Nonlinear Optical Devices Research Articles

Topologically-protected four-wave mixing enhanced by tailoring topological edge states

Laser pulse compression serves as a pivotal technique in nonlinear optics and light-matter interactions. Traditional methods, including Q-switching, mode-locking techniques, and chirped pulse amplification, are employed to generate high-intensity fields. However, these methods pose challenges when applied to topological lasers. In this study, we explore the pulse compression technique for topological edge states (TESs). Our findings reveal a significant correlation between the pulse width of TESs and their group velocity. Though factors such as nonlinear TES dispersion, disorders, and edge bending also affect pulse width, their impacts are comparatively less pronounced compared to that of group velocity. Through the customization of TES’s group velocity, we demonstrate a remarkable enhancement of four-wave mixing, showcasing it as a prime example of a nonlinear processing technique. Importantly, our approach promises seamless integration into topological laser systems, ensuring optimal performance with zero energy transfer loss and introducing a flexible dimension and robustness to topological nonlinear optical devices.

Investigation of structural, morphological and optical characteristics of (Ni,Co)S/Fe3O4 nanocomposites and (Ni,Co)-doped Fe3O4 nanoparticles

Abstract The present search seeks to customize the optical, magnetic, and structural characteristics of NiS/Fe3O4 and CoS/Fe3O4 nanocomposites in contrast to Ni-doped Fe3O4 and Co-doped Fe3O4 nanoparticles to investigate linear, nonlinear, and optoelectronic applications. In this regard, the preparation of magnetite nanoparticles (Fe3O4) doped by Ni and Co and also NiS/Fe3O4 and CoS/Fe3O4 nanocomposites was successfully carried out through the co-precipitation method. The XRD obtained results revealed the presence of a face-centered cubic structure in all samples. Moreover, the estimation of the crystalline size for the Fe3O4, Ni-doped Fe3O4, Co-doped Fe3O4 NiS/Fe3O4, and CoS/Fe3O4 nanopowders was carried out using the Debye–Scherrer formula, yielding values ranging from 8.45 nm to 10.13 nm. Furthermore, nanopowder microstructure images were taken through a field emission scanning electron microscope (FESEM), which represented that the shape of the grains was spherical and irregular. Furthermore, the samples validate the purity of the samples which revealed the presence of vibrational modes in the metal oxide bonds. An optical investigation was conducted on all samples utilizing a diffuse reflectance spectroscopy. Band gap values ​​were estimated based on diffuse reflectance spectroscopy data through Tauc plot analysis, which yielded a range from 2.88 eV to 3.01 eV, indicating that the red shift in the band gap of Fe3O4 with all impurities except CoS/Fe3O4, provides catalytic applications of synthesized materials. Additionally, numerical calculations utilizing the Kramers-Kronig relation and Wemple-DiDomenico (WDD) model, were performed to assess the extinction coefficient (k), refractive index (n), linear susceptibility ( χ 1 ), and third-order nonlinear susceptibility ( χ 3 ) parameters on the reflectance data. Compared to other studied samples, the maximum evaluated values of χ 3 and the density of polarizable constituents (N) were related to the Ni-doped Fe3O4 NPs. This observation suggests that the prepared nanopowders possess significant potential for utilization in both fields of linear and nonlinear optical devices.

Regulating Second‐Harmonic Generation in 2D Chiral Perovskites Through Achiral Organic Spacer Cation Alloying Strategy

AbstractThe inherent structural flexibility and chiroptical activity of 2D chiral perovskites make them promising for the nonlinear optical (NLO) application. A comprehensive understanding of the second‐harmonic generation (SHG) mechanism in 2D chiral perovskites is essential for developing NLO devices. However, the rational design of 2D chiral perovskite structures to regulate SHG properties remains challenging. Herein, to regulate SHG response, an achiral organic spacer cation alloying strategy is employed to construct a series of 2D chiral perovskites. Through the measurement of temperature‐dependent photoluminescence (PL) spectra, it is revealed that the material design strategy can effectively modulating self‐trapped exciton (STE) emission. More importantly, it is confirmed that there is a competitive relationship between STE emission and SHG in 2D chiral perovskites. Meanwhile, the microscopic imaging of circularly polarized‐SHG is demonstrated in chiral perovskites. This work will not only advance the understanding of the SHG mechanism in 2D chiral perovskites but also provide inspiration for the rational design and synthesis of perovskites for NLO devices.

Electrically switchable chiral nonlinear optics in an achiral ferroelectric 2D van der Waals halide perovskite.

Two-dimensional (2D) van der Waals (vdW) semiconductors play a key role in developing nanoscale nonlinear optical devices. 2D Ruddlesden-Popper lead halide perovskites (RPPs) expand the potential of using 2D vdW semiconductors in nonlinear optical applications because they exhibit electrically switchable and chiral second-order optical nonlinearity originating from the emergence of ferroelectricity and chirality. However, electrically switchable chiral nonlinear optics has not yet been realized because of the difficulty in electrically manipulating chiral structures. Here, we demonstrate that chiral second-harmonic generation (SHG) can be electrically induced and switched in an achiral biaxial ferroelectric 2D RPP. We observe reversible and continuous electrical switching of SHG circular dichroism and large nonlinear chiroptical activity. Polarization-resolved SHG imaging reveals that electrical poling induces the ferroelectric multidomain structure arising from the biaxial nature of the material, and the planar chirality appears. Our findings show a simple electrical control of the nonlinear chiroptical responses and establish chiral nonlinear optics based on ferroelectric 2D RPPs.

Peierls Distortion Induced Giant Linear Dichroism, Second-Harmonic Generation, and In-Plane Ferroelectricity in NbOBr2.

The Peierls distortion plays an essential role in governing the in-plane ferroelectricity and nonlinear optical characteristics of anisotropic niobium oxide dihalides, such as NbOCl2 and NbOI2. Despite its significance, experimental investigation into the structural, optical, and ferroelectric properties of NbOBr2 has been lacking. Here, the successful fabrication of centimeter-sized, high-quality NbOBr2 single crystals, enabling direct observation of Peierls distortion using aberration-corrected scanning transmission electron microscopy, is reported. Notably, the magnitude of Peierls distortion in NbOBr2 falls between that observed in NbOCl2 and NbOI2. Furthermore, the existence of giant linear dichroism absorption and second-harmonic generation (SHG) phenomena associated with Peierls distortion is confirmed. Exfoliated NbOBr2 flakes exhibit single-domain ferroelectricity, with the polarization switchable by an electric field. Temperature-dependent SHG measurements reveal a Curie temperature of ≈502K for ferroelectric NbOBr2. This work demonstrates that NbOBr2 holds promise for polarized nonlinear optical devices, as well as for nonvolatile information processing and storage devices.

Chirality-controlled second-order nonlinear frequency conversion in lithium niobate film metasurfaces.

The high-quality factor resonant metasurfaces have extensive applications in enhancing nonlinear frequency conversion efficiency at the subwavelength scale. However, methods for actively modulating the frequency conversion process are limited. We design a chiral lithium niobate film metasurface and investigate the photonic spin as a new degree of freedom to dynamically control the second-order nonlinear frequency conversion, without reconfiguring the structure by using external stimuli. The chiral resonance with circular dichroism (CD) of 0.62 gives rise to a high nonlinear CD of 0.84 in second-harmonic generation efficiency. Interestingly, combining the chiral resonance and an achiral quasi-bound state in the continuum enables us to investigate the photonic-spin-controlled sum-frequency generation and the photon pair generation from the spontaneous parametric downconversion process. Owing to the ultrahigh quality factor exceeding 103 both for two resonances, the second-order nonlinear frequency conversion occurs at a wavelength region of 0.2 nm, suggesting good monochromaticity. Our work opens new, to our knowledge, avenues for practical implementation of dynamically controlled nonlinear optical devices and will find utility in holography, switchable light sources, and information processing.

Synthesis, characterization, and study of linear and non-linear optical properties of some newly thieno[2,3-b]thiophene analogs

Abstract Newly 3,4-Diaminothieno[2,3-b]thiophene derivatives were synthesized by attaching with different aromatic have rich electron. The resulted compounds have been investigated by FT-IR, NMR, elemental analysis, and optical absorption spectra. Comparison between these resulted compounds revealed oxoindolin-3-ylidene)amino)thieno[2,3-b]thiophene has the highest absorption peak intensity at ~ 696nm, thin films have been prepared by thermal evaporation technique and characterized by UV-Visible-NIR spectroscopy as well as the allied absorption, dielectric and dispersion parameters have been investigated and compared with other reported results. Obtained results indicated diethyl 3,4-bis(((E)-2-oxoindolin-3-ylidene)amino)thieno[2,3-b]thiophene-2,5-dicarboxylate and 3,4-bis(((E)-2-oxoindolin-3-ylidene)amino)thieno[2,3-b]thiophene-2,5-dicarbonitrile have manifested small band energy gap energy 1.95, 1.66 eV; respectively as a result of increasing conjugation and high absorption coefficient, make these compounds ideal for use in solar cell. The high nonlinear parameters such as refractive index and third-order nonlinear susceptibility of these organic compound thin films are significantly asymptotic compared with chalcogenide and oxide materials, making them suitable for nonlinear optical devices.

Surface enhanced Raman scattering-based sensing and ultrafast nonlinear optical properties of silver-hexagonal boron nitride nanocomposites achieved by femtosecond laser ablation

This study investigated the surface-enhanced Raman spectroscopy (SERS) properties and nonlinear optical (NLO) behavior of silver nanoparticles (Ag NPs) decorated hexagonal boron nitride (hBN) nanocomposites. Although Ag NPs are known for their excellent plasmonic properties, their susceptibility to oxidation in ambient conditions significantly reduces SERS activity. To overcome this, a femtosecond laser-assisted single-step novel approach is developed for synthesizing hybrid Ag-hBN nanocomposites via ablating Ag target in a solution of exfoliated hBN nanosheets, forming uniformly embedded Ag NPs on hBN nanosheets. The morphological characteristics and elemental compositions were validated by field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and energy dispersive X-ray spectroscopy (EDS). TEM analysis revealed that Ag NPs averaged 15 nm in size, while hBN nanosheets had lateral dimensions of approximately 250 nm. The SERS activity of the prepared nanocomposites was investigated using dye and explosive molecules, achieving detection sensitivities of 1 μM and 100 μM, respectively, with high reproducibility. These detection sensitivities are significant as they demonstrate the potential of the Ag-hBN nanocomposites for sensitive and reliable detection of trace amounts of analytes. Notably, the Ag-hBN nanocomposites showed enhanced SERS activity compared to pure Ag NPs, with a 2.5-fold improvement for Nile blue, 3.6-fold for methylene blue, and 2.4-fold for RDX. The current study also demonstrates that hBN prevents Ag NPs’ oxidation and preserves the SERS functionality even at elevated temperatures. Furthermore, the NLO properties of the nanocomposites were investigated using the standard Z-scan technique, revealing two-photon and three-photon absorption coefficients of 3 × 10−4 cm/GW and 6.5 × 10−5 cm3/GW2, respectively. The findings highlight the potential of Ag-hBN nanocomposites to enhance SERS and NLO devices, enabling future applications in sensing and photonics.

Two-Dimensional Topological Ferroelectric Metal with Giant Shift Current.

The pursuit for "ferroelectric metal," which combines seemingly incompatible spontaneous electric polarization and metallicity, has been assiduously ongoing but remains elusive. Unlike traditional ferroelectrics with a wide band gap, ferroelectric (FE) metals can naturally incorporate nontrivial band topology near the Fermi level, endowing them with additional exotic properties. Here, we show first-principles evidence that the metallic PtBi_{2} monolayer is an intrinsic two-dimensional (2D) topological FE metal, characterized by out-of-plane polarization and a moderate switching barrier. Moreover, it exhibits a topologically nontrivial electronic structure with Z_{2} invariant equal to 1, leading to a significant FE bulk photovoltaic effect. A slight strain can further enhance this effect to a remarkable level, which far surpasses that of previously reported 2D and 3D FE materials. Our Letter provides an important step toward realizing intrinsic monolayer topological FE metals and paves a promising way for future nonlinear optical devices.

Promising LVHCL material for nonlinear optical devices and pyroelectric sensors

Promising LVHCL material for nonlinear optical devices and pyroelectric sensors

Bismorpholin-4-ium tetrabromo-cadmium metal-organic single crystal delivering Crystal structure, physicochemical properties and Characterizations for Optoelectronic Applications

For the development of nonlinear optical (NLO) materials, compositions of cadmium chloride (CC) and Morpholinium bromide (MB) molecules were utilized to form metal-organic materials. Morpholinium bromide was incorporated with cadmium metal to have electron charge transfer by constructing acentric structures that take advantage of strong third-order nonlinear optical properties. Bis Morpholinium cadmium bromide (BMCB) crystals were synthesized by a slow evaporation method (SEST). The BMCB crystal belongs to monoclinic P21/c space group with four molecules in the unit cell (a = 6.7607(4) Å, b = 16.5811(2) Å, c = 14.9744(2) Å, β=94.136(3) ° and Z = 4). The grown BMCB crystal phase purity and crystallinity were further investigated using powder X-ray diffraction (PXRD) analysis. Using Fourier transform infrared (FTIR) spectroscopy, the functional groups and their vibrational states were evaluated. From the results obtained from UV–vis-NIR spectral analysis, it is clear that the title compound is transparent in the visible range with the lower cut-off wavelength of 254 nm. The TG-DTA measurement has been used to evaluate thermal stability. Microhardness measurements were carried out to evaluate the mechanical stability of the grown crystal. The third-order nonlinear optical (NLO) characteristics were studied using Z-scan technique. The grown crystal exhibits outstanding third-order NLO response and wide laser damage threshold (LDT), which are crucial characteristics for developing practical NLO devices. The findings consequently open a novel path for the logical design of enormous, thermally stable and NLO-active metal-organic complexes for NLO applications.

Unified analytical theory of nonlinear optical diffraction by nonlinear gratings

When a pump laser shines upon a periodically poled lithium niobate (LN) thin plate nonlinear grating, second-harmonic generation (SHG) and its nonlinear diffraction occurs, with the nonlinear Raman–Nath diffraction (NRND), nonlinear Bragg diffraction (NBD), and nonlinear Cerenkov radiation (NCR) being several prominent examples. In this work we build and present a unified analytical theory to solve SHG for the NRND, NCR, and NBD processes from LN domains, domain walls, and defects. We find that the critical physical entity that governs the nonlinear diffraction is the effective nonlinear coefficient for each Fourier wave component. The analytical theory has a great generality and applicability scope. It allows us to retrieve and analyze everything about the dependence of SHG nonlinear diffraction on a series of physical and geometrical parameters such as the pump laser intensity, polarization, incidence polar and azimuthal angles, the LN thin plate thickness and its crystalline orientation, LN domain size and pitch, domain wall thickness and crystalline configuration, defect size and crystalline configuration, and the SHG diffraction beam angle and polarization. The analytical theory also enables us to analyze deeply the similarities and differences of the three nonlinear diffraction processes NRND, NCR, and NBD, build a smooth and broad connection bridge among these three processes, and construct a unified physical picture to understand, describe, and exploit these three processes of seemingly big difference. Besides, the analytical theory can be applicable to handle nonlinear diffraction by domains, domain walls, and defects in other more complicated 2D and 3D nonlinear gratings made from LN and other nonlinear crystals. Finally, the analytical theory can help to build a bridge connecting the extrinsic SHG nonlinear diffraction properties with the intrinsic domain poling and inversion material and physical properties of LN and other nonlinear crystals and explore novel nonlinear optical devices and technologies.

Ultrafast Charge Transfer-Induced Unusual Nonlinear Optical Response in ReSe2/ReS2 Heterostructure.

Ultrafast charge transfer in van der Waals heterostructures can effectively engineer the optical and electrical properties of two-dimensional semiconductors for designing photonic and optoelectronic devices. However, the nonlinear absorption conversion dynamics with the pump intensity and the underlying physical mechanisms in a type-II heterostructure remain largely unexplored, yet hold considerable potential for all-optical logic gates. Herein, two-dimensional ReSe2/ReS2 heterostructure is designed to realize an unusual transition from reverse saturable absorption to saturable absorption (SA) with a conversion pump intensity threshold of approximately 170 GW/cm2. Such an intriguing phenomenon is attributed to the decrease of two-photon absorption (TPA) of ReS2 and the increase of SA of ReSe2 with the pump intensity. Based on the characterization results of X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, femtosecond transient absorption spectrum, Kelvin probe force microscopy, and density functional theory calculation, a type-II charge-transfer-energy level model is proposed combined with the TPA of ReS2 and SA of ReSe2 processes. The results reveal the critical role of ultrafast interfacial charge transfer in tuning the unusual nonlinear absorption and improving the SA of ReSe2/ReS2 under different excitation wavelengths. Our finding deepens the understanding of nonlinear absorption physical mechanisms in two-dimensional heterostructure materials, which may further diversify the nonlinear optical materials and photonic devices.

Crystal growth, linear optical, thermal, mechanical and third-order nonlinear optical properties of 1,3-diphenyl prop‑2-en-1-one single crystals

This work brings out the viability of the chalcone derivative (E)-1,3-diphenyl-2-propen-1-one (DPP) for industrial applications in nonlinear optical technology and device fabrication, through investigations on its crystal structure and nonlinear optical properties. The unit cell features of the DPP single crystals grown by slow evaporation solution growth method have been determined and hkl values indexed. The optical transparency of DPP in the near infrared and visible range is found to be admirable and an optical bandgap of 3.42 eV is revealed in the UV–Vis-NIR analysis. The work hardening coefficient (n) of DPP, determined as 2 from Vickers microhardness measurement, shows the moderate mechanical strength of the crystal. The Laser Damage Threshold value of 3.9 GW/cm2 sheds light on the high tolerance of DPP to optical damage and suggests its suitability in device fabrication. The potential of DPP crystal in nonlinear optical applications is suggested from its superior value of 1.16×10−7 esu for third order susceptibility and appealing values of other nonlinear optical parameters.

Nonlinear optical research on 2D NbSe2 nanosheets and their ultrafast photonics applications

Two-dimensional (2D) NbSe2 is a new material with a variety of excellent properties. In this article, 2D NbSe2 nanosheets are prepared using liquid phase exfoliation (LPE) and spin coating methods. At the same time, the properties of NbSe2 were calculated by using density functional theory (DFT), exploring the changes in the electronic band structure of NbSe2 with the number of layers, and studying the optical properties of NbSe2. The nonlinear optical properties caused by the Pauli blocking effect and the absorption spectra are studied through typical nonlinear testing techniques and an ultraviolet–visible-near-infrared (UV–VIS-IR) spectrophotometer. In addition, 2 µm solid-state pulse lasers have important applications in a variety of fields. For the first time, 2D NbSe2 nanosheets are prepared as saturable absorbers (SA) and applied them to solid-state lasers as nonlinear optical modulation devices, successfully achieving the generation of ultra-short pulse lasers with a pulse duration of 445.4 ps in 2 µm band. Our research results prove that 2D NbSe2 nanosheets is a promising nanomaterial, can be prepared into nonlinear optical modulation devices with excellent performance, and show great application potential as ultrafast photonic devices. It is beneficial to the miniaturization of solid-state pulse lasers in subsequent applications.

Quantifying relaxation time constants in MoS2xSe2(1-x) alloys: Impact of Stoichiometry and Si/SiO2 interference

Despite a decade of extensive research on two-dimensional transition metal dichalcogenides, there are still some gaps in our understanding of their remarkable properties, limiting their potential applications. One such gap relates to the properties of these alloys, which offer tunable band gaps and can serve as the basis for various optoelectronic and nonlinear optical devices. A comprehensive understanding of the ultrafast charge carrier excitation and relaxation dynamics as well as their characteristic relaxation time constants, is crucial for the further use of these materials in specific applications. In this work, we experimentally investigate the dynamics of ultrafast relaxation processes in monolayer MoS2xSe2(1-x) alloys on a Si/SiO2 substrate using time-resolved spectroscopy. We determine the characteristic relaxation time constants for structures with different stoichiometric compositions and refine these constants by accounting for interference effects arising from the substrate.

Non-linear optical properties of hybrid materials of (OLi3) superalkali doped perylene diimide (PDI) derivative: comprehensively study via silico-technique

PDI-Imidazole and PDI-Imidazole combined with OLi3 (OLi3@PDI-Imidazole) were the two types of materials that we examined in this study to see how light behaved in each of the complex. To explore this, we employed the three different method such as rB3LYP/6–31G(d, p) DFT, CAM-B3LYP and WB97XD. The impact of PDI-Imidazole and OLi3@PDI-Imidazole geometries, maximum absorption ( λmax ), FMO, vertical ionization energies ( EVI ), Binding Energies ( Eb ), Hyperpolarizabilities, DOS, Dipole Moments (μ), ESP, EDDM, and Global Reactivity parameters have been examined. The type of contacts as well as the vibrational frequencies of PDI-Imidazole and OLi3@PDI-Imidazole were investigated using NCl, iso-surface, Raman spectroscopy, and IR research. The electron transport characteristics of the OLi3@PDI-Imidazole surface was significantly enhanced in comparison to the PDI-Imidazole surface by lowering the bandgap energies from 1.27 eV to 1.03 eV. In contrast to the pure PDI-Imidazole surface, which had lower values for linear polarizability ( α0 ) (547.08 au) and first hyperpolarizability ( β0 )(201.133au), OLi3@PDI-Imidazole surface displayed significant enhancements in linear polarizability ( α0 = 706.472 au) and first hyperpolarizability ( β0 = 21314.360 au). It was observed by TD-DFT calculations that all the compounds had appreciable improvements in their interaction energies, HOMO–LUMO and UV–vis absorption and vertical ionization potential. Future development of nonlinear optical (NLO) devices has been discovered to benefit from the addition of OLi3 to the PDI-Imidazole surface.

Manipulating four-photon absorption of ZnO via Ga doping.

Multi-photon absorption in the second near-infrared (NIR-II) regime has attracted extensive attention due to biological imaging and frequency-upconverted lasing applications. We report the dispersion of four-photon absorption (4 PA) response in pristine and Ga-doped ZnO single crystals over the spectral range 1180-1350 nm. Femtosecond Z-scan results demonstrate that Ga doping can significantly enhance the 4 PA coefficient β4 of ZnO. Interestingly, the wavelength dependency of β4 in Ga-doped ZnO shows a strong resonance around 1215-1250 nm, which is correlated with the PL peak of Ga-doped ZnO at 405 nm. Femtosecond pump-probe measurements validate that Ga doping has no profound impact on the ultrafast carrier relaxation of ZnO, indicating Ga doping leads to a shallow state rather than a deep trap within the bandgap. The possible mechanism of 4 PA enhancement induced by degeneracy with multi-photon absorption resonance to the Ga-doped state is discussed. Our results verify the strong potential of Ga-doped ZnO with tunable nonlinear optical properties as a promising candidate for nonlinear optical and nanophotonic devices in the NIR-II region.

Near-field enhancement of light by higher-order multipole excitations in a metal nanodisc trimer.

Near-field enhancement of light by dipole excitations in plasmonic nanoparticles plays an important role in many applications of optical nanotechnology, including solar cells, plasmonic sensors, and nonlinear optical devices. Recently, we have shown that a seemingly weak octupole resonance in a pair of metal nanospheres can provide a higher near-field enhancement than the dipole resonance. Being motivated by this discovery, we now design a plasmonic nanodisc trimer that supports hybridized higher-order excitations and simultaneously suppresses the dipole excitation. We show that, under these conditions, the near-field enhancement can reach a high level, exceeding the value achievable with a corresponding dimer structure. The interference of the electric currents belonging to different multipole moments is found to play an important role in the enhancement. We believe that arrays of similar metal nanostructures can be designed to enhance optical fields via higher-order resonances for many applications, e.g., in nonlinear optics and optical sensing based on surface-enhanced fluorescence or Raman scattering.

Physical, optical, spectroscopic features of Li2B4O7-Bi2O3-Sb2O3 glass system reinforced with molybdenum ions

To comprehend the physical, optical and spectroscopic properties of a novel multicomponent glass system with compositional formula 60Li2B4O7-30Bi2O3-(10-x)Sb2O3-xMoO3 (x = 0, 2.5, 5, 7.5 and 10 mol%) has been synthesized by melt quench process. The lack of intense peaks in the XRD confirmed the glassy nature of the prepared samples. On Substitution of Sb2O3 with MoO3 in lithium tetraborate-bismuthate glasses, a linear decrease in the density and an increase in the molar volume has been noticed. Physical parameters like oxygen packing density, oxygen molar volume and packing density have been computed. Optical energy bandgap evaluated from UV–Visible absorption spectra, declined with increase of MoO3. Refractive indices exhibited opposite trend with optical energy bandgap and opens applications for non-linear optical devices. Vibrational modes in the as-prepared glasses have been identified by FTIR and Raman spectra. With increase in MoO3 content, Mo6+ ions transformed to Mo5+ units which in turn converted BO4 to BO3 units as confirmed by FTIR and Raman spectroscopies.