Selective alignment of molecular spin isomers

We experimentally demonstrate field-free, spin-selective alignment of ortho- and para molecular spin isomers at room temperature. By means of two nonresonant, strong, properly delayed femtosecond pulses within a four wave mixing arrangement, we observed selective alignment for homonuclear diatomics composed of spin 1/2 (15N) or spin 1 (14N) atoms. The achieved selective control of the isomers' angular distribution and rotational excitation may find applications to analysis, enrichment, and actual physical separation of molecular spin modifications.     

Nonintrusive measurement of field-free molecular alignment

A technique was provided to nonintrusively quantify the field-free alignment of molecules by measuring the transient birefringence caused by the aligned molecules. Pure heterodyne alignment signals were obtained from the difference of the signals under an external electric field with opposite polarity and equal magnitude. The results demonstrated that the pure heterodyne alignment signal directly reproduced the revival structure of molecular alignment and its Fourier transform spectroscopy represented the actual populations of the different J states in the rotational wave packet.     

Nonparametric algorithms for vector optimization

Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 9, pp. 5–10, September, 1995.     

Field-free molecular alignment and its application

Field-free molecular alignment can be achieved by nonadiabatic rotational excitation of molecules with strong femtosecond laser pulses. We experimentally and theoretically demonstrate that the degree of alignment can be improved with multi-pulse excitation. An approach is proposed to tune the frequency of few-cycle pulses using field-free alignment of molecules.     

Field-free three dimensional molecular axis alignment

We investigate strategies for field-free three dimensional molecular axis alignment using strong nonresonant laser fields under experimentally realistic conditions. Using the polarizabilites and rotational constants of an asymmetric top rotor molecule (ethene, C2H4), we consider three different methods for axis alignment of a Boltzmann distribution of rotors at 4 K. Specifically, we compare the use of impulsive kick laser pulses having both linear and elliptical polarization to the use of elliptically polarized switched laser pulses. We show that an enhanced degree of field-free three dimensional alignment of ground vibronic state molecules obtains from the use of two orthogonally polarized, time-separated laser pulses.     

Electronic control of spin alignment in pi-conjugated molecular magnets

Intramolecular spin alignment in pi-conjugated molecules is studied theoretically in a model of a Peierls-Hubbard chain coupled with two localized spins. By means of the exact diagonalization technique, we demonstrate that a spin singlet (S=0) to quartet (S=3/2) transition can be induced by electronic doping, depending on the chain length, the positions of the localized spins, and the sign of the electron-spin coupling. The calculated results provide a theoretical basis for understanding the mechanism of spin alignment recently observed in a diradical donor molecule.     

Evolutionary algorithm for optimization of multilayer coatings

In this paper, a new evolutionary algorithm, the well-known imperialist competition algorithm, is proposed for optimizing the optical thin-films. In this method, the process is modeled of the competition between countries as imperialists and their colonizing of others as colonies. This algorithm could be an appropriate alternative to some of the more popular algorithms for optimizing the optical thin-films for good performance. The polarizer and edge filter for example are designed by using the imperialist competition algorithm method and the results are compared with those from two optimization high-performance methods: the genetic algorithm and differential evolutionary algorithm. Based on these results,the performance of the imperialist competition algorithm method shows that this algorithm is not sensitive to the change of its parameters and it can be an important advantage for quickly achieving a global optimal point. On the other hand the results show a better ratio of P-polarization transmittance to S-polarization transmittance in the design of a 1540-nm polarizer, which is more appropriate than the results from the other two methods. In the second design, an edge filter with a lower number of layers and more uniform bandpass spectrum than the counterparts of those methods is obtained. These results indicate that the imperialist competition algorithm is a robust method for optical thin-film designs.     

Collective alignment of polar filaments by molecular motors

We study the alignment of polar biofilaments, such as microtubules and actin, subject to the action of multiple molecular motors attached simultaneously to more than one filament. Focusing on a paradigm model of only two filaments interacting with multiple motors, we were able to investigate in detail the alignment dynamics. While almost no alignment occurs in the case of a single motor, the filaments become rapidly aligned due to the collective action of the motors. Our analysis shows that the alignment time is governed by the number of bound motors and the magnitude of the motors’ stepping fluctuations. We predict that the time scale of alignment is in the order of seconds, much faster than that reported for passive crosslink-induced bundling. In vitro experiments on the alignment of microtubules by multiple-motor covered beads are in qualitative agreement. We also discuss another mode of fast alignment of filaments, namely the cooperation between motors and passive crosslinks.     

Numerical Simulations of femtosecond-laser-induced dynamic alignment of molecules in the high-frequency off-resonance regime

The motion equation for ? between the molecular axis and laser polarization direction in a high-frequency off-resonance femtosecond laser field is deduced while simultaneously examining the effects of a permanent dipole moment and field-induced polarizability and hyperpolarizability to molecular rotation. Femtosecond-laser-induced dynamic alignment of CO, N₂, and Br₂ molecules are investigated by numerically solving the obtained rotation equation for the angle ?. The effects of the molecular permanent dipole moment and the field-induced polarizability and hyperpolarizability on the degree of alignment are presented at different intensities. Our computational results show that the dynamic alignment of molecules is primarily determined by field-induced polarizability and the second hyperpolarizability for the laser intensity range from 5 × 10¹⁴ to 5 × 10¹⁶ W/cm². The contributions of higher order correction terms to molecular alignment can usually be neglected. The polarizability-field interaction makes the angular distributions of a molecule have a maximum along the polarization axis and a minimum perpendicular to it. The role of the second hyperpolarizability keeps the molecular counts maximum along the laser polarization direction but minimum at an angle of 45° between the molecular axis and the polarization direction. There is also a second maximum of molecular counts perpendicular to the polarization axis. For CO, N₂, and Br₂ molecules, the dependences of laser-induced dynamic alignment on laser intensity exhibit completely different characteristics.     

Role of highest occupied molecular orbitals in molecular field-free alignment by a femtosecond pulse

This paper studies the molecular rotational excitation and field-free spatial alignment in a nonresonant intense laser field numerically and analytically by using the time-dependent Schr?dinger equation. The broad rotational wave packets excited by the femtosecond pulse are defined in conjugate angle space, and their coefficients are obtained by solving a set of coupled linear equations. Both single molecule orientation angles and an ensemble of O₂ and CO molecule angular distributions are calculated in detail. The numerical results show that, for single molecule highest occupied molecular orbital (HOMO) symmetry σ tends to have a molecular orientation along the laser polarization direction and the permanent dipole moment diminishes the mean of the orientation angles; for an ensemble of molecules, angular distributions provide more complex and additional information at times where there are no revivals in the single molecule plot. In particular, at the revival peak instant, with the increase of temperature of the molecular ensemble, the anisotropic angular distributions with respect to the laser polarization direction of the π _g orbital gradually transform to the symmetrical distributions regarding the laser polarization vector and for two HOMO configurations angular distributions of all directions are confined within a smaller angle when the temperature of the molecular ensemble is higher.     

Modified theory of photoinduced molecular polar alignment in azo polymers

An improvement on the simplified theory of all-optical poling [Chem. Phys. Lett. 286, 415 (1998)] is proposed. In this improvement the influence of the cis isomer is taken into account in the process of photoinduced molecular polar alignment. An analytical expression for the induced polar order in the steady-state regime is derived. This expression shows that, although the contribution to the photoinduced second-order susceptibility from the cis state itself can be neglected, the population of the cis state plays an important role. This result suggests the possibility that one can improve the induced polar order by increasing the poling temperature, so that thermal-assisted optical poling can be explained.     

Liapunov exponents and the reversibility of molecular dynamics algorithms

We study the phenomenon of lack of reversibility in molecular dynamics algorithms for the case of Wilson's lattice QCD. We demonstrate that the classical equations of motion that are employed in these algorithms are chaotic in nature. The leading Liapunov exponent is determined in a range of coupling parameters. We consider the consequences of the breakdown of reversibility due to round-off errors.     

Evolutionary optimization of non-periodic coupled-cavity semiconductor laser diodes

The analysis of different types of non-periodic multi-cavity laser structures will be presented. Deterministic non-periodic cavity concepts such as self-similar Cantor- or quasi-periodic Fibonacci sequences offer a distinct mode selectivity whilst having a significantly lower number of coupled cavities compared to an equivalent periodic solution. A heuristic numerical optimization procedure based on a breeder genetic algorithm scheme is favoured, also to give a sort of general information as to which kind of structures are well suited in terms of our requirements. By investigating the evolutionary optimized laser topologies according to the evolution of characteristic patterns, we propose a sort of superior meta-optimization strategy which relies on a population based information gathering.     

基于智能全局优化算法的理论结构预测

凝聚态物质内部的原子堆垛方式,即微观原子结构,是深入理解其各种宏观物理和化学性质的基础。近年来,随着基于群智理论的全局优化算法和第一性原理计算方法的发展,只根据物质的化学组分和外界条件,通过理论计算来确定或预测物质的微观原子结构成为可能。文章将对目前国内外主要理论结构预测方法进行简要的概述,重点介绍基于群智算法的卡里普索(CALYPSO)结构预测方法的基本原理及其在凝聚态物质结构研究中的一些典型应用。     

Controlling attosecond double ionization dynamics via molecular alignment

We investigate the dynamics of double ionization in aligned nitrogen molecules. An ultrashort, weak laser pulse creates an aligned ensemble of molecules that is ionized with a subsequent, strong probe pulse. We find that the two electrons involved in nonsequential double ionization more likely exit the molecule in the same direction if it is parallel to the probe laser polarization, indicating that they are ejected within a few hundred attoseconds of each other. Double ionization is less probable and takes longer for perpendicular molecules.     

Dynamics of heuristic optimization algorithms on random graphs

In this paper, the dynamics of heuristic algorithms for constructing small vertex covers (or independent sets) of finite-connectivity random graphs is analysed. In every algorithmic step, a vertex is chosen with respect to its vertex degree. This vertex, and some environment of it, is covered and removed from the graph. This graph reduction process can be described as a Markovian dynamics in the space of random graphs of arbitrary degree distribution. We discuss some solvable cases, including algorithms already analysed using different techniques, and develop approximation schemes for more complicated cases. The approximations are corroborated by numerical simulations. Received 14 March 2002 Published online 31 July 2002     

Characterization of the cholesteric phase of filamentous bacteriophage fd for molecular alignment

Residual dipolar couplings arise from small degrees of alignment of molecules in a magnetic field and have proven to provide valuable structural information. Colloidal suspensions of rod-shaped viruses and bacteriophages constitute a frequently employed medium for imparting such alignment onto biomolecules. The stability and behavior of the liquid crystalline phases with respect to solution conditions such as pH, ionic strength, and temperature vary, and characterization should benefit practical applications as well as theoretical understanding. In this Communication we describe the pH dependence of the cholesteric liquid crystalline phase of the filamentous bacteriophage fd and demonstrate that the alignment tensor of the solute protein is modulated by pH. We also report the interesting observation that the relative sign of the residual dipolar coupling changes at low pH values. In addition, we demonstrate that the degree of alignment inversely scales with the lengths of the phage particles for phages with identical mass and charge per unit length.     

Influence of rounding errors on the quality of heuristic optimization algorithms

Search space smoothing and related heuristic optimization algorithms provide an alternative approach to simulated annealing and its variants: while simulated annealing traverses barriers in the energy landscape at finite temperatures, search space smoothing intends to remove these barriers, so that a greedy algorithm is sufficient to find the global minimum. Several formulas for smoothing the energy landscape have already been applied, one of them making use of the finite numerical precision on a computer. In this paper, we thoroughly investigate the effect of finite numerical accuracy on the quality of results achieved with heuristic optimization algorithms. We present computational results for the traveling salesman problem.     

Improving the performance of DCT-based fragile watermarking using intelligent optimization algorithms

The performance of a fragile watermarking method based on discrete cosine transform (DCT) has been improved in this paper by using intelligent optimization algorithms (IOA), namely genetic algorithm, differential evolution algorithm, clonal selection algorithm and particle swarm optimization algorithm. In DCT based fragile watermarking techniques, watermark embedding can usually be achieved by modifying the least significant bits of the transformation coefficients. After the embedding process is completed, transforming the modified coefficients from the frequency domain to the spatial domain produces some rounding errors due to the conversion of real numbers to integers. The rounding errors caused by this transformation process were corrected by the use of intelligent optimization algorithms mentioned above. This paper gives experimental results which show the feasibility of using these optimization algorithms for the fragile watermarking and demonstrate the accuracy of these methods. The performance comparison of the algorithms was also realized.