Degenerate Four-wave Mixing Research Articles

A Study of Degenerate Four‐Wave Mixing and Phase Conjugation in Metallic Nanohybrids

AbstractA theory of degenerate four‐wave mixing (DFWM) and phase conjugation is developed for metallic nanohybrids, which consist of an ensemble of interacting metallic nanoshells and noninteracting quantum dots (QDs). It is considered that three incident waves are applied to the metallic nanohybrid, and they produce a fourth output mixed wave. These waves induce dipoles in metallic nanoshells, generating surface plasmon polaritons, and interact with each other via the dipole–dipole interactions (DDI). In DFWM, the input and output waves travel in opposite directions, and this retroreflective nature is responsible for the phenomenon of phase conjugation. The analytical expressions for the input transmitted and output reflected wave intensities are calculated in the presence of the surface plasmon polaritons (SPPs) and the DDI polaritons. It is demonstrated that the phase conjugation, the phase coherent phenomena, and the intensities of both input transmitted and output reflected waves are enhanced due to SPPs and DDI polaritons. These findings indicate that the nanohybrid acts as a phase conjugate device and a phase coherent optical amplifier, which can be applied to fabricate optical nanoamplifiers, phase conjugate mirrors, and nanosensors by measuring the intensity of the output reflected wave.

Structural and ultrafast third-order nonlinearities of methyl and methoxy substituted anthracene chalcones: Z-scan, four-wave mixing, and DFT approaches

We report on the structural, thermal, linear, and ultrafast third-order nonlinear optical (NLO) properties of two novel anthracene chalcones: (2E)-1-(anthracen-9-yl)-3-(5-methylthiophen-2-yl)prop-2-en-1-one (5ML2SANC) and (2E)-1-(9-anthryl)-3-(2,4,5-trimethoxyphenyl)prop-2-en-1-one (245TMANC). The chalcones were synthesized by Claisen-Schmidt condensation reaction, and the single crystals were grown by the solvent evaporation method. The molecular structure was confirmed by FTIR and NMR spectroscopy, while the crystal structure was determined using the single crystal XRD. Both crystals belong to centrosymmetric monoclinic crystal system with space group P21/n. The Hirshfeld surface was analyzed to understand intermolecular interactions, and the band structures - including HOMO-LUMO levels, excited state energies, GCRDs and MEPs-were studied using DFT. The ultrafast third-order NLO properties were investigated by Z-scan and degenerate four-wave mixing (DFWM) techniques using Ti: Sapphire amplifier laser delivering ∼50 fs pulses at 800 nm (1 kHz, ∼4 mJ, 2 W). Two-photon absorption, positive nonlinear refraction, optical limiting and optical switching behaviors were observed by Z-scan measurements. The time-resolved DFWM show that the decay time of 5ML2SANC is ∼127 fs, while for 245TMANC it is ∼142 fs. The second hyperpolarizability (γ) measured by Z-scan, DFWM and the estimations from the DFT theory are found to be in good agreement (∼10−34 esu). The ultrafast optical response, significant NLO properties and thermal stability of the synthesized chalcones demonstrate their potential suitability in optical limiting and switching applications.

The effect of metal-to-ligand charge transfer on linear and nonlinear optical properties of hexaphyrin and metallo-hexaphyrins

Charge transfer from metal to ligand has implications in various fields of chemistry, physics and biology. The manipulation of spin properties would be necessary for controlling charge transfer in spintronics and biological applications. Upon binding to the metal atoms (Ni, Cu, Au, etc.), the spin properties would be modulated in organic conjugated molecules of less intrinsic spin–orbit coupling (SOC) due to SOC coming from the heavy elements. Emission spectra calculation is necessary to validate them as suitable fluorescence quenchers. The nonlinear optical properties like first-order hyperpolarisability β and second-order hyperpolarisability γ calculations are important to find out their relation between fluorescence quenching and higher order nonlinear optical (NLO) properties. From the second-order NLO properties, we computed degenerate four-wave mixing (DFWM) component ( γ ( 2 ) ( − ω ; ω , ω , − ω )) and finally quadratic nonlinear refractive indices of the expanded porphyrins (EPs). How the linear and nonlinear optical properties are dependent on the SOC coming from the heavy materials (Ni, Cu, Au), and charge transfer process is the most interesting question to be addressed for their potential uses for various optoelectronic and spintronic applications.

Impact of doping with organic dopants and mixed doping with alkali metals and organic dopants on the absorption, electronic, optoelectronic, thermodynamic and nonlinear optical properties of dibenzo[b,def]chrysene in gaseous media: DFT and TD-DFT studies.

In this study, we evaluate the geometrical, absorption, optoelectronic, electronic, nonlinear optical (NLO) and thermodynamic properties of dibenzo[b,def]chrysene molecule derivatives by means of DFT and TD-DFT simulations. In view of the aim of producing new high-performance materials for non-linear optics (NLO) by doping test, two types of doping were used. We obtained six derivatives by doping with organic dopants (Nitro, amide and ticyanoethenyl) and mixed alkali metal (potassium) and organic dopants. Doping with organic dopants produced molecules A, B and C, respectively when substituting one hydrogen with nitro (NO2), amide (CONH2) and tricyanoethenyl (C5N3) groups, while mixed doping involved considering A, B and C and then substituting two hydrogens with two potassiums to obtain compounds D, E and F respectively. The negative values of the various interaction energies calculated for all the doped molecules show that they are all stable, but also that molecules C and F are the most stable in the case of both dopings. The gap energies calculated at the B3LYP level of theory are all below 3eV, which means that all the molecules obtained are semiconductors. Better still, compounds C and F, with gap energies of 1.852eV and 1.204eV, respectively, corresponding to decreases of 35.67% and 58.18% in gap energy compared with the pristine molecule, are more reactive than the other doped molecules. Mixed doping is therefore a highly effective way of narrowing the energy gap and boosting the semiconducting character and reactivity of organic materials. Optoelectronic properties have also been improved, with refractive index values higher than those of the reference material, glass. This shows that our compounds could be used under very high electric field conditions of the order of 4.164 109V.m-1 for C and 7.410 109V.m-1 for F the highest values at the B3LYP level of theory. The maximum first-order hyperpolarizability values for both types of doping are obtained at the CAM-B3LYP level of theory by C: 10-30esu and by F: 10-30esu, and second-order values are also given by these same compounds. These values are higher than the reference value, which is urea, making our compounds potential candidates for high-performance NLO applications. In dynamic mode and at a frequency of 1064nm, at the CAM-B3LYP level of theory, the highest dynamic hyperpolarizability coefficients were obtained by C and F. Hyper-Rayleigh scattering , coefficients of the electro-optical Pockel effect (EOPE), EFISHG, third-order NLO-response degree four-wave mixing , quadratic nonlinear refractive index n2 were also calculated. The maximum values of n2 are obtained by C (6.13 10-20 m2/W) and F (6.60 10-20 m2/W), these values are 2.24 times higher than that of fused silica which is the reference for degenerate four-wave mixing so our molecules could also have applications in optoelectronics as wavelength converters, optical pulse modulators and optical switches. Using the DFT method, we were able to determine the optimized and stable electronic structures of doped dibenzo[b,def]chrysene derivatives in the gas phase. We limited ourselves to using the proven B3LYP and CAMB3LYP levels of theory for calculating electronic properties, and non-linear optics with the 6-311G + + (d,p) basis set, which is a large basis set frequently used for these types of compound. Gaussian 09 software was used to run our calculations, and Gauss View 6.0.16 was used to visualize the output files. TD-DFT was also used to determine absorption properties at the B3LYP level of theory, using the same basis set.

Si metasurface supporting multiple quasi-BICs for degenerate four-wave mixing

Abstract Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom’s geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction through wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging.

Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame.

NLOphoric Anthraquinone Dyes – A Review

AbstractThis review is about anthraquinone dyes. One of the advantages of organic NLOphores materials is the variety of chromophores explored for a wide range of potential applications in optoelectronics and biology. The second and third harmonic generations, as well as hyper‐Rayleigh scattering (HRS), the Z‐scan technique, degenerate four‐wave mixing (DFWM), and density functional theory (DFT), are all covered in this review. The most active sites for establishing enhanced NLO properties were found to be positions 2 and 6 of the anthraquinone core. The structural characteristics of dyes are used to divide them into subcategories. In each section, structures with a higher NLO response are highlighted. Researchers will benefit from this review when designing and synthesizing NLOphores.

Optical reciprocity-nonreciprocity-amplification conversion based on degenerate four-wave mixing

Optical nonreciprocity plays an important role in optical communication and quantum networks. In this research, we propose and demonstrate a conversion scheme of magnetic-free dual-channel optical reciprocal amplification (RA) and nonreciprocal amplification (NRA) based on the multiple degenerate four-wave mixing (FWM) process in hot atoms. In our experiment, the dual-channel NRA works with the action of a single pump field based on the establishment of FWM in the same direction and breaking in the opposite direction. Based on stable ground-state Zeeman coherence, by introducing a counter-propagating pump field again, NRA can be changed to RA in the opposite direction of the two original amplified conjugate signals. Moreover, the frequencies of RA signals are very dependent on those of co-propagating pump fields. The experimental realization of NRA-RA conversion may have applications for multichannel angular momentum spatial multiplexing and quantum gate manipulation.

Features of Degenerate Four-Wave Mixing in Liquid Crystal Cell in Dynamic Photorefractivity Mode

Features of Degenerate Four-Wave Mixing in Liquid Crystal Cell in Dynamic Photorefractivity Mode

Temperature and Thermal Diffusivity Diagnostics in Laminar Methane Flames Using Infrared Four-Wave Mixing Techniques.

Four-wave mixing techniques, such as coherent anti-Stokes Raman spectroscopy (CARS), laser-induced grating spectroscopy (LIGS), and degenerate four-wave mixing (DFWM), have been widely used in combustion diagnostics due to their advantages of high signal-to-noise ratio (S/N), coherent signal, and spatial resolution. In this work, a nano-second pulsed laser is utilized to generate mid-infrared (near 3 µm) pump beams, exciting the rovibrational transitions of nascent water in flames. Combined LIGS and DFWM measurements are demonstrated in premixed laminar CH4/O2/N2 flames with equivalence ratios from 0.6 to 1.5, to achieve precise thermometry in a wide range of flame conditions. The flame temperatures were also measured by thermocouple as a reference, and the results from LIGS and DFWM align well with the trends shown in the thermocouple measurements. In fuel-lean flames, where the mass-to-specific-heat ratio variation is minimal, LIGS provides temperature data with a precision better than 16 K (0.8%). In fuel-rich flames, where the increased H2 concentration in the flame introduces uncertainty in gas constants thus affecting the accuracy of LIGS thermometry, DFWM is instead employed for temperature measurement since it is less sensitive to the gas composition within the measured volume. The high-precision LIGS temperatures in lean flames serve as temperature reference during the DFWM calibration of the degree of saturation, and a precision better than 90 K (4.5%) is achieved for DFWM thermometry. In addition to temperature, a theoretical model is employed to fit LIGS signal time waveforms, extracting the local speed of sound and thermal diffusivity with precisions better than 0.5% and 1.3%, respectively. These high-precision measurements contribute additional data for flame research and simulation calculations. This way, the combined use of DFWM and LIGS proves the potential for accurate thermometry and diagnostics of other thermodynamic parameters across a wide range of flame conditions.

Cascaded degenerate four-wave mixing generation in thin-film lithium tantalate microdisk cavity

Cascaded degenerate four-wave mixing generation in thin-film lithium tantalate microdisk cavity

All-optical encryption/decryption of DmPSK signals with key steganography for photonic layer security.

In the 5th Generation Fixed networks (F5G) era, full-fiber-connected optical networks support emerging bandwidth-hungry services. However, optical networks are vulnerable to attack by tapping or other methods, which has been paid more and more attention in modern optical infrastructure. Therefore, optical Exclusive OR (XOR) encryption/decryption for advanced modulation formats used for F5G appears as one of the promising technologies to guarantee security. Some current solutions either leave potential security hazards because of the degenerate four-wave mixing and keys without special treatment or are cost-consuming due to employing multiple wavelengths and coherent receivers. In this paper, a novel all-optical encryption/decryption system for Differential m-Phase Shift Keying (DmPSK) signals occupying only a single wavelength with key steganography is proposed and simulated. The proposed system mainly consists of a generalized XOR (GXOR) part and a steganography part. We implement the GXOR part by the cascaded IQ Mach-Zehnder Modulators and the steganography part by the Equvilent-Phase-Shifted Super-Structured Fiber Bragg Grating (EPS-SSFBG). The numerical simulation results demonstrate that the GXOR implementation can achieve reconfigurable encryption/decryption of DQPSK (m = 4) or D8PSK (m = 8) signals merely with a single wavelength and a differential direct-detection receiver. And the EPS-SSFBG can enhance key security in a cost-efficient method as well. The system can work at the recorded bit rate of 260Gbps, which can be applied to enhance the photonic layer security in F5G and beyond.

Near-resonant twin-beam generation from degenerate four-wave mixing in hot 133Cs vapor enabled by field-dressed energy levels.

Squeezed light near an atomic resonance is beneficial for efficient atom-light quantum interfaces. It is desirable but challenging to directly generate in atoms due to excess noise from spontaneous emission and reabsorption. Here, we report on the use of energy-level modulation to actively control atomic coherence and interference in degenerate four-wave mixing (DFWM) and then to enhance the DFWM gain process for the generation of near-resonant squeezed twin beams. With this technique, we obtain a -2.6 dB intensity-difference squeezing detuned 100 MHz from the D1 F = 4 to F' = 4 transition of 133Cs.

Absorption spectra and enhanced Kerr nonlinearity in a four-level system

In a coherent system, enhanced nonlinearity can be reached via far-detuned coupling fields in the presence of Autler--Townes splitting. We explore the absorption spectra and the Kerr nonlinearity of the coherent system via the interaction between a four-level atomic system and triple fields. We obtain the absorption spectra with double, triple and even quadruple peaks which depend on both the magnitude and the difference of the coupling fields. The Kerr nonlinearity always remains reversely correlated with the absorption spectra. We find that the large coupling detunings can lead to a significant growth of the Kerr nonlinearity and the degenerate four-wave mixing. Both the Kerr nonlinearity and the four-wave mixing can be managed by adjusting the detunings of the coupling fields.

Numerical study of generation mechanisms of narrow spectral modes, emerging in a raman fiber laser with randomly distributed feedback

The present paper discusses possible influence of nonlinear effects, namely – the degenerate four-wave mixing process – upon the build-up and attenuation of narrow spectral modes, emerging in radiation of a Raman fiber laser with randomly distributed feedback.

Toward integrated tantalum pentoxide optical parametric oscillators.

We present a hybrid waveguide-fiber optical parametric oscillator (OPO) exploiting degenerate four-wave mixing in tantalum pentoxide. The OPO, pumped with ultrashort pulses at 1.55 µm wavelength, generated tunable idler pulses with up to 4.1 pJ energy tunable center wavelength between 1.63 µm and 1.68 µm. An upper bound for the total tolerable cavity loss of 32 dB was found, rendering a chip-integrated OPO feasible as a compact and robust light source.

Combinations of orbital angular momentum in two degenerate four-wave mixing processes in Rb vapor

We present experimental measurements showing the combination of the orbital angular momentum (OAM) content of incident light beams in two distinct processes of degenerate four-wave mixing induced in hot rubidium vapor. These two processes, driven by the same fields, must satisfy distinct topological charge (TC) selection rules, which impose OAM conservation. These selection rules are readily obtained from the so-called overlap integral of the incident beams and allow us to control the relations between the two nonlinear signals, in particular, to characterize the conditions to obtain the two signals with symmetric or anti-symmetric TCs. The tilted lens method was employed to measure the OAM content of the output fields. We also discuss the transition from the near- to the far-field distributions of the generated signals.

Z-scan and degenerate four wave mixing studies on newly synthesized copper complexes of curcumin

Designing novel metal complexes with high nonlinear optical (NLO) susceptibilities is a special interest for coordination compounds. They include a wider selection of metals with a variety of ligands and oxidation states, which can result in tuneable electronic capabilities. Paramagnetic Copper (II) complexes of curcumin were synthesized using different metal precursors and keeping curcumin as the base ligand. All the complexes were characterized by elemental analysis, magnetic susceptibility, and spectroscopic methods (UV–vis, FT-IR, ESR, and mass spectrometry). Nonlinear optical transmission measurements were carried out using nanosecond laser pulses with 532 nm wavelength, via a Z-scan and Degenerate four-wave mixing (DFWM) techniques. CuAcCur, CuClCur, and CuThCur complexes provided with 1.34 × 1024, 3.61 × 1024, and 4.05 × 1024 m3/W2, proved that these complexes possess excellent NLO properties and CuThCur being best among them. The NT dropped from 100 % to 78 %, 65 %, and 75 % in CuAcCur, CuClCur, and CuThCur respectively, showing that all the complexes have great potential for optical limiting (OL) application. The Conceptual-Density-Functional-Theory (CDFT) were employed to perform the theoretical analyses of complexes. Calculations on the various CDFT-based parameters such as electronegativity, HOMO-LUMO energy gap, molecular hardness, softness, dipole moment, and electrophilicity index of both species are performed. This work introduces three copper complexes with curcumin that show an excellent NLO and OL behavior.

Photorefractive four-wave mixing cannot be treated perturbatively. Revisiting the undepleted-pump approximation

We theoretically consider photorefractive degenerate four-wave mixing oscillators and show that, for this particular system, the linear stability analysis technique leads to incorrect results. The reason for this astonishing failure lies in the unphysical predictions of the undepleted-pump approximation, which appear naturally during the linearization process of the full model. As a consequence, photorefractive four-wave mixing does not seem to permit a perturbative treatment that allows the derivation of mean-field models, and one is forced to use the full model in order to make sensible predictions.

Theoretical investigation of pure-state single-photon and large-bandwidth-correlation biphoton generation from micro/nanofiber.

Pure-state single photons and large-bandwidth-correlation biphotons are fundamental resources for quantum information processing. The dispersion properties of micro/nanofiber (MNF) can be tailored by carefully choosing its diameter, resulting in a flexibly tailored biphoton spectrum. We theoretically investigate pure-state single photons and large-bandwidth-correlation biphotons produced by degenerate spontaneous four-wave mixing in MNF. In our simulation, a single-photon state with a purity of 99% will be theoretically attained by choosing the appropriate pump bandwidth and center wavelength with respect to the diameter and length of the MNF. Further, when an appropriate diameter with a negligible curvature at the zero dispersion wavelength is chosen, even a narrow pump bandwidth is capable of motivating remarkably broadband correlation biphotons, e.g., for a MNF diameter of 0.7 μm, the theoretical full width at half maximum is 473 nm. In practice, the application of a MNF-based quantum light source is dependent on the technologies that precisely control and measure the diameter. Our theoretical investigation will guide the experimental realization of high-quality quantum light sources based on MNF.