Simplified theory of optical nonlinearities in spin-polarized semiconductors

The spin degree of freedom is largely disregarded in existing theories of the density-dependent optical properties of an interacting electron-hole plasma in quasiequilibrium. Here, we extended the pair equation, which is applicable to a bulk semiconductor at elevated temperatures, to calculate optical nonlinearities due to a spin-polarized plasma. We obtained agreement with recent circular dichroism data in laser-excited GaAs by using the plasma density alone as the fitting parameter. The simplicity of our theory, based on the analytical pair-equation formula, makes it ideal for conveniently modelling absorption in a carrier spin-polarized semiconductor.

Quasiequilibrium optical nonlinearities from spin-polarized carriers in GaAs

Semiconductor Bloch equations, which microscopically describe the dynamics of a Coulomb interacting, spin-unpolarized electron-hole plasma, can be solved in two limits: the coherent and the quasiequilibrium regimes. These equations have been recently extended to include the spin degree of freedom and used to explain spin dynamics in the coherent regime. In the quasiequilibrium limit, one solves the Bethe-Salpeter equation in a two-band model to describe how optical absorption is affected by Coulomb interactions within a spin unpolarized plasma of arbitrary density. In this work, we modified the solution of the Bethe-Salpeter equation to include spin polarization and light holes in a three-band model, which allowed us to account for spin-polarized versions of many-body effects in absorption. The calculated absorption reproduced the spin-dependent, density-dependent, and spectral trends observed in bulk GaAs at room temperature, in a recent pump-probe experiment with circularly polarized light. Hence, our results may be useful in the microscopic modeling of density-dependent optical nonlinearities due to spin-polarized carriers in semiconductors.

Simplified theory of optical nonlinearities in spin-polarized bulk GaAs

Apart from their intrinsic physical interest, spin-polarized many-body effects are expected to be important to the working of spintronic devices. A vast literature exists on the effects of a spin-unpolarized electron-hole plasma on the optical properties of a semiconductor. Here, we include the spin degree of freedom to model optical absorption of circularly polarized light by spin-polarized bulk GaAs. Our model is easy to implement and does not require elaborate numerics, since it is based on the closed-form analytical pair-equation formula that is valid in 3d. The efficacy of our approach is demonstrated by a comparison with recent experimental data.

Simplified theory of optical nonlinearities in spin-polarized bulk GaAs

Apart from their intrinsic physical interest, spin-polarized many-body effects are expected to be important to the working of spintronic devices. A vast literature exists on the effects of a spin-unpolarized electron-hole plasma on the optical properties of a semiconductor. Here, we include the spin degree of freedom to model optical absorption of circularly polarized light by spin-polarized bulk GaAs. Our model is easy to implement and does not require elaborate numerics, since it is based on the closed-form analytical pair-equation formula that is valid in 3d. The efficacy of our approach is demonstrated by a comparison with recent experimental data.

Spectrally broadened excitonic absorption and enhanced optical nonlinearities in Dy3+-doped ZnO nanoparticles

We have synthesized Dy3+-doped ZnO nanoparticles at room temperature through the sol-gel method. X-ray diffraction and Scanning electron microscopic studies confirm the crystalline nature of the particles. Excitonic absorption of ZnO shows three different bands, and we observe that incorporation of Dy3+ results in the shifting and broadening of the n=1 absorption band of ZnO. Photoluminescence studies done at the excitation wavelength of 335 nm show broad emission containing five different bands. Open-aperture z-scan studies done at 532 nm using 5 ns laser pulses show an optical limiting behavior, which numerically fits to a three-photon type absorption process. The nonlinearity is essentially resonant, as it is found to increase consistently with Dy3+ concentration. This feature makes Dy3+-doped ZnO a flexible optical limiter for potential device applications.

Hydrogen-bond-directed self-assembly of D-(+)-dibenzoyltartaric acid and 4-aminopyridine: optical nonlinearities and stoichiometry-dependent novel structural features

Attempts to prepare hydrogen-bond-directed nonlinear optical materials from a 1:1 molar mixture Of D-(+)-dibenzoyltartaric acid (DBT, I) and 4-aminopyridine (4-AP, II) resulted in two salts of different stoichiometry. One of them crystallizes in an unusual 1.5:1 (acid:base) monohydrate salt form III while the other one crystallizes as 1:1 (acid:base) salt IV. Crystal structures of both of the salts were determined from single-crystal X-ray diffraction data. The salt III crystallizes in a monoclinic space group C2 with a = 30.339(l), b = 7.881(2), c = 14.355(1) angstrom, beta = 97.48(1)degrees, V = 3403.1(9) angstrom3, Z = 4, R(w) = 0.058, R(w)= 0.058. The salt IV also crystallizes in a monoclinic space group P2(1) with a = 7.500(1), b = 14.968(2), c = 10.370(1) angstrom, beta = 102.67(1)degrees, V = 1135.9(2) angstrom3, Z = 2, R = 0.043, R(w) = 0.043. Interestingly, two DBT molecules with distinctly different conformation are present in the same crystal lattice of salt III. Extensive hydrogen-bonding interactions are found in both of the salts, and both of them show SHG intensity 1.4-1.6 times that of urea.

Optical nonlinearity in lead sulfide microtowers

Lead sulfide (PbS) microtowers on silicon substrates, having the physical properties of bulk PbS, have been synthesized. Optical nonlinearity studies using the open aperture z-scan technique employing 5 ns and 100 fs laser pulses reveal effective two-photon type absorption. For nanosecond excitation the nonlinear absorption coefficients (beta(eff)) are in the order of 10(-11) m W-1, two orders of magnitude less than the values reported for quantum confined PbS nanocrystals. For femtosecond excitation beta(eff) is of the order of 10(-14) m W-1. These results obtained in bulk PbS experimentally confirm the importance of quantum confinement in the enhancement of optical nonlinearities in semiconductor materials.

Large nonlinear refraction and two photon absorption in ferroelectric Bi2VO5.5 thin films

Ferroelectric c-oriented Bi2VO5.5 (BVO) thin films (thickness approximate to 300 nm) were fabricated by pulsed laser deposition on corning glass substrates. Nonlinear refractive index (n(2)) and two photon absorption coefficient (beta) were measured by Z-scan technique at 532 nm wavelength delivering pulses with 10 ns duration. Relatively large values of n(2) = 2.05 +/- 0.2 x 10(-10) cm(2)/W and beta = 9.36 +/- 0.3 cm/MW were obtained for BVO thin films. Origin of the large optical nonlinearities in BVO thin films was discussed based on bond-orbital theory of transition metal oxides. (c) 2012 Elsevier B.V. All rights reserved.

Base Triggered Enhancement of First Hyperpolarizability of a Keto-Enol Tautomer

This work describes the base triggered enhancement of first hyperpolarizability of a tautomeric organic molecule, namely, benzoylacetanilide (BA). We have used the hyper-Rayleigh scattering technique to measure the first hyperpolarizability (beta) of BA which exists in the pure keto form in water and as a keto-enol tautomer in ethanol. Its anion exists in equilibrium with the keto and enol forms at pH 11 in aqueous solution. The beta value of the anion form is 709 X 10(-30) esu, whereas that of the enol is 232 x 10(-3) esu and of the keto is 88 X 10(-30) esu. There is an enhancement of beta by similar to 8 times for the anion and similar to 3 times for the enol compared to the keto form. All these are achieved by altering the equilibrium between the three forms of BA by simple means. MP2 calculations reproduce the experimental trend, but the computed beta values are much lower than the measured values. DFT calculations with the standard B3LYP functional could not predict the right order in the beta values. The difference between experimental and calculated values is, perhaps, due to the fact that electron correlation effects are important in computing optical nonlinearities of large organic molecules and MP2 and B3LYP calculations done here for different forms of BA could not account for such effects adequately.

Singular value decomposition based computationally efficient algorithm for rapid dynamic near-infrared diffuse optical tomography

Purpose: A computationally efficient algorithm (linear iterative type) based on singular value decomposition (SVD) of the Jacobian has been developed that can be used in rapid dynamic near-infrared (NIR) diffuse optical tomography. Methods: Numerical and experimental studies have been conducted to prove the computational efficacy of this SVD-based algorithm over conventional optical image reconstruction algorithms. Results: These studies indicate that the performance of linear iterative algorithms in terms of contrast recovery (quantitation of optical images) is better compared to nonlinear iterative (conventional) algorithms, provided the initial guess is close to the actual solution. The nonlinear algorithms can provide better quality images compared to the linear iterative type algorithms. Moreover, the analytical and numerical equivalence of the SVD-based algorithm to linear iterative algorithms was also established as a part of this work. It is also demonstrated that the SVD-based image reconstruction typically requires O(NN2) operations per iteration, as contrasted with linear and nonlinear iterative methods that, respectively, requir O(NN3) and O(NN6) operations, with ``NN'' being the number of unknown parameters in the optical image reconstruction procedure. Conclusions: This SVD-based computationally efficient algorithm can make the integration of image reconstruction procedure with the data acquisition feasible, in turn making the rapid dynamic NIR tomography viable in the clinic to continuously monitor hemodynamic changes in the tissue pathophysiology.

Effective contrast recovery in rapid dynamic near-infrared diffuse optical tomography using l(1)-norm-based linear image reconstruction method

Traditional image reconstruction methods in rapid dynamic diffuse optical tomography employ l(2)-norm-based regularization, which is known to remove the high-frequency components in the reconstructed images and make them appear smooth. The contrast recovery in these type of methods is typically dependent on the iterative nature of method employed, where the nonlinear iterative technique is known to perform better in comparison to linear techniques (noniterative) with a caveat that nonlinear techniques are computationally complex. Assuming that there is a linear dependency of solution between successive frames resulted in a linear inverse problem. This new framework with the combination of l(1)-norm based regularization can provide better robustness to noise and provide better contrast recovery compared to conventional l(2)-based techniques. Moreover, it is shown that the proposed l(1)-based technique is computationally efficient compared to its counterpart (l(2)-based one). The proposed framework requires a reasonably close estimate of the actual solution for the initial frame, and any suboptimal estimate leads to erroneous reconstruction results for the subsequent frames.

Estimation of nonlinearities from pseudodynamic and dynamic responses of bridge structures using the Delay Vector Variance method

Analysis of the variability in the responses of large structural systems and quantification of their linearity or nonlinearity as a potential non-invasive means of structural system assessment from output-only condition remains a challenging problem. In this study, the Delay Vector Variance (DVV) method is used for full scale testing of both pseudo-dynamic and dynamic responses of two bridges, in order to study the degree of nonlinearity of their measured response signals. The DVV detects the presence of determinism and nonlinearity in a time series and is based upon the examination of local predictability of a signal. The pseudo-dynamic data is obtained from a concrete bridge during repair while the dynamic data is obtained from a steel railway bridge traversed by a train. We show that DVV is promising as a marker in establishing the degree to which a change in the signal nonlinearity reflects the change in the real behaviour of a structure. It is also useful in establishing the sensitivity of instruments or sensors deployed to monitor such changes. (C) 2015 Elsevier B.V. All rights reserved.

A Proposal for Concurrent Estimation of Static and Dynamic Nonlinearity of ADC

Despite great advances in very large scale integrated-circuit design and manufacturing, performance of even the best available high-speed, high-resolution analog-to-digital converter (ADC) is known to deteriorate while acquiring fast-rising, high-frequency, and nonrepetitive waveforms. Waveform digitizers (ADCs) used in high-voltage impulse recordings and measurements are invariably subjected to such waveforms. Errors resulting from a lowered ADC performance can be unacceptably high, especially when higher accuracies have to be achieved (e.g., when part of a reference measuring system). Static and dynamic nonlinearities (estimated independently) are vital indices for evaluating performance and suitability of ADCs to be used in such environments. Typically, the estimation of static nonlinearity involves 10-12 h of time or more (for a 12-b ADC) and the acquisition of millions of samples at high input frequencies for dynamic characterization. ADCs with even higher resolution and faster sampling speeds will soon become available. So, there is a need to reduce testing time for evaluating these parameters. This paper proposes a novel and time-efficient method for the simultaneous estimation of static and dynamic nonlinearity from a single test. This is achieved by conceiving a test signal, comprised of a high-frequency sinusoid (which addresses dynamic assessment) modulated by a low-frequency ramp (relevant to the static part). Details of implementation and results on two digitizers are presented and compared with nonlinearities determined by the existing standardized approaches. Good agreement in results and time savings achievable indicates its suitability.

A Proposal for Concurrent Estimation of Static and Dynamic Nonlinearity of ADC

Despite great advances in very large scale integrated-circuit design and manufacturing, performance of even the best available high-speed, high-resolution analog-to-digital converter (ADC) is known to deteriorate while acquiring fast-rising, high-frequency, and nonrepetitive waveforms. Waveform digitizers (ADCs) used in high-voltage impulse recordings and measurements are invariably subjected to such waveforms. Errors resulting from a lowered ADC performance can be unacceptably high, especially when higher accuracies have to be achieved (e.g., when part of a reference measuring system). Static and dynamic nonlinearities (estimated independently) are vital indices for evaluating performance and suitability of ADCs to be used in such environments. Typically, the estimation of static nonlinearity involves 10-12 h of time or more (for a 12-b ADC) and the acquisition of millions of samples at high input frequencies for dynamic characterization. ADCs with even higher resolution and faster sampling speeds will soon become available. So, there is a need to reduce testing time for evaluating these parameters. This paper proposes a novel and time-efficient method for the simultaneous estimation of static and dynamic nonlinearity from a single test. This is achieved by conceiving a test signal, comprised of a high-frequency sinusoid (which addresses dynamic assessment) modulated by a low-frequency ramp (relevant to the static part). Details of implementation and results on two digitizers are presented and compared with nonlinearities determined by the existing standardized approaches. Good agreement in results and time savings achievable indicates its suitability.

Compact fiber Bragg grating dynamic strain sensor cum broadband thermometer for thermally unstable ambience

An instrument for simultaneous measurement of dynamic strain and temperature in a thermally unstable ambience has been proposed, based on fiber Bragg grating technology. The instrument can function as a compact and stand-alone broadband thermometer and a dynamic strain gauge. It employs a source wavelength tracking procedure for linear dependence of the output on the measurand, offering high dynamic range. Two schemes have been demonstrated with their relative merits. As a thermometer, the present instrumental configuration can offer a linear response in excess of 500 degrees C that can be easily extended by adding a suitable grating and source without any alteration in the procedure. Temperature sensitivity is about 0.06 degrees C for a bandwidth of 1 Hz. For the current grating, the upper limit of strain measurement is about 150 mu epsilon with a sensitivity of about 80 n epsilon Hz(-1/2). The major source of uncertainty associated with dynamic strain measurement is the laser source intensity noise, which is of broad spectral band. A low noise source device or the use of optical power regulators can offer improved performance. The total harmonic distortion is less than 0.5% up to about 50 mu epsilon, 1.2% at 100 mu epsilon and about 2.3% at 150 mu epsilon. Calibrated results of temperature and strain measurement with the instrument have been presented. Traces of ultrasound signals recorded by the system at 200 kHz, in an ambience of 100-200 degrees C temperature fluctuation, have been included. Also, the vibration spectrum and engine temperature of a running internal combustion engine has been recorded as a realistic application of the system.