Off-resonant optical nonlinearities of phthalocyanine analogues: dihydroxy phosphorus(V) tetrabenzotriazacorroles

Third-order optical nonlinearity of a series phthalocyanine analogues, non-sulfonated {P(OH)₂TBC}, sulfonated {P(OH)₂TBCS_n} and isopropoxyl substituted {P(OH)₂TBC(OⁱPr)₄} dihydroxy phosphorus(V) tetrabenzotriazacorroles were measured by femtosecond degenerate four-wave mixing (DFWM) technique at 800 nm. Ultrafast off-resonant optical responses have been observed and the magnitude of the second-order hyperpolarizabilities of the phthalocyanine analogues were measured as high as (1.11-2.26) × 10⁻³¹ esu.     

Study of optical nonlinearity of functionalized multi-wall carbon nanotubes by using degenerate four wave mixing and Z-scan techniques

The phase conjugation geometry of degenerate four wave mixing (DFWM) technique has been employed to study the third-order optical nonlinear susceptibility (χ³) and second-order hyperpolarizability of multi-wall carbon nanotubes (MWCNTs). MWCNTs were grown by thermal chemical vapor deposition method and, subsequently functionalized with carboxylic acid group to improve their solubility in an organic solvent, ethylene glycol. The average hyperpolarizability for each carbon atom has been found to be 4.74 × 10⁻⁴⁶ m⁵/V² for the pump pulse of 8 ns at 532 nm. Decreasing the pulse width of the pump laser decreases the average value of hyperpolarizability. The absorption spectra show a monotonous increase from IR through visible and give an opportunity to estimate the imaginary part of the χ³ by the open aperture Z-scan technique.     

Analysis of degenerate four-wave mixing spectra of NO in a CH4/N2/O2 flame

4 /N₂/O₂ flame to spectral simulations based on a two-level theory for stationary, saturable absorbers by Abrams et al. Temperatures determined from least-squares fits of simulations to experimental spectra in the A²Σ⁺?X²Π⁺(0,0) band are compared to temperatures obtained from OH absorption spectroscopy and a radiation-corrected thermocouple. We find that DFWM rotational temperatures derived from Q-branch spectra agree with thermocouple and are independent of pump laser intensity for low to moderate saturation (I≈I_sat). However, the temperatures are systematically low and depend on pump intensity if the analysis neglects saturation effects. We demonstrate a method for obtaining an effective pump saturation intensity for use with the two-level model. This approach for analyzing saturated DFWM line intensities differs from previous work in that the use of the theory of Abrams et al. rather than a transition-dipole-moment power law allows treatment of a much wider range of saturation. Based on the observed signal-to-noise ratio an NO detection sensitivity of 25 ppm is projected, limited by a DFWM background interference specific to hydrocarbon flames. Received: 15 September 1998 / Revised version: 18 November 1998 / Published online: 24 February 1999     

Thermal grating and broadband degenerate four-wave mixing spectroscopy of OH in high-pressure flames

2 ∑–X²Π(0,0) band of OH has been studied in premixed methane/air flames using a cw Ar⁺ laser probe. Measurements of flame temperature and pressure were derived from fits of theoretical simulations to the observed time variation of signals over a pressure range of 10 to 40 bar and for different stoichiometry that were in agreement with independent measurements using N₂ CARS and predictions of a one-dimensional flame calculation. Broadband DFWM spectra in the same band of OH were observed up to a pressure of 9 bar, above which signals were obtained only from scattering from thermal gratings. Received: 10 November 1997/Revised version: 28 May 1998     

Detection of NO in a spark-ignition research engine using degenerate four-wave mixing

We report the first application of degenerate four-wave mixing (DFWM) to combustion diagnostics in a methane-fuelled internal combustion research engine. Combustion-generated NO in the spark-ignited engine was detected using scanning narrowband DFWM in a modified forward folded BOXCARS geometry. The resulting spectra of the X²Π-A²Σ⁺(0,0) band at 226 nm display an excellent signal-to-noise ratio. Extension of the technique to different engine operating conditions and to time-resolved multiplex DFWM is discussed. Received: 3 May 2001 / Revised version: 1 October 2001 / Published online: 29 November 2001     

Investigation of crystal structure and nonlinear optical properties of 2-methoxyanilinium nitrate

Single crystals of a new hybrid compound salt: 2-methoxyanilinium nitrate were prepared by slow evaporation at room temperature of diluted aqueous solutions containing 2-methoxyaniline with nitric acids. The compound crystallizes in a space group Pcab of orthorhombic system with cell parameters a = 8.8784 (6) Å, b = 10.6348 (7) Å, c = 18.3045 (7) Å, V = 1728.31 (17) ų at T = 100 K and Z = 8. The structure has been refined to an R-value of 0.044 for 1956 observed reflections using three-dimensional X-ray diffraction data. Third-order nonlinear optical susceptibility (χ^〈3〉) was measured by degenerate four wave mixing (DFWM) method at 532 nm. Third harmonic generation (THG) measurements at the 1064 nm were carried out for the 2-methoxyanilinium nitrate crystal with the following dimensions: 4 × 9 × 0.5 mm.     

Angular dependence of OH degenerate four-wave mixing signals in a flame

The dependencies of line intensity and linewidth of degenerate four wave mixing (DFWM) on the crossing angle have been investigated via OH A²Σ − X²Π transitions in a flame. The measured results were compared with the theoretical predictions and other experimental results. It was found that the saturation effect was important and must be considered. When using the DFWM method to measure the temperature, a suitable crossing angle should be chosen and the absorption correction should be taken into account.     

Experimental investigation of the effect of collisions and temperature on degenerate four-wave mixing

An experimental investigation (including a comparison with a simple theoretical model) of the effect of buffer-gas composition, pressure and temperature on resonant Degenerate Four-Wave Mixing (DFWM) has been performed. The DFWM signal from NO in a quartz cell was measured and the effect of quenching as well as elastic (phase-changing) collisions was studied by varying the total and partial pressures of N₂ and CO₂ as buffer gases. It was found that the DFWM signal first slowly increased with buffer-gas pressure (up to 10 mbar) and then rapidly decreased. It was furthermore found that the DFWM signal was considerably less sensitive to quenching collisions as compared to Laser-Induced Fluorescence (LIF) (for laser intensities approximately equal to half the DFWM saturation intensity of the transition). On the other hand, while LIF is virtually insensitive to elastic collisions, DFWM displays a larger sensitivity to elastic collisions than to quenching collisions. The DFWM saturation intensity was found to increase with buffer-gas pressure (although slower than expected). When varying the temperature of the gas composition, it was found that the DFWM signal decreased markedly with increasing temperature. This decrease is too fast to be explained solely by a change in the population of the molecular state probed by the laser.     

Nonlinear optical studies of a newly synthesized copolymer containing oxadiazole and substituted thiophenes

We investigated the third-order nonlinear optical properties of a newly synthesized soluble copolymer containing oxadiazole and thiophene units using Z-scan and Degenerate Four Wave Mixing (DFWM) techniques. The measurements were performed at 532 nm with 7 ns pulses from a Nd:YAG laser. We found a good agreement between the values of χ⁽³⁾ determined from both experiments. Z-scan results indicate a negative nonlinear refractive index, n₂, whose magnitude is of the order of 10⁻¹⁰ esu. The copolymer exhibits strong nonlinear absorption and good optical limiting properties at 532 nm, and hence may be a potential material for optical limiting applications.     

Third-order optical nonlinearities of α,ω-dithienylpolyenes and oligo(thienylvinylene)

α,ω-Dithienylpolyenes and oligo(thienylvinylene) are interesting third-order nonlinear optical materials for a variety of device applications. To better understand the third-order nonlinear response of these materials, the third-order susceptibilities (χ⁽³⁾) and nonlinear absorption behaviors of two α,ω-dithienylpolyenes with different conjugation length and two oligo(thienylvinylene) with different substituents on the thiophene rings have been studied using degenerate four wave mixing (DFWM) and nonlinear transmission techniques at 532 nm. The χ⁽³⁾ values of 1×10⁻³ mol/l solutions are all of the order of 10⁻¹³ esu. The χ⁽³⁾ values increase with the increase of the linear absorption coefficient. In addition, these compounds exhibit reverse saturable absorption for nanosecond laser pulses. The strength of reverse saturable absorption varies when the conjugation length and substituents change. Moreover, the nonlinear absorption characteristics of these compounds in the picosecond regime differ from those in the nanosecond regime. The different nonlinear absorption behavior is due to the relative contributions from excited singlet–singlet and triplet–triplet absorption. The strong reverse saturable absorption characteristics of two of the compounds suggest that they could be potential candidates for optical limiting applications in the nanosecond regime.     

偶氮材料中双波长共存的图象研究

测量了偶氮材料MO/PVA和EO/PVA的光致双折射,其值约为δ_n=2.7×10^-3.在同偏振态两路简并四波混频光同时作用于样品同一区域的条件下,研究了该材料的双波长共存特性,记录了光点存储和图象存储,并分析了双波长共存的竞争机制.     

Characteristics of degenerated four wave mixing in ZnS/CdSe/ZnS quantum dot quantum well with multi-shell structure

The wave functions and eigenenergies of electrons in ZnS/CdSe/ZnS cylindrical quantum dot quantum well (QDQW) have been calculated by solving a three-dimensional nonlinear Schrödinger equation, in the framework of the effective-mass envelope-function theory. The third-order susceptibilities of the degenerated four waves mixing (DFWM) have been calculated theoretically by means of compact density matrix. The third-order susceptibilities as the function of the shell radius R₂, R₃ have been analyzed. The results show that the magnitude of nonlinear susceptibility is increased with the increasing of well radius. The resonance frequency of the photon have a shift when R₂ or R₃ is increasing and the relation between nonlinear susceptibility and relaxation time has also been studied.     

Rotational and vibrational temperature determination by DFWM spectroscopy

Using the DFWM technique we determined rotational and vibrational temperatures of NaH molecules in a dynamical system consisting of NaH, Na, H and H₂ for several heat-pipe oven temperatures. We applied a new way to determine the dependence of the DFWM signalI _c ^int on the power of the transition dipole momentµ without previous knowledge of the temperature. The revealed dependence isI _c ^int µ ⁴. In this case the laser intensities were found to be of the same order as the saturation intensity in accordance with simple DFWM theory. A usual Boltzmann plot was employed for the determination of the relevant rotational temperatures, which displayed higher values than the oven temperature.     

Nonlinear optical properties and phase-relaxation processes in single-walled carbon nanotubes

We have investigated third-order nonlinear optical properties of bundled and isolated semiconducting single-walled carbon nanotubes (SWNTs) by means of Z-scan method, pump-probe method, and two-beam time-resolved degenerate four-wave mixing (DFWM) method. The figures of merit Im χ⁽³⁾/α in both bundled and isolated SWNTs samples were found to be enhanced with increasing tube diameter. The measured Im χ⁽³⁾/α value in the bundled SWNTs was an order of magnitude smaller than that in the isolated SWNTs. Both population relaxation time T₁ and phase-relaxation time T₂ for bundled samples were smaller than those in the isolated samples. These experimental results can be explained by an increase in nonradiative recombination rate and phase-relaxation rate in the bundled sample. The phase-relaxation time T₂ is considered to have a significant role in the enhancement of Im χ⁽³⁾/α.     

High-resolution degenerate four-wave-mixing spectroscopy of OH in a flame with a novel single-mode tunable laser

The first application of a novel single-mode tunable laser system to nonlinear spectroscopy is reported. The device uses a modeless dye laser, pumped by a single longitudinal mode (SLM) Q-switched Nd:YAG laser, as a narrow-bandwidth amplifier of the output of a SLM diode laser. The system provides pulses of 5-ns duration, 30-mJ energy and 165-MHz spectral line width tunable in the range 632–639 nm at 10-Hz repetition rate. The frequency-doubled output of the laser is used to record spectral line shapes of degenerate four wave mixing (DFWM) signals from the P₁(15) line of the A²–X² (0,0) band of OH in a methane/oxygen flame. Pressure broadening of the DFWM line shape is studied for the first time in a low-pressure flame and a pressure-broadening rate of 1.31±0.09×10^-4 cm^-1/Torr is derived from the data. Power-broadening effects are measured and compared with predictions of the standard perturbative model and of an analytical solution derived from a non-perturbative treatment of DFWM with arbitrary pump and probe intensities. PACS 42.55.Px; 42.62.Fi; 42.65.-k     

Optical phase-conjugation in erioglaucine dye-doped thin film

Optical phase-conjugation (OPC) has been demonstrated in erioglaucine (acid blue 9) dye-doped gelatin films via continuous-wave degenerate four-wave mixing (DFWM) using a low-power He-Ne laser at 633 nm. DFWM and holographic processes are found to contribute to the observed phase-conjugate signal. A maximum phase-conjugate beam reflectivity of about 0.24% has been observed in these dye-doped gelatin films.     

Search for high-spin states in29Si using a neutron time-of-flight spectrometer

The²⁶Mg(α,nγ) reaction has been used in connection with a neutron time-of-flight spectrometer to search for high spin states in²⁹Si betweenE _x =8.4 and 11.4 MeV. The γ-decay of twenty levels has been observed. Nine levels have not been observed before. A candidate for theJ ^π=13/2^?,K=7/2 state has been located with theE _x =8761 keV level.     

Newβ-delayed proton precursor135Gd

Unknownβ-delayed proton precursor¹³⁵Gd has been synthesized by the reaction¹⁰⁶Cd (³²S, 3n) and identified using a helium-jet recoil fast tape-transport system with aγ(X)-p coincidence measurements. Itsβ-delayed proton spectrum has been observed. The half-life of¹³⁵Gd decay has been determined to be 1.1±0.2 s.     

Investigation of states in 30P via the 30Si(3He,t)30P reaction at 30 MeV

The ³⁰Si(³⁰He, t)³⁰P reaction has been measured for about 100 levels in ³⁰P with E_x < 8.8 MeV. Little selectivity in the population of states has been observed. For 75 levels angular distributions have been analysed using a “fingerprint method” by determining the L-value from a comparison in shape with transitions to states with known J^π. For possible mixed L-transitions a dominance of the higher L-value is observed for almost all cases. Coulomb displacement energy calculations utilizing shell-model wave functions have been used to identify T = 1 states.     

Collective and intrinsic structures in 183W

The structure of ¹⁸³W has been studied by employing the ¹⁷⁶Yb(¹⁴C,α3n) reaction at 68 MeV. Five previously known rotational structure with one-quasiparticle configurations have been extended to higher spin states, and five new rotational bands with three- and five-quasiparticle configurations and a γ-vibration of a one-quasiparticle structure have been newly identified. In the ν7/2⁻[503] and ν11/2⁺[615] rotational structures, a signal of an admixture of an octupole-vibrational structure has been observed in their in-band B(M1)/B(E2) ratios and g_K factors. In the K^π=19⁻ rotational band, a Coriolis effect on the ν1/2⁻[510] neutron has been identified. In all, 17 K-forbidden transitions have been observed. Energies of intrinsic states below 4 MeV have been calculated based on the Blocked BCS theory, and they are used in support of the configuration assignments.