Observation of nonstationary effects in saturation spectroscopy

We have studied the nonstationary effects in saturated absorption spectroscopy of the ⁸⁷Rb D₂ line. Varying the size of the σ⁺ polarized pump laser beam, we observed saturated absorption spectra for the σ^± polarized probe beam. For equal polarizations of the pump and probe beams, we found that the resonance signal for the F_g = 1 → F_e = 2 line, and the crossover lines between F_g = 1 → F_e = 2 and F_g = 1 → F_e = 1 (and 0) lines increased to a greater extent than the others. This observation can be understood from the calculated time evolution of the populations of the ground-state sublevels by means of a rate equation model. We also compared experimental data for other conditions with the calculated results. We found good agreement between the calculated results and the data.     

Structural and optical properties of thermal evaporated magnesium phthalocyanine (MgPc) thin films

X-ray powder diffraction (XRD) of MgPc indicated that the material in the powder form is polycrystalline with monoclinic structure. Miller indices, h k l, values for each diffraction peak in XRD spectrum were calculated. Thermal evaporation technique was used to deposit MgPc thin films. The XRD studies were carried out for MgPc thin films where the results confirm the amorphous nature for the as-deposited films. While, polycrystalline films orientated preferentially to (1 0 0) plane with an amorphous background were obtained for films annealed at 623 K for 3 h. Optical properties of MgPc thin films were characterised by using spectrophotometric measurements of transmittance and reflectance in the spectral range from 190 to 2500 nm. The refractive index, n, and the absorption index, k, were calculated. According to the analysis of dispersion curves, the parameters, namely; the optical absorption coefficient (α), molar extinction coefficient (?_molar), oscillator energy (E_os), oscillator strength (f), and electric dipole strength (q²) were also evaluated. The recorded absorption measurements in the UV-vis region show two well defined absorption bands of phthalocyanine molecule; namely the Q-band and the Soret (B-band). The Q-band showed its splitting characteristic (Davydov splitting), and ΔQ was obtained as 0.15 eV. The analysis of the spectral behaviour of the absorption coefficient (α), in the absorption region revealed indirect transitions. The transport and the near onset energy gaps were estimated as respectively 2.74 ± 0.02 and 1.34 ± 0.01 eV.     

Narrow band optical filter in fluorescein doped boric acid glass saturable absorber thin films

We demonstrate narrow band optical filter like frequency response with full width half maximum (FWHM) of nearly (1.75 ± 0.25) Hz in fluorescein doped boric acid glass films [10⁻⁴ M], using modulated optical phase conjugation and a nearly non-degenerate four wave mixing technique. Modulated optical phase conjugation signals are described in the limit of a weak probe and relatively strong pump beams. Both pump beams are of nearly equal intensity at a wavelength of 514.5 nm from a continuous-wave Ar⁺ laser. The probe beam frequency has been detuned with a ramp signal using a piezo electric mirror.     

Fourier transforms method for measuring thermal lens induced in diluted liquid samples

Drawing on interferometry and Fourier analysis, this paper describes the use of a two-beam thermal lens technique for measuring thermo-optical properties in optical materials. The procedure consists of yield interference patterns deformed by a localized photothermal effect. The photothermal phase shift is locally induced by the pump beam focused on a tested sample located on an on-axis probe beam, which is the first arm of a Mach-Zehnder interferometer. The plane where the effect is localized is imaged onto a CCD camera. Then two interferograms are recorded: one without effect and the other one with the induced photothermal phase. Fourier analysis performed on these interferograms allow us to plot the thermal lens map and, therefore, to estimate thermo-optic constant of Malachite Green in water solution. The method is applied to measure low linear absorptions of a diluted sample of Rhodamine B in water solution at 633 nm, showing that the proposed technique allows to measure photothermal phase shift as low as 3.1 mrad at 8 mW of input power in diluted materials.     

3,3′-Benzene-1,4-diylbis[1-(substituted)phenylprop-2-en-1-one] derivatives: A new class of materials for third-order nonlinear optical applications

We have investigated the third-order nonlinear optical parameters of Bischalcones embedded in DMF solution and in solid PMMA matrix, by Z-scan technique using nanosecond laser pulse trains at 532 nm. Z-scan results reveal that the Bischalcones exhibits negative nonlinear refractive index as high as 10⁻¹¹ esu. The molecular two-photon absorption cross-section of Bischalcones were of the order 10⁻⁴⁶ cm⁴ s/photon, which is nearly two orders of magnitude larger than that of Rhodamine 6G which is 10⁻⁴⁸ - 10⁻⁵⁰ cm⁴ s/photon. We found that, the two-photon absorption (TPA) is the dominating nonlinear process leading to nonlinear absorption in both the cases in solution and as well as in solid medium. Based on TPA process, the Bischalcones exhibit good optical power limiting of nanosecond laser pulses at the input wavelength. The nonlinear optical parameters found to increase on enhancing the strength of the electron donor groups indicating the dependence and importance of electron donor/acceptor units on third-order nonlinear optical susceptibility χ⁽³⁾.     

Time resolved magnetic ordering and photo-induced gyrotropy at room temperature in CdMgTe-CdMnTe semiconductor micro-cavities

Using a picosecond pump and probe time-resolved technique we evidence a single pump pulse photo-induced magnetic ordering in a Mn-doped semiconductor magneto-photonic microcavity operating in the strong coupling regime at room temperature. This nanosecond duration magnetization is attributed to a magnetic ordering of the Mn-impurities mediated through photo-generated holes and enhanced through the confinement. It is distinct from the preceding short lived photo-induced spin orientation of carriers also evidenced by our technique for circularly polarized pump beams. The photo-generated magnetic flux density amounts to a 1 kG for beam fluences of few tens μJ cm⁻² and effective Mn concentrations of 5 nm⁻³; large photo-induced magneto-optic Kerr rotations are also evidenced.     

Refractive index, oscillator parameters and temperature-tuned energy band gap of Tl4In3GaS8-layered single crystals

Transmission and reflection measurements in the wavelength region 450-1100 nm were carried out on Tl₄In₃GaS₈-layered single crystals. The analysis of the room temperature absorption data revealed the presence of both optical indirect and direct transitions with band gap energies of 2.32 and 2.52 eV, respectively. The rate of change of the indirect band gap with temperature dE_gi/dT=-6.0×10⁻⁴ eV/K was determined from transmission measurements in the temperature range of 10-300 K. The absolute zero value of the band gap energy was obtained as E_gi(0)=2.44 eV. The dispersion of the refractive index is discussed in terms of the Wemple-DiDomenico single-effective-oscillator model. The refractive index dispersion parameters: oscillator energy, dispersion energy, oscillator strength and zero-frequency refractive index were found to be 4.87 eV, 26.77 eV, 8.48×10¹³ m⁻² and 2.55, respectively.     

Nonlinear optical properties of periodic gold nanoparticle arrays

Periodic Au nanoparticle arrays were fabricated on silica substrates using nanosphere lithography. The identical single-layer masks were prepared by self-assembly of polystyrene nanospheres with radius R = 350 nm. The structural characterization of nanosphere masks and periodic particle arrays was investigated by atomic force microscopy. The nonlinear optical properties of the Au nanoparticle arrays were determined using a single beam z-scan method at a wavelength of 532 nm with laser duration of 55 ps. The results show that periodic Au nanoparticle arrays exhibit a fast third-order nonlinear optical response with the nonlinear refractive index and nonlinear absorption coefficient being n₂ = 6.09 × 10⁻⁶ cm²/kW and β = −1.87 × 10⁻⁶ m/W, respectively.     

Effect of nonlinear absorption in estimation of order of nonlinear optical process by fluorescence intensity

We report the effect of nonlinear absorption on the fluorescence signal. Attenuation of the incident beam intensity (I) in the medium due to nonlinear absorption reduces the fluorescence signal. We show that fluorescence signal proportional to I² is not always indicative of two-photon absorption process but such a dependence can be obtained for three or four-photon absorption process due to attenuation of the pump beam by nonlinear absorption. This reduction in the fluorescence signal due to nonlinear absorption is found to be more sensitive in the higher order nonlinear optical processes.     

Nonlinear optical properties in SrTiO3 thin films by pulsed laser deposition

Well-crystallized 250 nm-thick SrTiO₃ thin films on fused-quartz substrate were prepared by pulsed laser deposition. The band-gap of SrTiO₃ thin film by transmittance spectra is equal to 3.50 eV, larger than 3.22 eV for the bulk crystal. The nonlinear optical properties of the films were examined with picosecond pulses at 1.064 μm excitation. A large two-photon absorption (TPA) with absorption coefficient of 87.7 cm/GW was obtained, larger than 51.7 cm/GW for BaTiO₃ thin films. The nonlinear refractive index n₂ is equal to 5.7×10⁻¹⁰ esu with a negative sign, larger than 0.267×10⁻¹¹ esu for bulk SrTiO₃. The large TPA is attributed to intermediate energy levels introduced by the grain boundaries, and the optical limiting behaviors stemming from both TPA and negative nonlinear refraction were also discussed.     

Doppler spectroscopy of arbitrarily polarized light in rubidium

We present an experimental and theoretical study of the transmission of an arbitrarily polarized laser beam for a Doppler broadened rubidium vapor cell. As the polarization of the probe beam was varied from linear to circular, the transmission for the transitions F_g = 3 → F_e = 2, 3, 4 of the D₂ line of ⁸⁵Rb atoms was measured and compared with calculated results. In the calculation, the time-dependent absorption coefficient, calculated numerically from the density-matrix equation, was averaged over the velocity distribution and various transit time crossing the laser beam. The final transmission was obtained by considering the Gaussian profile of the laser beam. We found good agreement between experimental and calculated results.     

Optical band gap of zinc nitride films prepared on quartz substrates from a zinc nitride target by reactive rf magnetron sputtering

Polycrystalline zinc nitride films have been synthesized onto quartz substrates from the zinc nitride target and the nitrogen working gas by reactive rf magnetron sputtering at room temperature. X-ray diffraction study indicates that polycrystalline zinc nitride films are of cubic structure with the lattice constant a = 0.979(1) nm and have preferred orientations with (3 2 1) and (4 4 2). Its absorption coefficients as well as the film thickness are calculated from the transmission spectra, which are measured with a double beam spectrophotometer. The optical band gap has been determined from the photon energy dependence of absorption coefficient, an indirect transition optical band gap of 2.12(3) eV has been obtained.     

Analysis of all-optical light modulation in proteorhodopsin protein molecules

We present a detailed steady-state and time-dependent theoretical analysis of all-optical light modulation in the recently discovered, wild-type proteorhodopsin (WTpR) protein molecules based on excited-state absorption. Amplitude modulation of cw probe laser beam transmissions at 520, 405, 555 and 560 nm, corresponding to the peak absorption of pR, pR_M, pR_K and pR_N intermediate states of pR photocycle, respectively, by cw and pulsed modulating pump laser beam at 520 nm have been analyzed. The effect of various spectral and kinetic parameters on modulation characteristics has been studied. There is an optimum value of concentration for a given pump intensity value for which maximum modulation of the probe beam can be achieved. The switching characteristics of probe beam at 405 and 520 nm exhibit dip and peak, respectively, which can be removed by decreasing the absorption of pR_M state at 520 nm. The modulation in WTpR is at lower pump powers with smaller contrast in comparison to WT bacteriorhodopsin (bR) and WT pharaonis phoborhodopsin (ppR). The modulation characteristics exhibit unique features compared to bR and ppR.     

Measurement of nonlinear absorption coefficients in GaAs, InP and Si by an optical pump THz probe technique

An optical pump terahertz (THz) probe method for measuring carrier mobility and multiphoton absorption coefficients in semiconductors is demonstrated. A THz probe pulse is used to detect the transient photoconductivity generated by an optical pump pulse. The change in transmission coefficient at THz frequencies due to a pump pulse with photon energy greater than the band gap energy is used to determine the sum of electron and hole mobilities. The weak nonlinear absorption of a pump pulse with photon energy less than the band gap energy produces an approximately uniform free carrier distribution. The THz transmission coefficient vs. pump fluence, and the mobility, are used in a bulk photoconductivity model to determine the multiphoton absorption coefficients. For GaAs, InP and Si we find two photon absorption coefficients at 1305 nm of 42.5 ± 11, 70 ± 18 and 3.3 ± 0.9 cm/GW, respectively. For GaAs and InP we determine three photon absorption coefficients at 2144 nm of 0.19 ± 0.07 and 0.22 ± 0.08 cm³/GW².     

Enhanced four-wave mixing in mercury isotopes, prepared by stark-chirped rapid adiabatic passage

We demonstrate significant enhancement of four-wave mixing in coherently driven mercury isotopes to generate vacuum-ultraviolet radiation at 125 nm. The enhancement is accomplished by preparation of the mercury atoms in a state of maximum coherence, i.e. maximum nonlinear-optical polarization, driven by Stark-chirped rapid adiabatic passage (SCRAP). In this technique, a pump laser at 313 nm excites the two-photon transition between the ground state 6s²¹S₀ and the target state 7s ¹S₀ in mercury. A strong, off-resonant radiation field at 1064 nm generates dynamic Stark shifts. These Stark shifts serve to induce a rapid adiabatic passage process on the two-photon transition. During the process a coherent superposition of the two states is established, which enhances the nonlinear-optical polarization in the medium to the maximum possible value. The maximum coherence permits efficient four-wave mixing of a pump laser and an additional probe laser at 626 nm. The efficiency is further enhanced, as the SCRAP process allows to stimulate the complete set of different mercury isotopes to participate in the frequency conversion process. This enlarges the effective atomic density of the medium. Thus, we observe the generation of vacuum-ultraviolet radiation at 125 nm enhanced by more than one order of magnitude with respect to conventional frequency conversion. Parallel to the frequency conversion process, we monitored the evolution of the population in the medium by laser-induced fluorescence. These data demonstrate efficient coherent population transfer by SCRAP.     

The luminescence and optoelectrical properties of ITO films prepared by a sputter type negative metal ion deposition

Transparent conducting indium tin oxide (ITO) thin films were prepared on glass substrates by a magnetron sputter type negative ion source which requires cesium (Cs) vapor injection for surface negative ionization on the ITO target surface. Although the film was prepared at 70 °C, it attained high optical transmittance, 88% and low resistivity, 2.03 × 10⁻⁴ Ω cm, at an optimized Cs partial pressure of P_Cs = 1.7 × 10⁻³ Pa. The as-deposited ITO films have a poly-crystalline structure with (2 1 1), (2 2 2), (4 0 0), (4 1 1) and (4 4 0) reflections.Also, ITO films prepared at P_Cs = 1.7 × 10⁻³ Pa were post-deposition vacuum annealed at 300 °C for 30 min. The films had a resistivity of 1.8 × 10⁻⁴ Ω cm and a transparency of 89.2%. The post-deposition vacuum annealed ITO film was used as an anode for a transparent organic light emitting diode (TOLED). A maximum luminance of 19,000 cd/m² was obtained.     

Laser conditioning and nonlinear absorption of LaF3/MgF2 dielectric multilayers at 193 nm

A sensitive and simple pulsed surface thermal lens (TL) technique is used in situ to investigate the laser conditioning and to measure the nonlinear absorption of LaF₃/MgF₂ dielectric multilayers deposited on CaF₂ substrates at 193 nm. Due to the high single-shot sensitivity of the surface TL technique, the laser conditioning can be monitored from the first shot of irradiation on a shot-by-shot basis. The LaF₃/MgF₂ multilayers show a very strong conditioning effect. The ratio of the absorption before and after the laser irradiation is in the range 4–8 for a highly reflective (LH)²⁰ LaF₃/MgF₂ multilayer, and 3–4 for (1L3H)⁷ and (3L1H)⁷ multilayers. In comparison, a (LH)²⁰ LaF₃/AlF₃ multilayer shows only a weak conditioning effect, with an absorption ratio of approximately 1.4. Our experimental results suggest that the strong conditioning effect of the LaF₃/MgF₂ multilayer is due to the absorption conditioning of the LaF₃ layers. However, the MgF₂ layers are shown to be responsible for the considerable increase in LaF₃ absorption as well as the ability to condition the absorption. The fluoride multilayers present non-negligible nonlinear absorption and the two-photon absorption coefficient of the multilayers is estimated to be approximately 5×10^-7 cm/W. Received: 11 December 2000 / Accepted: 20 February 2001 / Published online: 25 July 2001     

Optical properties of Al-doped ZnO thin films by ellipsometry

Al-doped ZnO thin films (AZO) were prepared on Si (1 0 0) substrates by using sub-molecule doping technique. The Al content was controlled by varying Al sputtering time. The as-prepared samples were annealed in vacuum chamber at 800 °C for 30 min. From the XRD observations, it is found that all films exhibit only the (0 0 2) peak, suggesting that they have c-axis preferred orientation. The average transmittance of the visible light is above 80%. Spectroscopic ellipsometry was used to extract the optical constants of the films. The absorption coefficient and the energy gap were then calculated. The results show that the absorption edge initially blue-shifts and then red-shifts with increase of Al content.     

Nonlinear optical studies of 1-3-diaryl-propenones containing 4-methylthiophenyl moieties

The third-order nonlinear optical properties of chalcone derivatives have been studied using the single beam Z-scan technique. The dependence of χ⁽³⁾ on different donor and acceptor type substituents demonstrates the electronic nonlinearity of compounds. The largest value of nonlinear refractive index, n₂, measured for a high electron donor substituted molecule is −2.033 × 10⁻¹¹ esu. These molecules exhibit a strong two-photon absorption and interesting optical limiting of nanosecond laser pulses at 532 nm.     

The nonlinear refraction and absorption dependence on the thermal effect for 4 ns pulse duration in binuclear Zn(II) phthalocyanine solution

The influence of thermal effect on the third-order nonlinear optical properties of binuclear Zn(II) phthalocyanine in chloroform solution was studied. The nonlinear refraction and absorption of the sample was measured by using Z-scan technique with 4 ns laser pulses at 532 nm wavelength. The opposite signs of the effective nonlinear refraction index were observed by changing the focal length of focusing lens from 10 cm to 20 cm in the experimental setup. Changing the focusing lens increased the beam waist radius from 7 μm to 20 μm. The nonlinear absorption coefficient was reduced about 200 times based on changing the fluence or beam waist radius. The drastic changes in the third-order nonlinear optical parameters were attributed to thermal effect. To investigate the role of thermal effects even further the effective nonlinear refraction and absorption coefficients were studied by using different repetition rates, input powers and concentrations.