Structure,electronic,and nonlinear optical properties of superalkaline M_(3)O(M=Li,Na)doped cyclo[18]carbon

Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic structure.Superalkalis have low ionization energy.Doping a superalkali in cyclo[18]carbon is an effective method to improve the optical properties of the system because considerable electron transfer occurs.In this paper,the geometry,bonding properties,electronic structure,absorption spectrum,and nonlinear optical(NLO)properties of superalkaline M_(3)O(M=Li,Na)-doped cyclo[18]carbon were studied by using density functional theory.M_(3)O and the C_(18) rings are not coplanar.The C_(18) ring still exhibits alternating long and short bonds.The charge transfer between M_(3)O and C_(18) forms stable[M_(3)O]+[C_(18)]-ionic complexes.C_(18)M_(3)O(M=Li,Na)shows striking optical nonlinearity,i.e.,their first-and second-order hyperpolarizability(βvec andγ||)increase considerably atλ=1907 nm and 1460 nm.

Electrical and nonlinear optical properties of TGZO transparent conducting films deposited by magnetron sputtering

Thin transparent oxide conducting films(TCOFs)of titanium and gallium substituted zinc oxide(TGZO)were fabricated via radio frequency(RF)magnetron sputtering technique.The effects of RF power on electrical,linear and nonlinear optical characteristics were investigated by Hall tester,Ultraviolet(UV)-visible spectrophotometer and optical characterization method.The results indicate that RF power significantly influences the electrical and optical properties of the deposited films.As RF power raises,the resistivity and Urbach energy fall initially and then rise,while the figure of merit,mean visible transmittance and optical bandgap show the reverse variation trend.At RF power of 190 W,the TGZO sample exhibits the highest electro-optical properties,with the maximum figure of merit(1.14×10^(4)Ω-1∙cm^(-1)),mean visible transmittance(86.9%)and optical bandgap(3.50 eV),the minimum resistivity(6.26×10^(-4)Ω∙cm)and Urbach energy(174.23 meV).In addition,the optical constants of the deposited films were determined by the optical spectrum fitting method,and the RF power dependence of nonlinear optical properties was studied.It is observed that all the thin films exhibit normal dispersion characteristics in the visible region,and the nonlinear optical parameters are greatly affected by the RF power in the ultraviolet region.

All-optical switching and nonlinear optical properties of HBT in ethanol solution

This paper demonstrates an all-optical switching model system comprising a single pulsed pump beam at 355 nm and a CW He-Ne signal beam at 632.8 nm with 2-（2＇-hydroxyphenyl）benzothiazole （HBT） in ethanol solution. The origins of the optical switching effect were discussed. By the study of nonlinear optical properties for HBT in ethanol solvent, this paper verified that the excited-state intramolecular proton transfer （ESIPT） effect of HBT and the thermal effect of solvent worked on quite different time scales and together induced the change of the refractive index of HBT solution, leading to the signal beam deflection. The results indicated that the HBT molecule could be an excellent candidate for high-speed and high-sensitive optical switching devices.

The Third-Order Nonlinear Optical Properties in Cobalt-Doped ZnO Films

We quantitatively investigate the third-order optical nonlinear response of Co-doped ZnO thin films prepared by magnetron sputtering using the Z-scan method. The two-photon absorption and optical Kerr effect are revealed to contribute to the third-order nonlinear response of the Co-doped ZnO films. The nonlinear absorption coefficient β is determined to be approximately 8.8 × 10-5 cm/W and the third-order nonlinear susceptibility X（3） is 2.93 × 10-6 esu. The defect-associated energy levels within the band gap are suggested to be responsible for the enhanced nonlinear response observed in Co-doped ZnO films.

UV-Vis Spectrum and the Third-order Nonlinear Optical Properties of the Chiral Camphorderived β-diketonate Platinum Complexes

UV-Vis spectrum and the third-order nonlinear optical properties of the chiral camphor-derived β-diketonate have been studied at the B3LYP/6-31G＊ level. The results showed that the introduction of electron-drawing group -CF3 and -C3F7 on β-diketonate made the strongest absorption peak red-shift and the lowest energy absorption blue-shied. Introduction of -OC2H5 on the benzene or pyridine ring made the lowest energy absorption blue-shift. When the -C2H3 was introduced on the benzene or pyridine ring, the lowest energy absorption was red-shifted. Introduction of electron-donating group on β-diketonate can enlarge their nonlinear optical properties. On the contrary, the introduction of electron-drawing group dropped it down.

Theoretical Investigation on Structures and Second-order Nonlinear Optical Properties of (Thiophene) Manganese Tricarbonyl Cations

The structures of several recently reported organometallic NLO chromophores, (thio-phene) manganese tricarbonyl cations, were fully optimized at the DFT non-local (GGA) level. The calculated results show that the fragments 2-SC4H3CH=CHC6H4-R in these organometallic chromophores are not planar with dihedral angles of 42.2~59.8 between two aromatic rings, which are different from those of uncoordinated counterparts. Based on the DFT geometry opti-mization, the second-order nonlinear optical polarizabilities were calculated by using RPA method. The calculated results indicate that incorporation of +3Mn(CO) unit with thiophene leads to a sub-stantial increase in the second-order polarizability (b).

First-principles study of structure and nonlinear optical properties of CdHg(SCN)_4 crystal

The geometric structure,electronic structure,and optical properties of CdHg（SCN）4 crystal are calculated by using the density functional perturbation theory and Green function screening Coulomb interaction approximation.The band gap of CdHg（SCN）4 crystal is calculated to be 3.198 eV,which is in good agreement with the experimental value 3.265 eV.The calculated second-order nonlinear optical coefficients are d14 = 1.2906 pm/V and d15 = 5.0928 pm/V,which are in agreement with the experimental results（d14=（1.4 ±0.6） pm/V and d15=（6.0 ±0.9） pm/V）.Moreover,it is found that the contribution to the valence band mainly comes from Cd-4d,Hg-5d states,and the contributions to the valence band top and the conduction band bottom predominantly come from C-2p,N-2p,and S-3p states.The second-order nonlinear optical effect of CdHg（SCN）_4 crystal results mainly from the internal electronic transition of（SCN）^-.

Linear and nonlinear optical properties of Sb-doped GeSe_2 thin films

Sb-doped GeSe2 chalcogenide thin films are prepared by the magnetron co-sputtering method. The linear optical properties of as-deposited films are derived by analyzing transmission spectra. The refractive index rises and the optical band gap decreases from 2.08 eV to 1.41 eV with increasing the Sb content. X-ray photoelectron spectra further confirm the formation of a covalent Sb--Se bond. The third-order nonlinear optical properties of thin films are investigated under femtosecond laser excitation at 800 nm. The results show that the third-order nonlinear optical properties are enhanced with increasing the concentration of Sb. The nonlinear refraction indices of these thin films are measured to be on the order of 10-18 m2/W with a positive sign and the nonlinear absorption coefficients are obtained to be on the order of 10-10 m/W. These excellent properties indicate that Sb-doped Ge-Se films have a good prospect in the applications of nonlinear optical devices.

THIRD ORDER NONLINEAR OPTICAL PROPERTIES OF PERNIGRANILINE SOLUTION IN CONCENTRATED SULFURIC ACID

The fully oxidized state of polyaniline (PANI), pernigraniline (PN), was synthesized by oxidation of the emeraldine base form of PAM dissolved in NMP solvent with m-chloroperoxybenzoic acid. The resulted PN was characterized by FTIR and UV-Visible spectra. The third-order nonlinear optical properties of PN in concentrated sulfuric acid (PN/H2SO4) were measured by a degenerated four wave mixing (DFWM) method. The results obtained suggest that the soliton-pair intermediate state associated with the degenerated state does not play a major role in the third order nonlinear optical properties of PANI.

Effects of built-in electric field and donor impurity on linear and nonlinear optical properties of wurtzite InxGa1-xN/GaN nanostructures

The linear and nonlinear optical absorption coefficients(ACs)and refraction index changes(RICs)of 1s-1p,1p-1d,and 1f-1d transitions are investigated in a wurtzite InxGa1-xN/GaN core-shell quantum dot(CSQD)with donor impurity by using density matrix approach.The effects of built-in electric field(BEF),ternary mixed crystal(TMC),impurity,and CSQD size are studied in detail.The finite element method is used to calculate the ground and excited energy state energy and wave function.The results reveal that the BEF has a great influence on the linear,nonlinear,and total ACs and RICs.The presence of impurity leads the resonant peaks of the ACs and RICs to be blue-shifted for all transitions,especially for 1s-1p transition.It is also found that the resonant peaks of the ACs and RICs present a red shift with In-composition decreasing or core radius increasing.Moreover,the amplitudes of the ACs and RICs are strongly affected by the incident optical intensity.The absorption saturation is more sensitive without the impurity than with the impurity,and the appearance of absorption saturation requires a larger incident optical intensity when considering the BEF.

SECOND ORDER NONLINEAR OPTICAL PROPERTIES OF DICYANOPYRAZINES

Second order nonlinear optical active 2,3-dichloro-5,6-dicyanopyrazine (DCDCP) and its monoamine-substituted derivatives had been synthesized. Their facile synthesis, high melt point, high incidence af substantial SHG activity and increased transparency inthe blue and near infrared make this class compounds appealling for further investigation.

Theoretical Investigation on the Second-order Nonlinear Optical Properties of Chiral Amino Acid Zinc(Ⅱ) Porphyrins

Static second-order nonlinear optical effects of amino acid zinc(II) porphyrins 1, 2, 3 and 4 were calculated by the TDHF/PM3 method based on the molecular structures optimized at the semiempirical PM3 quantum chemistry level, showing due to the cancellation of symmetric center, these amino acid zinc(II) porphyrins exhibit second order nonlinear optical response. The analysis of β components indicated that these amino acid zinc(II) porphyrins are of multipola- rizabilities, and they may be ascribed as the “mixture” of octupolar and dipoar molecules with ||βJ=3||/||βJ=1|| ≈ 5. It is found that there are no significant differences between the static β values of non-chiral and chiral amino acid zinc(II) porphyrins. However, the βxyz component, which is quite important to quadratic macroscopic χ (2) susceptibility of chiral material, is increased significantly with the increase of side chain group of amino acids.

Nonlinear optical properties of novel H-shaped chromophores

Novel and effective H-shaped chromophores were doped into polymethyl methacrylate （PMMA） to form guest-host polymer thin films. The measurement results of Maker fringe method show that the polymer thin films containing the H-shaped chromophores as a guest exhibit high second harmonic coefficients （d33） compared with other two-dimensional chromophores.

Nonlinear Optical Properties of Tri-nuclear Transition Metal Clusters M-(μ-S)s-M'(M=Mo,W;M'=Cu,Ag,Au)

The static polarizabilities and the second-order hyperpolarizabilities of a series of tri-nuclear metal cluster models MS4(MPPh3)2(MPPh3) (M=Mo,W; M=Cu, Ag, Au) have been calculated within the first-principle theoretical framework. The model clusters have two fragments of rhombic units and it is the charge transfer from one of these moieties to the other that is responsible for nonlinear optical property. This kind of electronic delocalization, differentiated from that of planar p-system, is very interesting and is worthy for further investigation.

Preparation of Organic Nanoparticle Colloids by Laser Ablation and Their Nonlinear Optical Properties

Suspension of micrometer-sized 1,4-bis（4-methylstyryl）benzene（p-MSB） was converted into colloidal nanocrystal solution by irradiation with an femtosecond laser（800 nm, 1 kHz）. The prepared nanocrystals were rectangular with ca. 100 nm in size. The same crystal structure as that of bulk crystals was confirmed by X-ray diffraction measurement. UV-Vis spectra and emission spectra of the nanoparticle dispersions in dichloromethane（poor solvent） were examined. The nanocrystal exhibits large quantum yield（89%）. The nonlinear optical properties of the nanocrystals were further studied by Z-scan technique with femtosecond laser duration of 120 fs at a wavelength of 800 nm. The results show that the nanocrystals exhibit strong nonlinear absorption.

Crystal Structure and Third order Nonlinear Optical Properties of cis-Configuration Biferrocene Trinuclear Complexes

The syntheses and characterization of novel biferrocene trinuclear complexes of Schiff base ligand, S methyl N (ferrocenyl 1 methyl methylidene)dithiocarbazate [hereafter abbreviated as HL (1)], are described. The X ray diffraction studies have established the structures of PdL 2 (3) and CuL 2 (4). The geometry of Pd(Ⅱ) in (3) is close to a square plane and in the novel cis configuration the two ferrocene moieties are in cis configuration, while that of Cu(Ⅱ) in (4) is close to a tetrahedral configuration. The electrochemical measurements suggested that the square planar configuration of Ni(Ⅱ) and Pd(Ⅱ) moieties can effectively transmit the redox effects of the ferrocene moieties, while the tetrahedral configuration of the Cu(Ⅱ) complex can not transmit the redox effects. The degenerate four wave mixing (DFWM) measurements showed that the complexes exhibit obviously nonlinear optical (NLO) response. The magnitude of their third order NLO susceptibility can be explained by their structure and electrochemical properties.

Fabrication of amorphous nanoporous ZrO_(2)/SiO_(2) aerogel enabling nonlinear optical properties

Amorphous oxides have unique physicochemical properties with extensive opto-electronic applications such as the thin-film transistor,light-emitting diode backplanes,and supercontinuum generation.In this contribution,we synthesize the amorphous ZrO_(2)/SiO_(2) nanoporous aerogel with high structural integrity.With the femtosecond excitation laser at 800–1,064 nm,the broadband second harmonic generation is observed.The nonlinear optical properties of the as-prepared ZrO_(2)/SiO_(2) aerogel are investigated at 1.0μm and 1.5μm for the first time.Subsequently,the amorphous ZrO_(2)/SiO_(2) saturable absorber is originally applied in the Yb-doped and Er-doped fiber lasers to realize the mode-locking operations.In the Yb-doped fiber laser,the dissipative soliton resonance mode-locking operation is demonstrated with the largest pulse duration of 22 ns at a repetition rate of 7.8 MHz and a high signal-to-noise ratio of 64 dB.In the Er-doped fiber laser,a conventional soliton mod-locking regime is observed with an ultrashort pulse width of 960 fs,a repetition frequency of 6.55 MHz,and a time-bandwidth production of 0.347.Our work shows the good ability of the ZrO_(2)/SiO_(2) aerogel in generating ultrafast pulses and extends the saturable absorber into the amorphous material realm.

Effect of Ba/Sr ratio on the nonlinear optical properties of Ba_(1-x)Sr_(x)TiO_(3)(x = 0.1–0.9) thin films

Perovskite-structured barium strontium titanate[Ba_(1-x)Sr_(x)Ti O_(3),x=0.1–0.9] films have been epitaxially fabricated by using a pulsed-laser deposition technique.The third-order nonlinear optical properties were studied through a z-scan method,allowing the resolution of the nonlinear refractive and absorptive contributions to the responses.Although all the samples show almost the same value of nonlinear absorption coefficient,the extracted nonlinear refractive index of the sample of x=0.3 is apparently larger than that of other samples.Dependency of the nonlinear optical properties on the Ba/Sr ratio is discussed in terms of the crystal phase transformation and metal-oxygen bond length of the selected materials.

Nonlinear optical properties of integrated GeSbS chalcogenide waveguides

In this paper, we report the experimental characterization of highly nonlinear GeSbS chalcogenide glass waveguides. We used a single-beam characterization protocol that accounts for the magnitude and sign of the real and imaginary parts of the third-order nonlinear susceptibility of integrated Ge23Sb7S70 （GeSbS） chalcogenide glass waveguides in the near-infrared wavdength range at λ = 1580 nm. We measured a waveguide nonlinear parameter of 7.0 4- 0.7 W-1 · m-1, which corresponds to a nonlinear refractive index of n2 =（0.93 ± 0.08） ×10-18 m2/W, comparable to that of silicon, but with an 80 times lower two-photon absorption coefficient βTPA = （0.010± 0.003） cm/GW, accompanied with linear propagation losses as low as 0.5 dB/cm. The outstanding linear and nonlinear properties of GeSbS, with a measured nonlinear figure of merit FOM TPA = 6.0 ± 1.4 at λ = 1580 nm, ultimately make it one of the most promising integrated platforms for the realization of nonlinear functionalities.

Effect of Surface Roughness on Laser Induced Nonlinear Optical Properties of Annealed ZnO Thin Films

Variation of nonlinear optical properties with surface roughness of ZnO thin films deposited on coming glass substrates at different annealing temperature （TA） was reported. The films were characterized by X-ray diffraction （XRD）, UV-Vis-NIR transmission and single beam z-scan technique using second harmonics of Nd：YAG laser. Surface morphology of the samples was investigated by atomic force microscopy （AFM）. Surface roughness was found minimum （8.4 nm） for ZnO sample annealed at 450℃. The nonlinear optical properties （NLO） were found to be dependent on surface roughness and the highest value of third order nonlinear susceptibility （X（3）=4.3x 10-7 esu） was obtained for ZnO at TA 450℃.