Temperature dependence of rectification and photovoltaic effects in regioregular poly(3-alkylthiophene) films at the Schottky junction with Al electrode

Current–voltage (I–V) characteristics of regioregular (head–tail) poly(3-hexylthiophene), HT-PHT films in the sandwich cell structure of Al/HT-PHT/Au have been studied as a function of temperature. The cells showed typical rectification characteristics with the ratio of more than 10³, indicating the formation of the Schottky type junction at the interface of Al/HT-PHT. The temperature dependence of I–V characteristics at the forward biases are discussed with the bulk property of the HT-PHT. The reversed current and its characteristics are discussed taking the thermionic emission and diffusion models at the junctions of Al/HT-PHT into consideration.     

Decay of orientational grating of weakly confined excitons in GaAs thin films

We report the dynamical properties of the exciton orientation in GaAs thin films using the orientational grating (OG) technique. From the results of excitation-power dependence of OG signal, we confirmed that the OG signal comes from the optical nonlinearity of weakly confined excitons. In addition, the OG-decay time decreases with an increase of excitation power due to exciton–exciton interaction, and the shortest decay time is below 1 ps. Our results may imply the potential application of optical nonlinearity of weakly confined exciton to ultrafast switching devices operating at 1 Tbit/s.     

Third-order nonlinear optical response in transparent solids using ultrashort laser pulses

The third-order optical nonlinearity, χ ⁽³⁾, is measured in transparent glasses (BK7 and fused silica) and crystals (BaF₂ and quartz) using 36-fs, 800-nm laser pulses and the optical Kerr gate (OKE) technique; values are found to lie in the range 1.3–1.7×10^-14 esu, in accordance with theoretical estimates. We probe the purely electronic response to the incident ultrashort laser pulse in fused silica and BK7 glass. In BaF₂ and quartz, apart from the electronic response we also observe contribution from the nuclear response to the incident ultrashort pulses. We observe oscillatory modulations that persist for ～400 fs. The response of the media (glasses and crystals) to ultrashort pulses is also measured using two-beam self-diffraction; the diffraction efficiency in the first-order grating is measured to be in the range of 0.06–0.13 %. Third harmonic generation due to self-phase matching in the transient grating geometry is measured as a function of temporal delay between the two incident ultrashort pulses, yielding the autocorrelation signal.     

Exciton-electron interaction in quantum wells with a two dimensional electron gas of low density

II–VI quantum-well structures containing a 2DEG of low density have been investigated by means of polarized photoluminescence, photoluminescence excitation and reflectivity in external magnetic fields up to 20 T. The spin splittings of the exciton X and the negatively charged exciton X ⁻ are measured as a function of the magnetic field strength. The behavior of the magnetic-field-induced polarization degree of the luminescence line related to X ⁻ demonstrates the formation process of negatively charged excitons from excitons and free carriers polarized by the external magnetic field. We have determined the binding energies of the trion formed either with the heavy-hole or the light-hole exciton. The optically detected magnetic resonance (ODMR) technique was applied for the first time to study the optical transition processes in a nanosecond timescale. The electron ODMR was observed with the detection on either the direct exciton or the negatively charged exciton X. Further evidence for the interaction of excitons with the electrons of the two-dimensional gas are demonstrated by a combined exciton-cyclotron resonance line observed in reflectivity and luminescence excitation, shake-up processes observed in photoluminescence, as well as inelastic and spin-dependent scattering processes. Fiz. Tverd. Tela (St. Petersburg) 41, 831–836 (May 1999) Published in English in the original Russian journal. Reproduced here with stylistic changes by the Translation Editor.     

Nonlinear optical properties of biexciton states in GaN quantum disks

The ground state energy of an exciton and biexciton states, in a GaN/Al_xGa_1-xN quantum disk are investigated by the variation method, within envelope function and effective mass approximations. Exciton and biexciton binding energy, and the dipole moments related to the transition between ground, exciton and biexciton states, are calculated as a function of quantum disk geometry. The optical nonlinearity via the exciton and biexciton states is studied on the basis of a three level model through the density matrix formalism. The behavior of different terms of third order susceptibility χ⁽³⁾, are studied around resonance frequencies and for different geometries of disk. The effect of values of the decay rates on χ⁽³⁾ are studied. It is found that these values have remarkable effect on the second term of, χ⁽³⁾.     

Synthesis and nonlinear optical properties of branched pyrroline chromophores

New tricyanopyrroline (TCP) chromophores with rigid–flexible dendron were prepared for second‐order nonlinear optical (NLO) application. The chromophores were fully characterized using ultraviolet‐visible spectroscopy, nuclear magnetic resonance spectroscopy and mass spectrometry. Thermal gravimetric analysis (TGA) revealed that the chromophores had excellent thermal stability. Large λ_max and high solvate chromic effects revealed that the chromophores had large second‐order optical nonlinearity. The electro‐optic coefficients (r₃₃) were measured in the chromophores‐doped poly(bisphenol A carbonate) films at the fundamental wavelength of 1310 nm, and the highest γ₃₃ achieved was 217 pmV^?1. Copyright © 2010 John Wiley & Sons, Ltd.     

Dynamics of nonlinear optical response of CuBr-doped glasses

Nonlinear absorption of the Z_1,2 exciton band in CuBr-doped glasses was observed at band-to-band excitation and described in terms of damping of the Lorentzian-shaped band. Microcrystal-radius dependent time evolution of the nonlinearity was investigated, and the full recovery of initial absorption was observed to be as short as 20 ps in the smallest microcrystals. Radiative exciton-exciton Interaction and surface recombination were claimed to be the main mechanisms of exciton density decay, and the rate constant of the first process was estimated to be equal to 5·10^-8 cm³s^-1.     

Two-Photon Excited Diffraction Grating: Self-Diffraction and Nonlinear Optical Properties of Colloidal CdSe/ZnS QDs

Specific features have been revealed of nonlinear optical processes occurring when the total energy of two photons of a mode-locked Nd³⁺:YAG laser coincides with the energy of the main electron—hole (exciton) transition in colloidal CdSe/ZnS QDs and the effective self-diffraction of two laser beams arises on the induced diffraction grating.     

Surface Plasmon Resonance of Au Nanoparticles Fabricated by Negative Ion Implantation and Grid Structure toward Plasmonic Applications

Optical properties of Au nanoparticle composites and a grid structure of Cu nanoparticle composite were studied. Negative ion implantation was applied to synthesize Au and Cu nanoparticles in amorphous SiO₂ and Al₂O₃. Au nanoparticles were embedded within a depth of 30 nm by 60keV Au⁻ implantation. The surface plasmon resonance (SPR) of Au:SiO₂ and Au: Al₂O₃ composites shifted to red and to blue, respectively, compared to calculated ones by the Mie theory. Optical nonlinearity was measured with pump-probe femtosecond spectroscopy and the transient spectrum of Au: Al₂O₃ composite presented a large red shift from the SPR peak. Image mapping of far-field transmitted intensity of Cu-implanted SiO₂ with a fine grid structure drawn by laser-lithography was observed by a scanning near-field optical microscopy (SNOM) system.     

Optical magnetic resonance imaging with an ultra-narrow optical transition

We demonstrate optical magnetic resonance imaging (OMRI) of a Bose?CEinstein condensate of ytterbium atoms trapped in a one-dimensional (1D) optical lattice using an ultra-narrow optical transition ¹S₀?³P₂ (m=?2). We developed a vacuum chamber equipped with a thin glass cell, which provides high optical access and allows a compact design of magnetic coils. A line shape of a measured spectrum of the OMRI is well described by a spatial distribution of the atoms in a 1D optical lattice with the Thomas?CFermi approximation and an applied magnetic field gradient. The observed spectrum exhibits a periodic structure corresponding to the optical lattice periodicity.     

Bragg solitons in quantum-well structures

Soliton pulse propagation in a periodic quantum-well structure with a period close to one-half the light wavelength corresponding to the exciton resonance frequency was studied. The various kinds of exciton nonlinearity characteristic of a quantum well (P³-and EP²-type nonlinearities, biexciton nonlinearity) were included. The characteristic features of the soliton were studied in each of the cases considered. The effect of refractive index mismatch between the barrier and quantum-well materials on the soliton parameters was analyzed. Soliton solutions to the Maxwell-Bloch nonlinear equations are compared with their plane-wave solutions.     

Phase contribution to dynamic gratings recorded in Er-doped fiber with saturable absorption

Experimental observation of phase (i.e. refractive index) component in the dynamic gratings recorded in erbium-doped optical fiber with saturation of optical absorption is reported. We utilized configuration of transient two-wave mixing with rectangular phase modulation of one of counterpropagating recording waves, where unshifted phase grating resulted in a transient energy exchange. The reported experiments were performed with heavily doped (≈5400 ppm erbium) fibers in a wide spectral range of Er³⁺ fundamental absorption at selected laser wavelengths 1492, 1526, 1549, and 1568 nm. Relative contribution of phase grating was especially large (up to ≈100% of the maximal amplitude component) at the opposite sides of the investigated spectral range and was significantly lower in its central part. The amplitude grating was found especially strong at short wavelength side of the spectrum (i.e. at 1492 nm), where the grating amplitude proved to be only two times lower than the theoretically predicted from consideration of two-level model.     

Novel polymer nanocomposites with giant dynamical optical nonlinearity

The giant optical nonlinearity of a novel organic nanocomposite based on a conducting polymer, namely, poly(9-vinylcarbazole), and quinone derivatives as a charge photogenerator is investigated. The change in the refractive index of a thin polymer film (60 μm thick) is determined to be Δn = ?7.3 × 10^?3. The inference is made that the origin of the optical nonlinearity is associated with the difference between the polarizabilities of the quinone molecule and the quinone radical anion formed under exposure to laser radiation. The optical nonlinearity is examined using two methods: (i) the self-action of a Gaussian beam in a layer of the material and (ii) Z-scan measurements of a thin film at a wavelength of 633 nm. These nanocomposite materials can serve as active media in diverse applications, including image processing, high-density optical information storage, and phase conjugation.     

Picosecond studies of highly excited CdS

Results on picosecond luminescence and excite-and-probe transmission as well as transient grating measurements for highly excited CdS measured at a bath temperature of 5 K will be presented. The luminescence and optical gain both due to electron-hole plasma and excitonic molecule recombination are observed. The electron-hole plasma decays very fast by bimolecular recombination of electrons and holes in the plasma and diffusion of the carrier toward the low density regions, and transforms into excitons and excitonic molecules within 100–200 ps. The possibility of electron-hole liquid formation is definitely excluded. The exciton and excitonic molecule decay rather slowly and govern the optical properties for times longer than 200 ps.     

Nonlinear responses and optical limiting behavior of Basic Violet 16 dye under CW laser illumination

Nonlinear optical properties of Basic Violet 16 dye solution in water are studied employing different optical techniques. Experiments are performed using the second harmonic of a continuous Nd-Yag laser beam at 532 nm wavelength and 100 mW power. The effect of nonlinearity of Basic Violet 16 dye in broadening the laser beam is observed. The optical limiting behavior is investigated by measuring the transmission of the samples. The third-order nonlinearity, χ³ of Basic Violet 16 dye, is measured using Z-scan data. The nonlinear absorption coefficient is calculated using the open aperture Z-scan data, while its nonlinear refractive index is measured using the closed aperture Z-scan data. All experiments are done for different concentrations and thicknesses of Basic Violet 16 dye solution. The effect of intensity of input laser beam on the nonlinear susceptibility is studied experimentally. Results indicate that Basic Violet 16 dye is a potential candidate for low-power optical limiting applications.     

Theory of multi-exciton states in semiconductor nanocrystals

In this article, the fundamental physics of multi-exciton states in semiconductor nano-crystals is reviewed focusing on the mesoscopic enhancement of the excitonic radiative decay rate and the excitonic optical nonlinearity and the mechanism of their saturation with increase of the nanocrystal size. In the case of the radiative decay rate the thermal excitation of excited exciton states having small oscillator strength within the homogeneous linewidth of the exciton ground state is essential in determining the saturation behavior. The weakly correlated exciton pair states are found to cause a cancellation effect in the third-order nonlinear optical susceptibility at the exciton resonance, providing the first consistent understanding of the experimentally observed saturation of the mesoscopic enhancement of the excitonic optical nonlinearity. The presence of the weakly correlated exciton pair states is confirmed convincingly from the good correspondence between theory and experiments on the induced absorption spectra from the exciton state in CuCl nanocrystals. Furthermore, ultrafast relaxation processes of biexcitons are discussed in conjunction with the observed very fast rise of the biexciton gain in nanocrystals. In prospect of future progress in research, the theoretical formulation to calculate the triexciton states as one of the multi-exciton states beyond the biexciton is presented for the first time including the electron-hole exchange interaction.     

Exciton-polariton state in nanocrystalline SiC films

We studied the features of optical absorption in the films of nanocrystalline SiC (nc-SiC) obtained on the sapphire substrates by the method of direct ion deposition. The optical absorption spectra of the films with a thickness less than ~500 nm contain a maximum which position and intensity depend on the structure and thickness of the nc-SiC films. The most intense peak at 2.36 eV is observed in the nc-SiC film with predominant 3C-SiC polytype structure and a thickness of 392 nm. Proposed is a resonance absorption model based on excitation of exciton polaritons in a microcavity. In the latter, under the conditions of resonance, there occurs strong interaction between photon modes of light with λ_ph=521 nm and exciton of the 3С polytype with an excitation energy of 2.36 eV that results in the formation of polariton. A mismatch of the frequencies of photon modes of the cavity and exciton explains the dependence of the maximum of the optical absorption on the film thickness.     

Large optical nonlinearity in CaCu<Subscript>3</Subscript>Ti<Subscript>4</Subscript>O<Subscript>12</Subscript> thin films

CaCu₃Ti₄O₁₂ (CCTO) thin films were successfully prepared on LaAlO₃ substrates by pulsed laser deposition technique. We measured the nonlinear optical susceptibility of the thin films using Z-scan method at a wavelength of 532 nm with pulse durations of 25 ps and 7 ns. The large values of the third-order nonlinear optical susceptibility, χ ⁽³⁾, of the CCTO film were obtained to be 2.79×10⁻⁸ esu and 3.30×10⁻⁶ esu in picosecond and nanosecond time regimes, respectively, which are among the best results of some representative nonlinear optical materials. The origin of optical nonlinearity of CCTO films was discussed. The results indicate that the CCTO films on LaAlO₃ substrates are promising candidate materials for applications in nonlinear optical devices.     

Degradation process in organic thin film devices fabricated using P3HT

The stability of regioregular poly(3-hexylthiophene 2,5-diyl) (P3HT) thin films sandwiched between indium tin oxide (ITO) and aluminium (Al) electrodes have been investigated under normal environmental conditions (25°C and RH∼45–50%). Electrical and optical properties of ITO/P3HT/Al devices have been studied over a period of 30 days. Mobility μ of the order of 10⁻⁴ cm²/V-s has been obtained from the V ² law in the as-deposited P3HT films. Scanning electron microscopy (SEM) investigations show blistering of Al contacts in devices with a poly(3,4-ethylenedioxythiophene) (PEDOT) interlayer on application of voltage whereas no blistering is seen in devices without PEDOT. The results have been explained in terms of trap generation and propagation and the moisture-absorbing nature of PEDOT.      

Studies of relaxation times of secondary radiations in ZnTe by circular polarization correlation

Population and spin relaxation rates concerned with exciton luminescence and multiple LO-phonon emission lines are studied in ZnTe at 77 K by means of optical circular polarization correlation between the exciting and emitted lights. The decay times of the LO lines are determined to be much less than 10^-11sec, which are definitely shorter than the obtained exciton lifetime of 10^-10-10^-9sec. It is concluded that the LO lines are not due to hot luminescence but due to resonance Raman scattering.