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2013


Hybrid nanocolloids with programmed three-dimensional shape and material composition
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]


Chiral Colloidal Molecules And Observation of The Propeller Effect
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]


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


Plasmonic nanohelix metamaterials with tailorable giant circular dichroism
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


Voltage-Controllable Magnetic Composite Based on Multifunctional Polyethylene Microparticles
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


2007


Frequency-domain displacement sensing with a fiber ring-resonator containing a variable gap
Frequency-domain displacement sensing with a fiber ring-resonator containing a variable gap

Vollmer, F., Fischer, P.

SENSORS AND ACTUATORS A-PHYSICAL, 134(2):410-413, 2007 (article)

Abstract
Ring-resonators are in general not amenable to strain-free (non-contact) displacement measurements. We show that this limitation may be overcome if the ring-resonator, here a fiber-loop, is designed to contain a gap, such that the light traverses a free-space part between two aligned waveguide ends. Displacements are determined with nanometer sensitivity by measuring the associated changes in the resonance frequencies. Miniaturization should increase the sensitivity of the ring-resonator interferometer. Ring geometries that contain an optical circulator can be used to profile reflective samples. (c) 2006 Elsevier B.V. All rights reserved.

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DOI [BibTex]

2007


DOI [BibTex]


Observation of the Faraday effect via beam deflection in a longitudinal magnetic field
Observation of the Faraday effect via beam deflection in a longitudinal magnetic field

Ghosh, A., Hill, W., Fischer, P.

PHYSICAL REVIEW A, 76(5), 2007 (article)

Abstract
We show that magnetic-field-induced circular differential deflection of light can be observed in reflection or refraction at a single interface. The difference in the reflection or refraction angles between the two circular polarization components is a function of the magnetic-field strength and the Verdet constant, and permits the observation of the Faraday effect not via polarization rotation in transmission, but via changes in the propagation direction. Deflection measurements do not suffer from n-pi ambiguities and are shown to be another means to map magnetic fields with high axial resolution, or to determine the sign and magnitude of magnetic-field pulses in a single measurement.

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DOI [BibTex]


Circular differential double diffraction in chiral media
Circular differential double diffraction in chiral media

Ghosh, A., Fazal, F. M., Fischer, P.

OPTICS LETTERS, 32(13):1836-1838, 2007 (article)

Abstract
In an optically active liquid the diffraction angle depends on the circular polarization state of the incident light beam. We report the observation of circular differential diffraction in an isotropic chiral medium, and we demonstrate that double diffraction is an alternate means to determine the handedness (enantiomeric excess) of a solution. (c) 2007 Optical Society of America.

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DOI [BibTex]

DOI [BibTex]

2006


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

2006


DOI [BibTex]


Direct chiral discrimination in NMR spectroscopy
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]


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


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

2000


Phenomenological damping in optical response tensors
Phenomenological damping in optical response tensors

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 61(3), 2000 (article)

Abstract
Although perturbation theory applied to the optical response of a molecule or material system is only strictly valid far from resonances, it is often applied to ``near-resonance{''} conditions by means of complex energies incorporating damping. Inconsistent signs of the damping in optical response tensors have appeared in the recent literature, as have errors in the treatment of the perturbation by a static held. The ``equal-sign{''} convention used in a recent publication yields an unphysical material response, and Koroteev's intimation that linear electro-optical circular dichroism may exist in an optically active liquid under resonance conditions is also flawed. We show that the isotropic part of the Pockels tensor vanishes.

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DOI [BibTex]

2000


DOI [BibTex]


Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules
Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules

Champagne, B., Fischer, P., Buckingham, A.

CHEMICAL PHYSICS LETTERS, 331(1):83-88, 2000 (article)

Abstract
Using a sum-over-states procedure based on configuration interaction singles /6-311++G{*}{*}, we have computed the sum-frequency hyperpolarizability beta (ijk)(-3 omega; 2 omega, omega) Of two small chiral molecules, R-monofluoro-oxirane and R-(+)-propylene oxide. Excitation energies were scaled to fit experimental UV-absorption data and checked with ab initio values from time-dependent density functional theory. The isotropic part of the computed hyperpolarizabilities, beta(-3 omega; 2 omega, omega), is much smaller than that reported previously from sum-frequency generation experiments on aqueous solutions of arabinose. Comparison is made with a single-centre chiral model. (C) 2000 Elsevier Science B.V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]


Three-wave mixing in chiral liquids
Three-wave mixing in chiral liquids

Fischer, P., Wiersma, D., Righini, R., Champagne, B., Buckingham, A.

PHYSICAL REVIEW LETTERS, 85(20):4253-4256, 2000 (article)

Abstract
Second-order nonlinear optical frequency conversion in isotropic systems is only dipole allowed for sum- and difference-frequency generation in chiral media. We develop a single-center chiral model of the three-wave mixing (sum:frequency generation) nonlinearity and estimate its magnitude. We also report results from ab initio calculations and from three- and four-wave mixing experiments in support of the theoretical estimates. We show that the second-order susceptibility in chiral liquids is much smaller than previously thought.

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DOI [BibTex]

DOI [BibTex]


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Deep Graph Matching via Blackbox Differentiation of Combinatorial Solvers

Rolinek, M., Swoboda, P., Zietlow, D., Paulus, A., Musil, V., Martius, G.

Arxiv (article)

Abstract
Building on recent progress at the intersection of combinatorial optimization and deep learning, we propose an end-to-end trainable architecture for deep graph matching that contains unmodified combinatorial solvers. Using the presence of heavily optimized combinatorial solvers together with some improvements in architecture design, we advance state-of-the-art on deep graph matching benchmarks for keypoint correspondence. In addition, we highlight the conceptual advantages of incorporating solvers into deep learning architectures, such as the possibility of post-processing with a strong multi-graph matching solver or the indifference to changes in the training setting. Finally, we propose two new challenging experimental setups

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Arxiv [BibTex]