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Nanopropellers and Their Actuation in Complex Viscoelastic Media

Schamel, D., Mark, A. G., Gibbs, J. G., Miksch, C., Morozov, K. I., Leshansky, A. M., Fischer, P.

ACS Nano, 8(9):8794-8801, June 2014, Featured cover article. (article)

Abstract
Tissue and biological fluids are complex viscoelastic media with a nanoporous macromolecular structure. Here, we demonstrate that helical nanopropellers can be controllably steered through such a biological gel. The screw-propellers have a filament diameter of about 70 nm and are smaller than previously reported nanopropellers as well as any swimming microorganism. We show that the nanoscrews will move through high-viscosity solutions with comparable velocities to that of larger micropropellers, even though they are so small that Brownian forces suppress their actuation in pure water. When actuated in viscoelastic hyaluronan gels, the nanopropellers appear to have a significant advantage, as they are of the same size range as the gel’s mesh size. Whereas larger helices will show very low or negligible propulsion in hyaluronan solutions, the nanoscrews actually display significantly enhanced propulsion velocities that exceed the highest measured speeds in Newtonian fluids. The nanopropellers are not only promising for applications in the extracellular environment but small enough to be taken up by cells.

Featured cover article.

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Video - Helical Micro and Nanopropellers for Applications in Biological Fluidic Environments link (url) DOI [BibTex]


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Convertor

Fischer, P., Mark, A.

May 2014 (patent)

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[BibTex]

[BibTex]


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Circular polarization interferometry: circularly polarized modes of cholesteric liquid crystals

Sanchez-Castillo, A., Eslami, S., Giesselmann, F., Fischer, P.

OPTICS EXPRESS, 22(25):31227-31236, 2014 (article)

Abstract
We describe a novel polarization interferometer which permits the determination of the refractive indices for circularly-polarized light. It is based on a Jamin-Lebedeff interferometer, modified with waveplates, and permits us to experimentally determine the refractive indices n(L) and n(R) of the respectively left- and right-circularly polarized modes in a cholesteric liquid crystal. Whereas optical rotation measurements only determine the circular birefringence, i.e. the difference (n(L) - n(R)), the interferometer also permits the determination of their absolute values. We report refractive indices of a cholesteric liquid crystal in the region of selective (Bragg) reflection as a function of temperature. (C) 2014 Optical Society of America

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DOI [BibTex]

DOI [BibTex]


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Self-Propelling Nanomotors in the Presence of Strong Brownian Forces

Lee, T., Alarcon-Correa, M., Miksch, C., Hahn, K., Gibbs, J. G., Fischer, P.

NANO LETTERS, 14(5):2407-2412, 2014 (article)

Abstract
Motility in living systems is due to an array of complex molecular nanomotors that are essential for the function and survival of cells. These protein nanomotors operate not only despite of but also because of stochastic forces. Artificial means of realizing motility rely on local concentration or temperature gradients that are established across a particle, resulting in slip velocities at the particle surface and thus motion of the particle relative to the fluid. However, it remains unclear if these artificial motors can function at the smallest of scales, where Brownian motion dominates and no actively propelled living organisms can be found. Recently, the first reports have appeared suggesting that the swimming mechanisms of artificial structures may also apply to enzymes that are catalytically active. Here we report a scheme to realize artificial Janus nanoparticles (JNPs) with an overall size that is comparable to that of some enzymes similar to 30 nm. Our JNPs can catalyze the decomposition of hydrogen peroxide to water and oxygen and thus actively move by self-electrophoresis. Geometric anisotropy of the Pt-Au Janus nanoparticles permits the simultaneous observation of their translational and rotational motion by dynamic light scattering. While their dynamics is strongly influenced by Brownian rotation, the artificial Janus nanomotors show bursts of linear ballistic motion resulting in enhanced diffusion.

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DOI [BibTex]


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Shape control in wafer-based aperiodic 3D nanostructures

Hyeon-Ho, J., Mark, A. G., Gibbs, J. G., Reindl, T., Waizmann, U., Weis, J., Fischer, P.

NANOTECHNOLOGY, 25(23), 2014, Cover article. (article)

Abstract
Controlled local fabrication of three-dimensional (3D) nanostructures is important to explore and enhance the function of single nanodevices, but is experimentally challenging. We present a scheme based on e-beam lithography (EBL) written seeds, and glancing angle deposition (GLAD) grown structures to create nanoscale objects with defined shapes but in aperiodic arrangements. By using a continuous sacrificial corral surrounding the features of interest we grow isolated 3D nanostructures that have complex cross-sections and sidewall morphology that are surrounded by zones of clean substrate.

Cover article.

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DOI [BibTex]

DOI [BibTex]


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Swimming by reciprocal motion at low Reynolds number

Qiu, T., Lee, T., Mark, A. G., Morozov, K. I., Muenster, R., Mierka, O., Turek, S., Leshansky, A. M., Fischer, P.

NATURE COMMUNICATIONS, 5, 2014, Max Planck Press Release. (article)

Abstract
Biological microorganisms swim with flagella and cilia that execute nonreciprocal motions for low Reynolds number (Re) propulsion in viscous fluids. This symmetry requirement is a consequence of Purcell's scallop theorem, which complicates the actuation scheme needed by microswimmers. However, most biomedically important fluids are non-Newtonian where the scallop theorem no longer holds. It should therefore be possible to realize a microswimmer that moves with reciprocal periodic body-shape changes in non-Newtonian fluids. Here we report a symmetric `micro-scallop', a single-hinge microswimmer that can propel in shear thickening and shear thinning (non-Newtonian) fluids by reciprocal motion at low Re. Excellent agreement between our measurements and both numerical and analytical theoretical predictions indicates that the net propulsion is caused by modulation of the fluid viscosity upon varying the shear rate. This reciprocal swimming mechanism opens new possibilities in designing biomedical microdevices that can propel by a simple actuation scheme in non-Newtonian biological fluids.

Max Planck Press Release.

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Video - A Swimming Micro-Scallop Video - Winner of the Micro-robotic Design Challenge in Hamlyn Symposium on Medical Robotics DOI [BibTex]

Video - A Swimming Micro-Scallop Video - Winner of the Micro-robotic Design Challenge in Hamlyn Symposium on Medical Robotics DOI [BibTex]


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Nanohelices by shadow growth

Gibbs, J. G., Mark, A. G., Lee, T., Eslami, S., Schamel, D., Fischer, P.

NANOSCALE, 6(16):9457-9466, 2014 (article)

Abstract
The helix has remarkable qualities and is prevalent in many fields including mathematics, physics, chemistry, and biology. This shape, which is chiral by nature, is ubiquitous in biology with perhaps the most famous example being DNA. Other naturally occurring helices are common at the nanoscale in the form of protein secondary structures and in various macromolecules. Nanoscale helices exhibit a wide range of interesting mechanical, optical, and electrical properties which can be intentionally engineered into the structure by choosing the correct morphology and material. As technology advances, these fabrication parameters can be fine-tuned and matched to the application of interest. Herein, we focus on the fabrication and properties of nanohelices grown by a dynamic shadowing growth method combined with fast wafer-scale substrate patterning which has a number of distinct advantages. We review the fabrication methodology and provide several examples that illustrate the generality and utility of nanohelices shadow-grown on nanopatterns.

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Video - Fabrication of Designer Nanostructures DOI [BibTex]


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Chiral Nanomagnets

Eslami, S., Gibbs, J. G., Rechkemmer, Y., van Slageren, J., Alarcon-Correa, M., Lee, T., Mark, A. G., Rikken, G. L. J. A., Fischer, P.

ACS PHOTONICS, 1(11):1231-1236, 2014 (article)

Abstract
We report on the enhanced optical properties of chiral magnetic nanohelices with critical dimensions comparable to the ferromagnetic domain size. They are shown to be ferromagnetic at room temperature, have defined chirality, and exhibit large optical activity in the visible as verified by electron microscopy, superconducting quantum interference device (SQUID) magnetometry, natural circular dichroism (NCD), and magnetic circular dichroism (MCD) measurements. The structures exhibit magneto-chiral dichroism (MChD), which directly demonstrates coupling between their structural chirality and magnetism. A chiral nickel (Ni) film consisting of an array of nanohelices similar to 100 nm in length exhibits an MChD anisotropy factor g(MChD) approximate to 10(-4) T-1 at room temperature in a saturation field of similar to 0.2 T, permitting polarization-independent control of the film's absorption properties through magnetic field modulation. This is also the first report of MChD in a material with structural chirality on the order of the wavelength of light, and therefore the Ni nanohelix array is a metamaterial with magnetochiral properties that can be tailored through a dynamic deposition process.

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DOI [BibTex]

DOI [BibTex]


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Wireless powering of e-swimmers

Roche, J., Carrara, S., Sanchez, J., Lannelongue, J., Loget, G., Bouffier, L., Fischer, P., Kuhn, A.

SCIENTIFIC REPORTS, 4, 2014 (article)

Abstract
Miniaturized structures that can move in a controlled way in solution and integrate various functionalities are attracting considerable attention due to the potential applications in fields ranging from autonomous micromotors to roving sensors. Here we introduce a concept which allows, depending on their specific design, the controlled directional motion of objects in water, combined with electronic functionalities such as the emission of light, sensing, signal conversion, treatment and transmission. The approach is based on electric field-induced polarization, which triggers different chemical reactions at the surface of the object and thereby its propulsion. This results in a localized electric current that can power in a wireless way electronic devices in water, leading to a new class of electronic swimmers (e-swimmers).

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DOI [BibTex]

DOI [BibTex]


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Swelling and shrinking behaviour of photoresponsive phosphonium-based ionogel microstructures

Czugala, M., O’Connell, C., Blin, C., Fischer, P., Fraser, K. J., Benito-Lopez, F., Diamond, D.

SENSORS AND ACTUATORS B-CHEMICAL, 194, pages: 105-113, 2014 (article)

Abstract
Photoresponsive N-isopropylacrylamide ionogel microstructures are presented in this study. These ionogels are synthesised using phosphonium based room temperature ionic liquids, together with the photochromic compound benzospiropyran. The microstructures can be actuated using light irradiation, facilitating non-contact and non-invasive operation. For the first time, the characterisation of the swelling and shrinking behaviour of several photopatterned ionogel microstructures is presented and the influence of surface-area-to-volume ratio on the swelling kinetics is evaluated. It was found that the swelling and shrinking behaviour of the ionogels is strongly dependent on the nature of the ionic liquid. In particular, the {[}P-6,P-6,P-6,P-14]{[}NTf2] ionogel exhibits the greatest degree of swelling, reaching up to 180\% of its initial size, and the fastest shrinkage rate (k(sh) = 29 +/- 4 x 10(-2) s(-1)). (C) 2014 Elsevier B. V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]

2013


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Hybrid nanocolloids with programmed three-dimensional shape and material composition

Mark, A. G., Gibbs, J. G., Lee, T., Fischer, P.

NATURE MATERIALS, 12(9):802-807, 2013, Max Planck Press Release. (article)

Abstract
Tuning the optical(1,2), electromagnetic(3,4) and mechanical properties of a material requires simultaneous control over its composition and shape(5). This is particularly challenging for complex structures at the nanoscale because surface-energy minimization generally causes small structures to be highly symmetric(5). Here we combine low-temperature shadow deposition with nanoscale patterning to realize nanocolloids with anisotropic three-dimensional shapes, feature sizes down to 20 nm and a wide choice of materials. We demonstrate the versatility of the fabrication scheme by growing three-dimensional hybrid nanostructures that contain several functional materials with the lowest possible symmetry, and by fabricating hundreds of billions of plasmonic nanohelices, which we use as chiral metafluids with record circular dichroism and tunable chiroptical properties.

Max Planck Press Release.

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Video - Fabrication of Designer Nanostructures DOI [BibTex]


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Chiral Colloidal Molecules And Observation of The Propeller Effect

Schamel, D., Pfeifer, M., Gibbs, J. G., Miksch, B., Mark, A. G., Fischer, P.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 135(33):12353-12359, 2013 (article)

Abstract
Chiral molecules play an important role in biological and chemical processes, but physical effects due to their symmetry-breaking are generally weak. Several physical chiral separation schemes which could potentially be useful, including the propeller effect, have therefore not yet been demonstrated at the molecular scale. However, it has been proposed that complex nonspherical colloidal particles could act as ``colloidal molecules{''} in mesoscopic model systems to permit the visualization of molecular phenomena that are otherwise difficult to observe. Unfortunately, it is difficult to synthesize such colloids because surface minimization generally favors the growth of symmetric particles. Here we demonstrate the production of large numbers of complex colloids with glancing angle physical vapor deposition. We use chiral colloids to demonstrate the Baranova and Zel'dovich (Baranova, N. B.; Zel'dovich, B. Y. Chem. Phys. Lett. 1978, 57, 435) propeller effect: the separation of a racemic mixture by application of a rotating field that couples to the dipole moment of the enantiomers and screw propels them in opposite directions. The handedness of the colloidal suspensions is monitored with circular differential light scattering. An exact solution for the colloid's propulsion is derived, and comparisons between the colloidal system and the corresponding effect at the molecular scale are made.

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Video - Nanospropellers DOI [BibTex]

Video - Nanospropellers DOI [BibTex]


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Indirect absorption spectroscopy using quantum cascade lasers: mid-infrared refractometry and photothermal spectroscopy

Pfeifer, M., Ruf, A., Fischer, P.

OPTICS EXPRESS, 21(22):25643-25654, 2013 (article)

Abstract
We record vibrational spectra with two indirect schemes that depend on the real part of the index of refraction: mid-infrared refractometry and photothermal spectroscopy. In the former, a quantum cascade laser (QCL) spot is imaged to determine the angles of total internal reflection, which yields the absorption line via a beam profile analysis. In the photothermal measurements, a tunable QCL excites vibrational resonances of a molecular monolayer, which heats the surrounding medium and changes its refractive index. This is observed with a probe laser in the visible. Sub-monolayer sensitivities are demonstrated. (C) 2013 Optical Society of America

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DOI [BibTex]


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Plasmonic nanohelix metamaterials with tailorable giant circular dichroism

Gibbs, J. G., Mark, A. G., Eslami, S., Fischer, P.

APPLIED PHYSICS LETTERS, 103(21), 2013, Featured cover article. (article)

Abstract
Plasmonic nanohelix arrays are shown to interact with electromagnetic fields in ways not typically seen with ordinary matter. Chiral metamaterials (CMMs) with feature sizes small with respect to the wavelength of visible light are a promising route to experimentally achieve such phenomena as negative refraction without the need for simultaneously negative e and mu. Here we not only show that giant circular dichroism in the visible is achievable with hexagonally arranged plasmonic nanohelix arrays, but that we can precisely tune the optical activity via morphology and lattice spacing. The discrete dipole approximation is implemented to support experimental data. (C) 2013 AIP Publishing LLC.

Featured cover article.

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DOI [BibTex]

DOI [BibTex]


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Information Driven Self-Organization of Complex Robotic Behaviors

Martius, G., Der, R., Ay, N.

PLoS ONE, 8(5):e63400, Public Library of Science, 2013 (article)

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Linear combination of one-step predictive information with an external reward in an episodic policy gradient setting: a critical analysis

Zahedi, K., Martius, G., Ay, N.

Frontiers in Psychology, 4(801), 2013 (article)

Abstract
One of the main challenges in the field of embodied artificial intelligence is the open-ended autonomous learning of complex behaviours. Our approach is to use task-independent, information-driven intrinsic motivation(s) to support task-dependent learning. The work presented here is a preliminary step in which we investigate the predictive information (the mutual information of the past and future of the sensor stream) as an intrinsic drive, ideally supporting any kind of task acquisition. Previous experiments have shown that the predictive information (PI) is a good candidate to support autonomous, open-ended learning of complex behaviours, because a maximisation of the PI corresponds to an exploration of morphology- and environment-dependent behavioural regularities. The idea is that these regularities can then be exploited in order to solve any given task. Three different experiments are presented and their results lead to the conclusion that the linear combination of the one-step PI with an external reward function is not generally recommended in an episodic policy gradient setting. Only for hard tasks a great speed-up can be achieved at the cost of an asymptotic performance lost.

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link (url) DOI [BibTex]


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Robustness of guided self-organization against sensorimotor disruptions

Martius, G.

Advances in Complex Systems, 16(02n03):1350001, 2013 (article)

Abstract
Self-organizing processes are crucial for the development of living beings. Practical applications in robots may benefit from the self-organization of behavior, e.g.~to increase fault tolerance and enhance flexibility, provided that external goals can also be achieved. We present results on the guidance of self-organizing control by visual target stimuli and show a remarkable robustness to sensorimotor disruptions. In a proof of concept study an autonomous wheeled robot is learning an object finding and ball-pushing task from scratch within a few minutes in continuous domains. The robustness is demonstrated by the rapid recovery of the performance after severe changes of the sensor configuration.

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DOI [BibTex]

DOI [BibTex]

2008


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Voltage-Controllable Magnetic Composite Based on Multifunctional Polyethylene Microparticles

Ghosh, A., Sheridon, N. K., Fischer, P.

SMALL, 4(11):1956-1958, 2008 (article)

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DOI [BibTex]

2008



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Chiral molecules split light: Reflection and refraction in a chiral liquid

Ghosh, A., Fischer, P.

PHYSICAL REVIEW LETTERS, 97(17), 2006, Featured highlight ‘Fundamental optical physics: Refraction’ Nature Photonics, Nov. 2006. (article)

Abstract
A light beam changes direction as it enters a liquid at an angle from another medium, such as air. Should the liquid contain molecules that lack mirror symmetry, then it has been predicted by Fresnel that the light beam will not only change direction, but will actually split into two separate beams with a small difference in the respective angles of refraction. Here we report the observation of this phenomenon. We also demonstrate that the angle of reflection does not equal the angle of incidence in a chiral medium. Unlike conventional optical rotation, which depends on the path-length through the sample, the reported reflection and refraction phenomena arise within a few wavelengths at the interface and thereby suggest a new approach to polarimetry that can be used in microfluidic volumes.

Featured highlight ‘Fundamental optical physics: Refraction’ Nature Photonics, Nov. 2006.

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DOI [BibTex]

DOI [BibTex]


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Direct chiral discrimination in NMR spectroscopy

Buckingham, A., Fischer, P.

CHEMICAL PHYSICS, 324(1):111-116, 2006 (article)

Abstract
Conventional nuclear magnetic resonance spectroscopy is unable to distinguish between the two mirror-image forms (enantiomers) of a chiral molecule. This is because the NMR spectrum is determined by the chemical shifts and spin-spin coupling constants which - in the absence of a chiral solvent - are identical for the two enantiomers. We discuss how chirality may nevertheless be directly detected in liquid-state NMR spectroscopy: In a chiral molecule, the rotating nuclear magnetic moment induces an electric dipole moment in the direction perpendicular to itself and to the permanent magnetic field of the spectrometer. We present computations of the precessing electric polarization following a pi/2 pulse. Our estimates indicate that the electric polarization should be detectable in favourable cases. We also predict that application of an electrostatic field induces a chirally sensitive magnetization oscillating in the direction of the permanent magnetic field. We show that the electric-field-perturbed chemical shift tensor, the nuclear magnetic shielding polarizability, underlies these chiral NMR effects. (c) 2005 Elsevier B.V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]


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Ring-resonator-based frequency-domain optical activity measurements of a chiral liquid

Vollmer, F., Fischer, P.

OPTICS LETTERS, 31(4):453-455, 2006 (article)

Abstract
Chiral liquids rotate the plane of polarization of linearly polarized light and are therefore optically active. Here we show that optical rotation can be observed in the frequency domain. A chiral liquid introduced in a fiber-loop ring resonator that supports left and right circularly polarized modes gives rise to relative frequency shifts that are a direct measure of the liquid's circular birefringence and hence of its optical activity. The effect is in principle not diminished if the circumference of the ring is reduced. The technique is similarly applicable to refractive index and linear birefringence measurements. (c) 2006 Optical Society of America.

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DOI [BibTex]


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Sign of the refractive index in a gain medium with negative permittivity and permeability

Chen, Y., Fischer, P., Wise, F.

JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 23(1):45-50, 2006 (article)

Abstract
We show how the sign of the refractive index in any medium may be derived using a rigorous analysis based on Einstein causality. In particular, we consider left-handed materials, i.e., media that have negative permittivities and permeabilities at the frequency of interest. We find that the consideration of gain in such media can give rise to a positive refractive index. (c) 2006 Optical Society of America.

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DOI [BibTex]

DOI [BibTex]


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Rocking Stamper and Jumping Snake from a Dynamical System Approach to Artificial Life

Der, R., Hesse, F., Martius, G.

Adaptive Behavior, 14(2):105-115, 2006 (article)

Abstract
Dynamical systems offer intriguing possibilities as a substrate for the generation of behavior because of their rich behavioral complexity. However this complexity together with the largely covert relation between the parameters and the behavior of the agent is also the main hindrance in the goal-oriented design of a behavior system. This paper presents a general approach to the self-regulation of dynamical systems so that the design problem is circumvented. We consider the controller (a neural net work) as the mediator for changes in the sensor values over time and define a dynamics for the parameters of the controller by maximizing the dynamical complexity of the sensorimotor loop under the condition that the consequences of the actions taken are still predictable. This very general principle is given a concrete mathematical formulation and is implemented in an extremely robust and versatile algorithm for the parameter dynamics of the controller. We consider two different applications, a mechanical device called the rocking stamper and the ODE simulations of a "snake" with five degrees of freedom. In these and many other examples studied we observed various behavior modes of high dynamical complexity.

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DOI [BibTex]

DOI [BibTex]


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Nonlinear optical spectroscopy of chiral molecules

Fischer, P., Hache, F.

CHIRALITY, 17(8):421-437, 2005 (article)

Abstract
We review nonlinear optical processes that are specific to chiral molecules in solution and on surfaces. In contrast to conventional natural optical activity phenomena, which depend linearly on the electric field strength of the optical field, we discuss how optical processes that are nonlinear (quadratic, cubic, and quartic) functions of the electromagnetic field strength may probe optically active centers and chiral vibrations. We show that nonlinear techniques open entirely new ways of exploring chirality in chemical and biological systems: The cubic processes give rise to nonlinear circular dichroism and nonlinear optical rotation and make it possible to observe dynamic chiral processes at ultrafast time scales. The quadratic second-harmonic and sum-frequency-generation phenomena and the quartic processes may arise entirely in the electric-dipole approximation and do not require the use of circularly polarized light to detect chirality: They provide surface selectivity and their observables can be relatively much larger than in linear optical activity. These processes also give rise to the generation of light at a new color, and in liquids this frequency conversion only occurs if the solution is optically active. We survey recent chiral nonlinear optical experiments and give examples of their application to problems of biophysical interest. (C) 2005 Wiley-Liss, Inc.

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DOI [BibTex]

DOI [BibTex]


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Negative refraction at optical frequencies in nonmagnetic two-component molecular media

Chen, Y., Fischer, P., Wise, F.

PHYSICAL REVIEW LETTERS, 95(6), 2005 (article)

Abstract
There is significant motivation to develop media with negative refractive indices at optical frequencies, but efforts in this direction are hampered by the weakness of the magnetic response at such frequencies. We show theoretically that a nonmagnetic medium with two atomic or molecular constituents can exhibit a negative refractive index. A negative index is possible even when the real parts of both the permittivity and permeability are positive. This surprising result provides a route to isotropic negative-index media at optical frequencies.

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DOI [BibTex]

DOI [BibTex]