Nonlinear Optical Devices Research Articles

Low loss polycrystalline SiGe core fibers for nonlinear photonics.

Polycrystalline silicon-germanium (SiGe) core fibers offer great potential as flexible platforms for microscale optoelectronic and nonlinear optical devices. Compared to silicon (Si) core fibers, the SiGe material provides the potential for higher nonlinear coefficients, extended mid-infrared wavelength coverage, and a means to tune the bandgap and index of refraction by varying the Ge composition. Here, SiGe core fibers (10 at% Ge) were fabricated using the molten core drawing method, followed by CO2 laser irradiation to improve the homogeneity of the core. The transmission properties of the fibers were further optimized using a fiber tapering method to tailor the core diameter and re-grow the crystal grains. The resulting tapered SiGe fiber exhibited an average linear loss of ∼3 dB cm-1 across the wavelength range 1.5 - 2.5 µm, allowing for nonlinear optical characterization of this new fiber type. Measurements of the nonlinear figure of merit demonstrate the potential for higher nonlinear performance compared to the pure Si core fibers, particularly for wavelengths >2 µm, indicating that the SiGe fiber platform could open up new opportunities for mid-infrared nonlinear photonics.

Impact of Tamm plasmon structures on fluorescence and optical nonlinearity of graphene quantum dots

Graphene Quantum Dots (GQDs) are crucial in biomedicine for sensitive biosensing and high-resolution bioimaging and in photonics for their nonlinear optical properties. Integrating GQDs with photonic structures enhances optical properties by optimizing light-matter interactions and enabling precise control over their emission wavelengths. In this work, we explore a facile synthesis method for GQDs by pulsed laser irradiation in chlorobenzene and highlight the transformative potential of Tamm Plasmon Cavity (TPC) structures for tuning and amplifying the photoluminescence and nonlinear optical properties of GQDs. The characterization of GQDs revealed their exceptional properties, including efficient optical limiting and stable photoluminescence. The study demonstrated that the TPC structure significantly amplifies nonlinear optical effects due to the high light-matter interaction, indicating the potential for advanced optical systems, including optical limiters and nonlinear optical devices. Furthermore, introducing GQDs into the TPC structure leads to a significant enhancement and tuning of fluorescence emission. The Purcell effect, in combination with the confined electromagnetic fields within the TPC, increases the spontaneous emission rate of GQDs and subsequently enhances the fluorescence intensity. This enhanced and tunable fluorescence has exciting implications for high-sensitivity applications such as biosensing and single-molecule detection.

In situ formation of silver nanoparticles within labradorite mineral crystals exhibiting third-order nonlinearity

Silver nanoparticles are cost-effective plasmonic materials for the nonlinear optics, but the applications suffer incompatibility with the matrices. This study explores the in situ formation of silver nanoparticles within the crystalline matrix of labradorite minerals. The methodology involves a high-temperature diffusion process, enabling the nucleation and growth of silver nanoparticles directly within the labradorite crystal lattice. Characterization through spectroscopic and microscopic techniques reveals the successful formation of silver nanoparticles with a diameter of 8.40 ± 4.32 nm, exhibiting notable surface plasmonic resonances absorption at 414 nm. Additionally, the nonlinear optical property of the resulting material is investigated through Z-scan experiments. The third-order nonlinear optical susceptibility β at 400 nm was estimated to be 5.0 × 10−12 m/W. This research not only advances our understanding of nanoscale phenomena within mineral crystals but also underscores their potential applications in nonlinear optical devices and related fields.

Quasi-BICs enhanced second harmonic generation from WSe2 monolayer.

Quasi-bound states in the continuum (quasi-BICs) offer unique advantages in enhancing nonlinear optical processes and advancing the development of active optical devices. Here, the tunable robust quasi-BICs resonances are experimentally achieved through the engineering of multiple-hole Si-metasurface. Notably, the quasi-BICs mode exhibits flat bands with minimal dispersion at a wide range of incident angles, as demonstrated by the angle-resolved spectroscopy measurements. Furthermore, we demonstrate a giant second-harmonic generation (SHG) enhancement by coupling a WSe2 monolayer to the quasi-BICs hosted in the metasurface. Leveraging the strong local electric field and high state density of the observed quasi-BICs, the SHG from the WSe2 monolayer can be enhanced by more than two orders of magnitude. Our work paves the way for effectively enhancing nonlinear optical processes in two dimensional (2D) materials within the framework of silicon photonics and is expected to be applied in nonlinear optical devices.

Tunable third harmonic generation based on high-Q polarization-controlled hybrid phase-change metasurface.

Dielectric metasurfaces have made significant advancements in the past decade for enhancing light-matter interaction at the nanoscale. Particularly, bound states in the continuum (BICs) based on dielectric metasurfaces have been employed to enhance nonlinear harmonic generation. However, conventional nonlinear metasurfaces are typically fixed in their operating wavelength after fabrication. In this work, we numerically demonstrate tunable third harmonic generation (THG) by integrating a dielectric metasurface with the phase-change material Ge2Sb2Te5 (GST). The hybrid phase-change metasurface can support two BICs with different electromagnetic origins, which are transformed into two high-Q quasi-BICs through the introduction of structural asymmetry. The two quasi-BICs are selectively excited by controlling the polarization of incident light, and their wavelengths are tunable due to the phase transition of GST. Notably, the efficiency of THG is significantly enhanced at the fundamental wavelengths corresponding to the two quasi-BICs, and the operating wavelength for THG enhancement can be dynamically tuned through the GST phase transition. Furthermore, the wavelength of THG enhancement can be further tuned by manipulating the polarization of pump light. Additionally, a high-Q analog of electromagnetically induced transparency is numerically achieved through the interaction between a low-Q Mie resonance and a quasi-BIC mode, which also improves the THG efficiency. The high-Q polarization-controlled hybrid phase-change metasurface holds promise for applications in dynamically tunable nonlinear optical devices.

Lithium niobate on insulator - fundamental opto-electronic properties and photonic device prospects.

Lithium niobate on insulator (LNOI) combines a variety of optoelectronic properties and can meet practical performance requirements that are uncommon in optoelectronic materials. This review introduces the fundamentals and the photonic device concepts that arise from the LNOI materials platform. Firstly, the nonlinear optical response of LNOI is presented, including birefringent phase matching (BPM), modal phase matching (MPM), and quasi-phase matching (QPM). The tunable properties are also introduced, including electro-optical (EO), thermo-optical (TO), and acousto-optical (AO) effects. The structures of nonlinear optical devices, such as ridge waveguides (including periodically polarized inversion waveguides), Mach-Zehnder interferometer (MZI) modulators and micro-resonators (such as disks and rings) are demonstrated. Finally, the future of LNOI devices is discussed. In the already mature and developed optoelectronic material systems, it is rare to find one particular material system supporting so many basic optical components, photonic devices and optoelectronic devices as LNOI does in the field of integrated photonic chips.

Broadband and ascendant nonlinear optical properties of the wide bandgap material GaN nanowires

Gallium nitride (GaN) nanowire, as a type of wide bandgap nanomaterial, has attracted considerable interest because of its outstanding physicochemical properties and applications in energy storage and photoelectric devices. In this study, we prepared GaN nanowires via a facile chemical vapor deposition method and investigated their nonlinear absorption responses ranging from ultraviolet to near-infrared in the z-scan technology under irradiation by picosecond laser pulses. The experiment revealed that GaN nanowires exhibit remarkable nonlinear absorption characteristics attributed to their wide bandgap and nanostructure, including saturable absorption and reverse saturable absorption. When compared to bulk GaN crystals, the nanowires provide a richer and more potent set of nonlinear optical effects. Furthermore, we conducted an analysis of the corresponding electronic transition processes associated with photon absorption. Under high peak power density laser excitation, two-photon absorption or three-photon absorption dominate, with maximum modulation depths of 73.6%, 74.9%, 63.1% and 64.3% at 266 nm, 355 nm, 532 nm, and 1064 nm, respectively, corresponding to absorption coefficients of 0.22 cm/GW, 0.28 cm/GW, 0.08 cm/GW, and 2.82 ×10−4 cm3/GW2. At lower peak energy densities, GaN nanowires demonstrate rare and excellent saturation absorption characteristics at wavelength of 355 nm due to interband transitions, while saturable absorption is also observed at 532 nm and 1064 nm due to band tail absorption. The modulation depths are 85.2%, 41.9%, and 13.7% for 355 nm, 532 nm, and 1064 nm, corresponding to saturation intensities of 3.39 GW/cm2, 5.58 GW/cm2 and 14.13 GW/cm2. This indicates that GaN nanowires can be utilized as broadband optical limiters and high-performance pulse laser modulating devices, particularly for scarce ultraviolet optical limiters, and saturable absorbers for ultraviolet and visible lasers. Furthermore, our study demonstrates the application potential of wide bandgap nanomaterials in nonlinear optical devices.

Twist-Angle-Controlled Nonlinear Circular Dichroism on Gold-Crystal Hybrid Metasurfaces.

Optical chirality, which plays important roles in liquid crystal display and biological and chemical detection, has been attracting scientists' attention due to its potential applications in optical information processing. Usually, the chiral optical response of natural molecules is very weak. However, the emergence of metasurfaces offers a promising solution to solve this issue. By judiciously designing the geometry of meta-atoms, we have realized strong optical circular dichroism (CD) in both linear and nonlinear optical regimes. However, tuning of the CD with a metasurface remains challenging. Here, we propose the twist-angle-controlled nonlinear CD effect by using the second-harmonic generation process on a gold-crystal hybrid metasurface. The CD effect of the second-harmonic waves can be tuned well by controlling the twist angle between the two constituent materials. The proposed hybrid metasurface may open new avenues for developing ultracompact and multifunctional nonlinear optical devices.

Controlled growth of 3R phase niobium diselenide and its properties

Inversion symmetry broken 3R phase transition metal dichalcogenides (TMDs) show fascinating prospects in spintronics, valleytronics, and nonlinear optics. However, the controlled synthesis of 3R phase TMDs is still a great challenge. In this work, two-dimensional 3R-NbSe2 single crystals up to 0.2 mm were synthesized for the first time through chemical vapor deposition method by designing a space-confined system. The crystal size and morphology can be controlled by the location of the stacked substrates and the amount of the Nb2O5 precursor. Scanning transmission electron microscopy and Raman measurements reveal the NbSe2 exhibits a pure 3R stacking mode with relatively weak interlayer van der Waals interactions. Importantly, 3R-NbSe2 shows obvious second harmonic generation signal which intensity intensified as thickness increases. Density functional theory calculations and optical absorption demonstrate the coexistence of metallic and semiconducting optical properties of 3R-NbSe2. We designed a NbSe2/WS2/NbSe2 photodetector utilizing the metallicity of 3R-NbSe2, which shows good performance especially an ultrafast response (6–7 μs, 0.5 ms − 7.9 s for Au electrodes in literature). The proposed strategy and findings are of great significance for the growth of many other 3R-TMDs and applications of nonlinear optical and ultrafast devices.

Luminescence and two-photon absorption assisted optical limiting properties of Ag-doped CdWO4 nanorods

The emerging demand for the fabrication of nonlinear optical materials with high limits of optical power is obvious in nonlinear optics due to their wide application in photonic devices. We report the linear and third-order nonlinear optical properties of Ag-doped CdWO4 nanorods and their dependence on Ag-doping concentration. CdWO4 nanorods with different Ag concentrations were synthesized by the chemical precipitation method and characterized by UV–Vis absorption, X-ray diffraction (XRD), Raman, Photoluminescence and its lifetime studies, X-ray Photoelectron spectroscopy and Transmission Electron Microscopy (TEM). The introduction of Ag ions has led to an increased redshift in the CdWO4 absorption spectra extended into longer wavelength bands, thus enhancing optical absorption within the visible range. The XRD pattern showed that the nanorods crystallized in a monoclinic wolframite structure. The incorporation of Ag in CdWO4 decreases the luminescence emission intensity due to surface quenching effect. Luminescence lifetime measurement reveals the longer decay lifetime for Ag-doped CdWO4 nanorods due to the reduction of density of defects and deep trap state. The nonlinear optical behaviour of the nanorods was investigated by an Open aperture Z-scan technique at 532 nm using pulsed wave Nd: YAG laser. Experimental results showed that reverse saturable absorption is responsible for the observed nonlinearity in the nanorods. The addition of Ag can significantly improve the nonlinear absorption coefficient and optical limiting effects of CdWO4 which can be used as a potential material in nonlinear optical devices.

Studies on the synthesis, growth, and characterization of 2-cyanopyridinium salicylate single crystals for nonlinear optical applications

By employing methanol as the solvent in slow solvent evaporation method, a new nonlinear optical organic single crystal of 2-cyanopyridinium salicylate (2-CPSC) was grown. The lattice parameters of the 2-CPSC crystals were found out to be a = 7.7764(9) Å, b = 12.3938(17) Å, c = 12.3685(18) Å, and β = 94.44º using single crystal X-ray diffraction (SCXRD) analysis. The confirmation of crystalline nature was done by powder XRD analysis. The 2-CPSC crystal's chemical composition and functional groups were confirmed by Fourier transform infrared (FTIR) spectral analysis. The optical study was done by ultraviolet-visible-near infrared (UV–Vis-NIR) spectral analysis showing a cutoff wavelength of 338 nm. Studies on the grown 2-CPSC crystal's dielectric and Vicker's microhardness were also conducted. The linear dependence of photocurrent with the applied electric field was revealed for the grown crystals. The 2-CPSC crystal's third-order nonlinearity was investigated by the single-beam Z-scan technique using a continuous He-Ne laser. The open aperture Z-scan reveals the two-photo absorption mechanism and the closed aperture Z-scan study reveals the positive nonlinearity of the 2-CPSC crystals with third order susceptibility value of χ3=2.6763×10−6(esu). The density functional theory (DFT) method of B3LYP level with the 6–31++G(d,p) basis set was used for different quantum chemical calculations like geometry optimization, natural bond orbital (NBO) analysis, mulliken atomic charge, and molecular electrostatic potential (MEP). The higher nonlinearity of the 2-CPSC can be a potential alternative for commercially available potassium dihydrogen phosphate (KDP) and candidate for its application in nonlinear optical devices like optical limiting and optical switching.

Role of donor/acceptor of doping on nonlinear optical properties of CdS nanocomposite decorated by carbon quantum dots and reduced graphene oxide

Cadmium sulfide (CdS), reduced graphene oxide (RGO), carbon quantum dots (CQDs), CQDs/CdS and RGO/CdS nanocomposites have been synthesized. The products have been characterized by FESEM, XRD, UV–visible spectroscopy and diffuse reflectance spectroscopy (DRS). The nonlinear optical (NLO) properties of all products are measured using Z-scan technique at 532 nm wavelength. The results reveal that the formation of structures resulting in dπ–pπ delocalized systems makes the samples a perfect choice for NLO devices. NLO properties of CQDs/CdS is attributed to the charges or energy transfer between CQDs and CdS, in the CQDs/CdS hybrid. Overall, the laser excitation of the small CdS (36 nm) in the RGO/CdS hybrid material promotes electron and/or energy transfer to the RGO component. Therefore, RGO has more effect on NLO properties of CdS than CQDs on CdS nanocomposites. This enhanced electron transfer process leads to improved NLO performances, making the hybrid material a promising candidate for various optoelectronic applications.

Enhanced second harmonic generation from supercavity mode and magnetic resonance in dumbbell-shaped silicon nanoblock

Abstract Electromagnetic multipole resonance can be excited by dielectric nanostructures of appropriate size to effectively promote light-matter interaction. The interactions between light and nanostructures have the capability to enhance the electromagnetic field in the near field, thereby improving the nonlinear effect of nanostructures. We illustrate that the supercavity mode and magnetic dipole resonance are activated by a single dumbbell-shaped silicon nanoblock (DS-SiNB), to trap the near-field electromagnetic field energy. Enhanced second harmonic generation is achieved by exploiting the localized electromagnetic field at the surface of the nanostructure. Numerical simulations reveal that magnetic quadrupole (MQ) and total electric dipole (TED) can be coupled to the same radiation channel by adjusting continuously the aspect ratio Lout/Ly (the outer edge length to the length of DS-SiNB) of the nanoblock. When the aspect ratio Lout/Ly = 1, the supercavity mode formed by the interference of MQ and TED is excited at λ1 = 1124 nm. And, the strong magnetic resonance mode formed by the coupling of two magnetic dipoles (MD) in the same direction is also excited at λ2 = 1124 nm. Supercavity mode and strong magnetic dipole resonance can effectively capture electromagnetic fields on the surface of nanostructures to attain enhanced second harmonic generation (SHG). Our study presents a novel approach to enhance the nonlinear optical effect of a single silicon nanostructure, which can lead to the development of more efficient nonlinear optical devices.

Extraordinary Enhancement of Nonlinear Optical Interaction in NbOBr2 Microcavities.

2D materials are burgeoning as promising candidates for investigating nonlinear optical effects due to high nonlinear susceptibilities, broadband optical response, and tunable nonlinearity. However, most 2D materials suffer from poor nonlinear conversion efficiencies, resulting from reduced light-matter interactions and lack of phase matching at atomic thicknesses. Herein, a new 2D nonlinear material, niobium oxide dibromide (NbOBr2) is reported, featuring strong and anisotropic optical nonlinearities with scalable nonlinear intensity. Furthermore, Fabry-Pérot (F-P) microcavities are constructed by coupling NbOBr2 with air holes in silicon. Remarkable enhancement factors of ≈630 times in second harmonic generation (SHG) and 210 times in third harmonic generation (THG) are achieved on cavity at the resonance wavelength of 1500nm. Notably, the cavity enhancement effect exhibits strong anisotropic feature tunable with pump wavelength, owing to the robust optical birefringence of NbOBr2. The ratio of the enhancement factor along the b- and c-axis of NbOBr2 reaches 2.43 and 5.27 for SHG and THG at 1500nm pump, respectively, which leads to an extraordinarily high SHG anisotropic ratio of 17.82 and a 10° rotation of THG polarization. The research presents a feasible and practical strategy for developing high-efficiency and low-power-pumped on-chip nonlinear optical devices with tunable anisotropy.

Interfacial second harmonic generation switching with 2D monolayer/VO2 heterostructure

To establish a facile nonlinear optical switching mechanism activated by thermal field, that is compatible with on-chip integration, we develop a physical model to quantify the interfacial second harmonic generation (SHG) of 2D monolayer/3D phase-changing material heterostructure. Our results show that heat-induced phase transition of VO2 can realize temperature-reversible interfacial SHG switching, with an ON-OFF ratio of about 3 and a low temperature threshold of about 60 °C. Experimental results can be well addressed by quantitative calculations based on the physical model. This work constitutes substantial insights into interfacial SHG switching, which will benefit design and construction of on-chip nonlinear optical devices based on 2D monolayers.

The growth aspects and experimental techniques for the characterization of amino acid L-histidine hybrid crystals for nonlinear optical device applications

The development of crystal growth and measurement methods opens new possibilities for studying materials with remarkable nonlinear optical features. The development of bulk crystals is a constant concern to be beneficial for device applications. This study focuses on the development of nonlinear optical crystals of l-histidine complexes, characterization approaches, and prospective applications. The solution growth approach, a straightforward, inexpensive, and low-temperature growth technique, was adopted broadly. Recent studies show that l-histidine derivatives have potential optical, SHG, thermal, dielectric, and mechanical properties, making them an excellent choice for nonlinear optical devices. In this work, structural, spectroscopic, chemical composition, linear and nonlinear optical analyses, thermal, and dielectric characterizations of l-histidine derivatives were conducted. Most of the l-histidine complexes were found to be crystallized in orthorhombic and monoclinic crystal systems with P212121 and P21 space groups. The crystalline perfections of the samples were analyzed by the HR-XRD method. The energy-dispersive X-ray (EDX) spectroscopic technique was applied to evaluate the chemical content of the compounds. FT-IR and FT-Raman techniques were used to recognize the molecular vibrations and functional groups of the l-histidine derivatives. The UV-visible and photoconductivity studies were done to examine the optical behaviors of the developed crystals. Most of the crystals were found to have excellent optical transparency and wide bandgaps. It has been observed that l-histidine hydro-fluoride dehydrate and l-histidine tetrafluoroborate are found to have the highest second harmonic generation (SHG) efficiencies. The dielectric analyses were utilized to study the dielectric constant and dielectric loss variations with the applied frequency. According to the thermal analyses, most of the crystals were found to have substantial thermal stabilities suitable for device applications.

Novel third order nonlinear optical stilbazolium crystal replaced with 3-methoxy benzaldehyde as donor for optical device applications

A novel organic nonlinear optical stilbazolium group single crystal of 1-methyl-2-[2-(3-methoxystyryl)]-pyridinium iodide (subsequently referred to as MSMI) was grown by the solution growth technique using the method of slow evaporation at ambient temperature. The Single-crystal XRD investigation indicates that the MSMI crystal belongs to a monoclinic crystal system with a centrosymmetric space group. CHN elemental analyser confirms the weight percentage of carbon (C = 51.00 %) hydrogen (H = 4.55 %) and nitrogen (N = 3.94 %) in the MSMI crystal structure. The presence of 16 hydrogen atoms and 15 carbon atoms in the MSMI was affirmed by the Nuclear Magnetic Resonance (NMR) spectroscopic analysis. Fourier Transform Infrared (FTIR) studies confirmed the fundamental vibrations for different functional groups found in the MSMI crystal. The Hirsfeld surface analysis figured out the hydrogen bond interaction and π…π interaction which supports the stability of the crystal structure. The crystal is found to exhibit transmittance of wavelength above 400 nm and has a band gap of 3.05 eV ascertained from UV–Vis-NIR spectroscopic analysis. Photoluminescence (PL) studies reveal that the title crystal has an emission wavelength of 572 nm. The surface characteristics of the title crystal were examined by Atomic Force Microscopy (AFM), and etching studies. The value of Meyer's number is n = 1.8 which is determined by the Vickers microhardness studies. The value of the third-order nonlinear refractive index (n2) is 4.662×10−8 cm2/W, the nonlinear absorption coefficient (β) is 1.305×10−3 cm/W, nonlinear susceptibility (χ(3)) is 9.297×10−5 esu and the optical limiting threshold is 11.43 J/cm2 was ascertained form the Z-scan technique. The results indicate that the MSMI crystal is a potential optical limiter and has promising applications in nonlinear optical devices.

Artificial Domain Patterning in Ultrathin Ferroelectric Films via Modifying the Surface Electrostatic Boundary Conditions.

Nanoscale spatially controlled modulation of the properties of ferroelectrics via artificial domain pattering is crucial to their emerging optoelectronics applications. New patterning strategies to achieve high precision and efficiency and to link the resultant domain structures with device functionalities are being sought. Here, we present an epitaxial heterostructure of SrRuO3/PbTiO3/SrRuO3, wherein the domain configuration is delicately determined by the charge screening conditions in the SrRuO3 layer and the substrate strains. Chemical etching of the top SrRuO3 layer leads to a transition from in-plane a domains to out-of-plane c domains, accompanied by a giant (>105) modification in the second harmonic generation response. The modulation effect, coupled with the plasmonic resonance effect from SrRuO3, enables a highly flexible design of nonlinear optical devices, as demonstrated by a simulated split-ring resonator metasurface. This domain patterning strategy may be extended to more thin-film ferroelectric systems with domain stabilities amenable to electrostatic boundary conditions.

Nonlinear optical properties in Pr3+-Er3+-codoped tellurite glasses

In this investigation, we systematically probe the structural, optical, and, notably, the nonlinear optical properties of Pr3+-Er3+-codoped tellurite glasses to understand the potential new functionalities of the glass and, thus, their applicability. The glass samples were synthesized employing the melt-quenching technique and subsequently characterized using X-ray photoelectron spectroscopy (XPS) and femtosecond (fs) pulse Z-scan measurements at 720 and 750 nm wavelengths. XPS analyses unveiled increased non-bridging oxygens (NBO) with ascending Pr2O3 content. It was observed that the increasing concentrations of Pr3+ ions show a linear dependence with the increase of NBO in the glass network (r2 > 0.95). This trend further supported the formation of Te3+ ions via the oxidation of Te4+ for charge compensation and was affirmed by a decrement in average TeO bond as Pr2O3 concentrations increased. The tellurite glasses showcased positive nonlinear refraction on the nonlinear optical (NLO) front. The rise in n2 values was directly linked to the Pr2O3 content, a phenomenon attributed to the increased presence of non-bridging oxygens and the inherent polarizability of Pr3+ ions. Collectively, our findings offer pivotal insights into the modulation of NLO attributes in Er3+-doped tellurite glasses via Pr3+ ion doping, underscoring their potential in advanced NLO device applications.

Realizing the effect of s-block metals on a charge transfer crystal of indol-2-one for enhanced NLO responses with efficient energetic offsets.

Due to their unique photophysical properties, organic charge transfer crystals are becoming promising materials for next-generation optoelectronic devices. This research paper explores the impact of s-block metals on a charge transfer crystal of indol-2-one for enhanced nonlinear optical (NLO) responses with efficient energetic offsets. The study reveals that alkali metals can enhance NLO performance due to their free electrons. The Perdew-Burke-Ernzerhof functional of DFT with dispersion correction (D3) was used, and the λmax values ranged between 596 and 669nm, with the highest value for dichloromethane (DCM). Leveraging the unique properties of metals allowed for the development of nonlinear optical materials with improved performance and versatility. Softness (σ) values provide insight into electron density changes, with higher values indicating a greater tendency for changes and lower values indicating the opposite. The NLO results for the chromophores MMI1-MMI6 show varying linear polarizability (< α0 >) along with their first (β0) and second (γ0) hyperpolarizabilities. Chromophore MMI4 stands out with the highest NLO performance, having two potassium (K) atoms. Its < α0 > , β0, and γ0 values of 4.19, 7.09, and 17.43 (× 10-24 e.s.u), respectively, indicate a significant enhancement in NLO response compared to the other chromophores. The transitions involving (O20)LP → (C3-N5)π* and (O19)LP → (N12-C13)π* exhibit the highest level of stabilization, followed by (O23)π → (C10-C11)π*, while (C6-N12)π → (C6-C7)π* shows the lowest level of stabilization for chromophore MMI4. The present research work is facile in its nature, and it can be helpful for synthetic scientist to design the new materials for uniting crystal properties with metal doping for efficient NLO devices.