3 (X = Cl, Br, I) perovskite precursor solutions and thin films using femtosecond and nanosecond laser pulses. We show that these samples possess strong two-photon absorption (TPA) and reverse saturable absorption (RSA), which depend on the excitation wavelength. The obtained nonlinear absorption and refraction coefficients for precursor solutions are followed by the relation CsPbCl3 > CsPbBr3 > CsPbI3 for the 800 and 1,064 nm excitation wavelengths, whereas this relation became reverse in the case of 355 and 400 nm laser pulses. It was shown that CsPbCl3 thin film possesses RSA at 400 nm, CsPbCI3 shows RSA+ saturable absorption (SA), and CsPbBr3 demonstrates SA + RSA. In addition, at 800 nm excitation, the CsPbBr3 thin films show SA + RSA at low peak intensity, and the absorption becomes reverse (TPA+SA) with a further increase in the input laser intensity. The suitability of nonlinear absorption depends on the band gap of the thin films with respect to the pumping photon energy. Our studies demonstrate that these perovskites can be used as the excellent materials for the all-optical signal processing.
ABSTRACT
Mixed-halide perovskite materials (MHSCs) hold significant interest in photonics applications owing to their inherent advantages, including tunable bandgap properties, remarkable defect tolerance characteristics, and facile processability. These attributes position MHSCs as up-and-coming materials for various applications. However, the commercialization of these materials is severely affected by external factors, such as humidity and oxygen. The current work studies change in higher harmonics generation (HHG) in MAPbBr3-xClx single crystals (MHSC) with changing nitrogen-based additives. These additives act as a passivating layer and improve the nanolevel crystallinity. The additive engineering strategy impacts morphological and optical properties, depending on the additive's interaction.
ABSTRACT
Mixed halide perovskite (MHP) materials are promising candidates for photonic applications, owing to their tunable bandgap and pronounced optoelectronic properties. However, phase segregation in these materials severely impacts their scalability. The additive engineering (AE) strategy in the growth of most perovskite crystals (PSCs) has proven more effective. Current work focused toward enhancing the stability of 6.67% Cl-doped methylammonium lead(II) bromide single crystals (MHSCs) using aromatic nitrogen-based additives. Modified MHSCs showed enhanced terahertz (THz) radiation transmission and reflection. Moreover, the evidence from powder X-ray diffraction (p-XRD), X-ray photoelectron spectroscopy (XPS), and THz transmission in modified MHSCs revealed the mitigated phase segregation in modified MHSCs.
ABSTRACT
The transition metal dichalcogenides have instigated a lot of interest as harmonic generators due to their exceptional nonlinear optical properties. Here, the molybdenum disulfide (MoS2) molecular structures with dopants being in a plasma state are used to demonstrate the generation of intense high-order harmonics. The MoS2 nanoflakes and nickel-doped MoS2 nanoflakes produced stronger harmonics with higher cut-offs compared with Mo bulk and MoS2 bulk. Conversely, the MoS2 with nickel nanoparticles and carbon nanotubes (MoS2-NiCNT) produced weaker coherent XUV emissions than other materials, which is attributed to the influence of phase mismatch. The influence of heating and driving pulse intensities on the harmonic yield and cut-off energies are investigated in MoS2 molecular structures. The enhanced coherent extreme ultraviolet emission at ~32 nm (38 eV) due to the 4p-4d resonant transitions is obtained from all aforementioned molecular structures, except for MoS2-NiCNT.
Subject(s)
Nanotubes, Carbon , Transition Elements , Nickel , Molybdenum , Heart RateABSTRACT
Organometallic lead bromide and iodide perovskite single crystals (PSCs) are potential candidates for terahertz applications. Herein, we performed terahertz time-domain spectroscopy (THz-TDS) in the frequency range of 0.1-3.0 THz on different thicknesses of MAPbBr3 (0.3, 0.6, and 0.8 mm) and MAPbI3 (0.6, 0.8, 0.9, 1.3, and 2.3 mm). The measurements were carried out with respect to the position (along the focal area), azimuthal rotation of the PSCs, and incidence angles of the reference THz pulse on the PSCs' surface. Based on the transmitted THz pulses from PSCs from the above measurements, we calculated the real and imaginary parts of the refractive index, dielectric constants, absorption coefficients, and dark conductivity. These optical parameters tend to increase with decreases in the PSCs' thicknesses. The transmission spectra of the terahertz electric field indicate that the measured optical properties do not vary significantly with the position and orientation of PSCs. The real parts of the refractive index and dielectric constants are higher than the imaginary values for both PSCs. On the other hand, a slight blueshift in the optical phonon vibrations corresponding to Pb-Br/I-Pb and Pb-Br/I bonds is observed with an increase in thickness. Interestingly, the phonon vibrations do not vary with the incidence angle of the THz pulses on the same crystal's surface. The optical parameters based on THz-TDS reveal that the PSCs satisfy the requirement for tunable THz devices which need suitable, sensitive, and stable absorption properties between 0.1 and 3 THz.
ABSTRACT
Carbon-containing plasma is an attractive medium for generation of harmonics of laser pulses in the extreme ultraviolet range. We ablate two metal carbide (B4C and Cr3C2) nanoparticles and silicon carbide (SiC) nanoparticles and generate harmonics after propagation of 35 fs pulses through the laser-induced plasmas. We analyze the spectra, spectral shifts, and splitting of harmonics from nanoparticles-contained plasmas, which demonstrate the chirp-related harmonic cut-off scaling. In addition, we present the simplified two-color pump model calculations of HHG based on the strong field approximation.
ABSTRACT
We demonstrate high-order harmonic generation in Ni-doped CsPbBr3perovskite nanocrystals ablated by nanosecond pulses using chirp-free 35 fs, and chirped 135 fs pulses in the case of single-color pump (800 nm) and a two-color pump (800 and 400 nm). We analyzed the spectral shift, cut-off, and intensity distribution of harmonics in the case of chirped drving pulses compared to chirp-free pulses. It is shown that the presence of Ni dopants and CsPbBr3plasma components improves the harmonics emission. Also, we measured the third-order nonlinear optical (NLO) properties of these nanocrystals using 800 nm, 60 fs, 1 kHz pulses. The variations of measured NLO parameters of CsPbBr3perovskite nanocrystals containing different concentrations of nickel correlate with variations of generated high-order harmonics from laser induced plasmas of studied nanocrystals in terms of harmonics intensity, cut-off, and spectral shift (in case of chirped driving pulses). The spectral shift of the harmonics generated from the Ni-doped CsPbBr3perovskite nanocrystals can be used to form tunable extreme ultraviolet sources.
ABSTRACT
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.