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2009


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In situ synthesis and hydrogen storage properties of PdNi alloy nanoparticles in an ordered mesoporous carbon template

Campesi, R., Cuevas, F., Leroy, E., Hirscher, M., Gadiou, R., Vix-Guterl, C., Latroche, M.

{Microporous and Mesoporous Materials}, 117, pages: 511-514, 2009 (article)

mms

DOI [BibTex]

2009


DOI [BibTex]


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On-line learning and modulation of periodic movements with nonlinear dynamical systems

Gams, A., Ijspeert, A., Schaal, S., Lenarčič, J.

Autonomous Robots, 27(1):3-23, 2009, clmc (article)

Abstract
Abstract  The paper presents a two-layered system for (1) learning and encoding a periodic signal without any knowledge on its frequency and waveform, and (2) modulating the learned periodic trajectory in response to external events. The system is used to learn periodic tasks on a humanoid HOAP-2 robot. The first layer of the system is a dynamical system responsible for extracting the fundamental frequency of the input signal, based on adaptive frequency oscillators. The second layer is a dynamical system responsible for learning of the waveform based on a built-in learning algorithm. By combining the two dynamical systems into one system we can rapidly teach new trajectories to robots without any knowledge of the frequency of the demonstration signal. The system extracts and learns only one period of the demonstration signal. Furthermore, the trajectories are robust to perturbations and can be modulated to cope with a dynamic environment. The system is computationally inexpensive, works on-line for any periodic signal, requires no additional signal processing to determine the frequency of the input signal and can be applied in parallel to multiple dimensions. Additionally, it can adapt to changes in frequency and shape, e.g. to non-stationary signals, such as hand-generated signals and human demonstrations.

am

link (url) [BibTex]

link (url) [BibTex]


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Local dimensionality reduction for non-parametric regression

Hoffman, H., Schaal, S., Vijayakumar, S.

Neural Processing Letters, 2009, clmc (article)

Abstract
Locally-weighted regression is a computationally-efficient technique for non-linear regression. However, for high-dimensional data, this technique becomes numerically brittle and computationally too expensive if many local models need to be maintained simultaneously. Thus, local linear dimensionality reduction combined with locally-weighted regression seems to be a promising solution. In this context, we review linear dimensionality-reduction methods, compare their performance on nonparametric locally-linear regression, and discuss their ability to extend to incremental learning. The considered methods belong to the following three groups: (1) reducing dimensionality only on the input data, (2) modeling the joint input-output data distribution, and (3) optimizing the correlation between projection directions and output data. Group 1 contains principal component regression (PCR); group 2 contains principal component analysis (PCA) in joint input and output space, factor analysis, and probabilistic PCA; and group 3 contains reduced rank regression (RRR) and partial least squares (PLS) regression. Among the tested methods, only group 3 managed to achieve robust performance even for a non-optimal number of components (factors or projection directions). In contrast, group 1 and 2 failed for fewer components since these methods rely on the correct estimate of the true intrinsic dimensionality. In group 3, PLS is the only method for which a computationally-efficient incremental implementation exists. Thus, PLS appears to be ideally suited as a building block for a locally-weighted regressor in which projection directions are incrementally added on the fly.

am

link (url) [BibTex]

link (url) [BibTex]


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Enhanced adhesion by gecko-inspired hierarchical fibrillar adhesives

Murphy, M. P., Kim, S., Sitti, M.

ACS applied materials \& interfaces, 1(4):849-855, American Chemical Society, 2009 (article)

pi

Project Page [BibTex]

Project Page [BibTex]


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Miniature devices: Voyage of the microrobots

Sitti, M.

Nature, 458(7242):1121-1122, Nature Publishing Group, 2009 (article)

pi

[BibTex]

[BibTex]


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Dry spinning based spinneret based tunable engineered parameters (STEP) technique for controlled and aligned deposition of polymeric nanofibers

Nain, A. S., Sitti, M., Jacobson, A., Kowalewski, T., Amon, C.

Macromolecular rapid communications, 30(16):1406-1412, WILEY-VCH Verlag, 2009 (article)

pi

[BibTex]

[BibTex]


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Two-dimensional contact and noncontact micromanipulation in liquid using an untethered mobile magnetic microrobot

Floyd, S., Pawashe, C., Sitti, M.

IEEE Transactions on Robotics, 25(6):1332-1342, IEEE, 2009 (article)

pi

[BibTex]

[BibTex]


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Mit Röntgenblitzen zu neuen Erkenntnissen

Hedderich, R., Weigand, M., Baretzky, B.

{Nanotechnik - Molek\"ule Materialien Mikrosysteme}, (6 (Beilage zu Photonik 41. 2009)), 2009 (article)

mms

[BibTex]

[BibTex]


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Second-order faceting-roughening of the tilt grain boundary in zinc

Straumal, B. B., Gornakova, A. S., Sursaeva, V. G., Yashnikov, V. P.

{International Journal of Materials Research}, 100(4):525-529, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Improvement of interface structure and magnetic properties of Co on Si (100) by surfactant (Sb) mediated growth

Dash, S. P., Goll, D., Carstanjen, H. D.

{Applied Physics A}, 97(3):651-656, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Effect of severe plastic deformation on the coercivity of Co-Cu alloys

Straumal, B. B., Protasova, S. G., Mazilkin, A. A., Baretzky, B., Goll, D., Gunderov, D. V., Valiev, R. Z.

{Philosophical Magazine Letters}, 89(10):649-654, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Magnetic properties of cobalt-covered MgB2 films

Treiber, S., Stuhlhofer, B., Habermeier, H.-U., Albrecht, J.

{Superconductor Science and Technology}, 22, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Reconstruction of historic alloys for pipe organs brings true Baroque music back to life

Baretzky, B., Friesel, M., Straumal, B.

{Japan Organist}, 36, pages: 29-38, 2009 (article)

mms

[BibTex]

[BibTex]


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Exchange-coupled L10-FePt/Fe composite patterns with perpendicular magnetization

Breitling, A., Bublat, T., Goll, D.

{Physica Status Solidi - Rapid Research Letters}, 3(5):130-132, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Proton NMR studies of the NaAlH4 structure

Valiente-Banuet, L. E., Majer, G., Müller, K.

{Journal of Magnetic Resonance}, 200, pages: 280-284, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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A scaled bilateral control system for experimental one-dimensional teleoperated nanomanipulation

Onal, C. D., Sitti, M.

The International Journal of Robotics Research, 28(4):484-497, Sage Publications, 2009 (article)

pi

[BibTex]

[BibTex]


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A Swallowable Tethered Capsule Endoscope for Diagnosing Barrett’s Esophagus

Glass, P., Sitti, M., Pennathur, A., Appasamy, R.

Gastrointestinal Endoscopy, 69(5):AB106, Mosby, 2009 (article)

pi

Project Page [BibTex]

Project Page [BibTex]


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Adhesion of biologically inspired polymer microfibers on soft surfaces

Cheung, E., Sitti, M.

Langmuir, 25(12):6613-6616, ACS Publications, 2009 (article)

pi

[BibTex]

[BibTex]


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Dangling chain elastomers as repeatable fibrillar adhesives

Sitti, M., Cusick, B., Aksak, B., Nese, A., Lee, H., Dong, H., Kowalewski, T., Matyjaszewski, K.

ACS applied materials \& interfaces, 1(10):2277-2287, American Chemical Society, 2009 (article)

pi

[BibTex]

[BibTex]


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A Sensor-Based Learning Algorithm for the Self-Organization of Robot Behavior

Hesse, F., Martius, G., Der, R., Herrmann, J. M.

Algorithms, 2(1):398-409, 2009 (article)

Abstract
Ideally, sensory information forms the only source of information to a robot. We consider an algorithm for the self-organization of a controller. At short timescales the controller is merely reactive but the parameter dynamics and the acquisition of knowledge by an internal model lead to seemingly purposeful behavior on longer timescales. As a paradigmatic example, we study the simulation of an underactuated snake-like robot. By interacting with the real physical system formed by the robotic hardware and the environment, the controller achieves a sensitive and body-specific actuation of the robot.

al

link (url) [BibTex]

link (url) [BibTex]


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Magnetism of FePt surface alloys

Honolka, J., Lee, T. Y., Kuhnke, K., Enders, A., Skomski, R., Bornemann, S., Mankovsky, S., Minár, J., Staunton, J., Ebert, H., Hessler, M., Fauth, K., Schütz, G., Buchsbaum, A., Schmid, M., Varga, P., Kern, K.

{Physical Review Letters}, 102(6), 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Enhanced 95Zr diffusion in grain boundaries of nano-crystalline ZrO2 \mbox⋅ 9.5 mol\textpercent Y2O3

Drings, H., Brossmann, U., Carstanjen, H. D., Szökefalvi-Nagy, A., Noll, C., Schaefer, H.-E.

{Physica Status Solidi (A)}, 206(1):54-58, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Magnetism of nanostructured materials for advanced magnetic recording

Goll, D.

{International Journal of Materials Research}, 100, pages: 652-662, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Vortex core switching by coherent excitation with single in-plane magnetic field pulses

Weigand, M., van Waeyenberge, B., Vansteenkiste, A., Curcic, M., Sackmann, V., Stoll, H., Tyliszczak, T., Kaznatcheev, K., Bertwistle, D., Woltersdorf, G., Back, C. H., Schütz, G.

{Physical Review Letters}, 102, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Increase of Mn solubility with decreasing grain size in ZnO

Straumal, B., Baretzky, B., Mazilkin, A., Protasova, S., Myatiev, A., Straumal, P.

{Journal of the European Ceramic Society}, 29(10):1963-1970, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Fe-C nanograined alloys obtained by high-pressure torsion: Structure and magnetic properties

Straumal, B. B., Mazilkin, A. A., Protasova, S. G., Dobatkin, S. V., Rodin, A. O., Baretzky, B., Goll, D., Schütz, G.

{Materials Science and Engineering A}, 503, pages: 185-189, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Chiral symmetry breaking of magnetic vortices by sample roughness

Vansteenkiste, A., Weigand, M., Curcic, M., Stoll, H., Schütz, G., Van Waeyenberge, B.

{New Journal of Physics}, 11, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Extended s-d model for magnetization dynamics of strongly noncollinear configurations

De Angeli, L., Steiauf, D., Singer, R., Köberle, I., Dietermann, F., Fähnle, M.

{Physical Review B}, 79, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Incorporating Muscle Activation-Contraction dynamics to an optimal control framework for finger movements

Theodorou, Evangelos A., Valero-Cuevas, Francisco J.

Abstracts of Neural Control of Movement Conference (NCM 2009), 2009, clmc (article)

Abstract
Recent experimental and theoretical work [1] investigated the neural control of contact transition between motion and force during tapping with the index finger as a nonlinear optimization problem. Such transitions from motion to well-directed contact force are a fundamental part of dexterous manipulation. There are 3 alternative hypotheses of how this transition could be accomplished by the nervous system as a function of changes in direction and magnitude of the torque vector controlling the finger. These hypotheses are 1) an initial change in direction with a subsequent change in magnitude of the torque vector; 2) an initial change in magnitude with a subsequent directional change of the torque vector; and 3) a simultaneous and proportionally equal change of both direction and magnitude of the torque vector. Experimental work in [2] shows that the nervous system selects the first strategy, and in [1] we suggest that this may in fact be the optimal strategy. In [4] the framework of Iterative Linear Quadratic Optimal Regulator (ILQR) was extended to incorporate motion and force control. However, our prior simulation work assumed direct and instantaneous control of joint torques, which ignores the known delays and filtering properties of skeletal muscle. In this study, we implement an ILQR controller for a more biologically plausible biomechanical model of the index finger than [4], and add activation-contraction dynamics to the system to simulate muscle function. The planar biomechanical model includes the kinematics of the 3 joints while the applied torques are driven by activation?contraction dynamics with biologically plausible time constants [3]. In agreement with our experimental work [2], the task is to, within 500 ms, move the finger from a given resting configuration to target configuration with a desired terminal velocity. ILQR does not only stabilize the finger dynamics according to the objective function, but it also generates smooth joint space trajectories with minimal tuning and without an a-priori initial control policy (which is difficult to find for highly dimensional biomechanical systems). Furthemore, the use of this optimal control framework and the addition of activation-contraction dynamics considers the full nonlinear dynamics of the index finger and produces a sequence of postures which are compatible with experimental motion data [2]. These simulations combined with prior experimental results suggest that optimal control is a strong candidate for the generation of finger movements prior to abrupt motion-to-force transitions. This work is funded in part by grants NIH R01 0505520 and NSF EFRI-0836042 to Dr. Francisco J. Valero- Cuevas 1 Venkadesan M, Valero-Cuevas FJ. 
Effects of neuromuscular lags on controlling contact transitions. 
Philosophical Transactions of the Royal Society A: 2008. 2 Venkadesan M, Valero-Cuevas FJ. 
Neural Control of Motion-to-Force Transitions with the Fingertip. 
J. Neurosci., Feb 2008; 28: 1366 - 1373; 3 Zajac. Muscle and tendon: properties, models, scaling, and application to biomechanics and motor control. Crit Rev Biomed Eng, 17 4. Weiwei Li., Francisco Valero Cuevas: ?Linear Quadratic Optimal Control of Contact Transition with Fingertip ? ACC 2009

am

PDF [BibTex]

PDF [BibTex]


no image
On-line learning and modulation of periodic movements with nonlinear dynamical systems

Gams, A., Ijspeert, A., Schaal, S., Lenarčič, J.

Autonomous Robots, 27(1):3-23, 2009, clmc (article)

Abstract
Abstract  The paper presents a two-layered system for (1) learning and encoding a periodic signal without any knowledge on its frequency and waveform, and (2) modulating the learned periodic trajectory in response to external events. The system is used to learn periodic tasks on a humanoid HOAP-2 robot. The first layer of the system is a dynamical system responsible for extracting the fundamental frequency of the input signal, based on adaptive frequency oscillators. The second layer is a dynamical system responsible for learning of the waveform based on a built-in learning algorithm. By combining the two dynamical systems into one system we can rapidly teach new trajectories to robots without any knowledge of the frequency of the demonstration signal. The system extracts and learns only one period of the demonstration signal. Furthermore, the trajectories are robust to perturbations and can be modulated to cope with a dynamic environment. The system is computationally inexpensive, works on-line for any periodic signal, requires no additional signal processing to determine the frequency of the input signal and can be applied in parallel to multiple dimensions. Additionally, it can adapt to changes in frequency and shape, e.g. to non-stationary signals, such as hand-generated signals and human demonstrations.

am

link (url) [BibTex]

link (url) [BibTex]


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Reversible dry micro-fibrillar adhesives with thermally controllable adhesion

Kim, S., Sitti, M., Xie, T., Xiao, X.

Soft Matter, 5(19):3689-3693, Royal Society of Chemistry, 2009 (article)

pi

Project Page [BibTex]

Project Page [BibTex]


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Enhanced reversible adhesion of dopamine methacrylamide-coated elastomer microfibrillar structures under wet conditions

Glass, P., Chung, H., Washburn, N. R., Sitti, M.

Langmuir, 25(12):6607-6612, ACS Publications, 2009 (article)

pi

Project Page [BibTex]

Project Page [BibTex]


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Superconducting phase formation in random neck syntheses: a study of the Y-Ba-Cu-O system by magneto-optics and magnetometry

Willems, J. B., Albrecht, J., Landau, I. L., Hulliger, J.

{Superconductor Science and Technology}, 22, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Determination of spin moments from magnetic EXAFS

Popescu, V., Gü\ssmann, M., Fähnle, M., Schütz, G.

{Physical Review B}, 79, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Linewidth of ferromagnetic resonance for systems with anisotropic damping

Seib, J., Steiauf, D., Fähnle, M.

{Physical Review B}, 79, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Structural and magnetic deconvolution of FePt/FeOx-nanoparticles using x-ray magnetic circular dichroism

Nolle, D., Goering, E., Tietze, T., Schütz, G., Figuerola, A., Manna, L.

{New Journal of Physics}, 11, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Magnetic imaging with femtosecond temporal resolution

Li, J., Lee, M.-S., He, W., Redeker, B., Remhof, A., Amaladass, E., Hassel, C., Eimüller, T.

{Review of Scientific Instruments}, 80(7), 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Elliott-Yafet mechanism and the discussion of femtosecond magnetization dynamics

Steiauf, D., Fähnle, M.

{Physical Review B}, 79, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]


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Investigation of the stability of Mn12 single molecule magnets

Voss, S., Fonin, M., Burova, L., Burgert, M., Dedkov, Y. S., Preobrajenski, A. B., Goering, E., Groth, U., Kaul, A. R., Ruediger, U.

{Applied Physics A}, 94(3):491-495, 2009 (article)

mms

DOI [BibTex]

DOI [BibTex]

2002


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Learning with Kernels: Support Vector Machines, Regularization, Optimization, and Beyond

Schölkopf, B., Smola, A.

pages: 644, Adaptive Computation and Machine Learning, MIT Press, Cambridge, MA, USA, December 2002, Parts of this book, including an introduction to kernel methods, can be downloaded here. (book)

Abstract
In the 1990s, a new type of learning algorithm was developed, based on results from statistical learning theory: the Support Vector Machine (SVM). This gave rise to a new class of theoretically elegant learning machines that use a central concept of SVMs-kernels—for a number of learning tasks. Kernel machines provide a modular framework that can be adapted to different tasks and domains by the choice of the kernel function and the base algorithm. They are replacing neural networks in a variety of fields, including engineering, information retrieval, and bioinformatics. Learning with Kernels provides an introduction to SVMs and related kernel methods. Although the book begins with the basics, it also includes the latest research. It provides all of the concepts necessary to enable a reader equipped with some basic mathematical knowledge to enter the world of machine learning using theoretically well-founded yet easy-to-use kernel algorithms and to understand and apply the powerful algorithms that have been developed over the last few years.

ei

Web [BibTex]

2002


Web [BibTex]


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Constructing Boosting algorithms from SVMs: an application to one-class classification.

Rätsch, G., Mika, S., Schölkopf, B., Müller, K.

IEEE Transactions on Pattern Analysis and Machine Intelligence, 24(9):1184-1199, September 2002 (article)

Abstract
We show via an equivalence of mathematical programs that a support vector (SV) algorithm can be translated into an equivalent boosting-like algorithm and vice versa. We exemplify this translation procedure for a new algorithm—one-class leveraging—starting from the one-class support vector machine (1-SVM). This is a first step toward unsupervised learning in a boosting framework. Building on so-called barrier methods known from the theory of constrained optimization, it returns a function, written as a convex combination of base hypotheses, that characterizes whether a given test point is likely to have been generated from the distribution underlying the training data. Simulations on one-class classification problems demonstrate the usefulness of our approach.

ei

DOI [BibTex]

DOI [BibTex]


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Forward models in visuomotor control

Mehta, B., Schaal, S.

J Neurophysiol, 88(2):942-53, August 2002, clmc (article)

Abstract
In recent years, an increasing number of research projects investigated whether the central nervous system employs internal models in motor control. While inverse models in the control loop can be identified more readily in both motor behavior and the firing of single neurons, providing direct evidence for the existence of forward models is more complicated. In this paper, we will discuss such an identification of forward models in the context of the visuomotor control of an unstable dynamic system, the balancing of a pole on a finger. Pole balancing imposes stringent constraints on the biological controller, as it needs to cope with the large delays of visual information processing while keeping the pole at an unstable equilibrium. We hypothesize various model-based and non-model-based control schemes of how visuomotor control can be accomplished in this task, including Smith Predictors, predictors with Kalman filters, tapped-delay line control, and delay-uncompensated control. Behavioral experiments with human participants allow exclusion of most of the hypothesized control schemes. In the end, our data support the existence of a forward model in the sensory preprocessing loop of control. As an important part of our research, we will provide a discussion of when and how forward models can be identified and also the possible pitfalls in the search for forward models in control.

am

link (url) [BibTex]

link (url) [BibTex]


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The contributions of color to recognition memory for natural scenes

Wichmann, F., Sharpe, L., Gegenfurtner, K.

Journal of Experimental Psychology: Learning, Memory and Cognition, 28(3):509-520, May 2002 (article)

Abstract
The authors used a recognition memory paradigm to assess the influence of color information on visual memory for images of natural scenes. Subjects performed 5-10% better for colored than for black-and-white images independent of exposure duration. Experiment 2 indicated little influence of contrast once the images were suprathreshold, and Experiment 3 revealed that performance worsened when images were presented in color and tested in black and white, or vice versa, leading to the conclusion that the surface property color is part of the memory representation. Experiments 4 and 5 exclude the possibility that the superior recognition memory for colored images results solely from attentional factors or saliency. Finally, the recognition memory advantage disappears for falsely colored images of natural scenes: The improvement in recognition memory depends on the color congruence of presented images with learned knowledge about the color gamut found within natural scenes. The results can be accounted for within a multiple memory systems framework.

ei

PDF Web DOI [BibTex]

PDF Web DOI [BibTex]


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Training invariant support vector machines

DeCoste, D., Schölkopf, B.

Machine Learning, 46(1-3):161-190, January 2002 (article)

Abstract
Practical experience has shown that in order to obtain the best possible performance, prior knowledge about invariances of a classification problem at hand ought to be incorporated into the training procedure. We describe and review all known methods for doing so in support vector machines, provide experimental results, and discuss their respective merits. One of the significant new results reported in this work is our recent achievement of the lowest reported test error on the well-known MNIST digit recognition benchmark task, with SVM training times that are also significantly faster than previous SVM methods.

ei

PDF DOI [BibTex]

PDF DOI [BibTex]


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Contrast discrimination with sinusoidal gratings of different spatial frequency

Bird, C., Henning, G., Wichmann, F.

Journal of the Optical Society of America A, 19(7), pages: 1267-1273, 2002 (article)

Abstract
The detectability of contrast increments was measured as a function of the contrast of a masking or “pedestal” grating at a number of different spatial frequencies ranging from 2 to 16 cycles per degree of visual angle. The pedestal grating always had the same orientation, spatial frequency and phase as the signal. The shape of the contrast increment threshold versus pedestal contrast (TvC) functions depend of the performance level used to define the “threshold,” but when both axes are normalized by the contrast corresponding to 75% correct detection at each frequency, the (TvC) functions at a given performance level are identical. Confidence intervals on the slope of the rising part of the TvC functions are so wide that it is not possible with our data to reject Weber’s Law.

ei

PDF [BibTex]

PDF [BibTex]


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Support Vector Machines and Kernel Methods: The New Generation of Learning Machines

Cristianini, N., Schölkopf, B.

AI Magazine, 23(3):31-41, 2002 (article)

ei

[BibTex]


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Contrast discrimination with pulse-trains in pink noise

Henning, G., Bird, C., Wichmann, F.

Journal of the Optical Society of America A, 19(7), pages: 1259-1266, 2002 (article)

Abstract
Detection performance was measured with sinusoidal and pulse-train gratings. Although the 2.09-c/deg pulse-train, or line gratings, contained at least 8 harmonics all at equal contrast, they were no more detectable than their most detectable component. The addition of broadband pink noise designed to equalize the detectability of the components of the pulse train made the pulse train about a factor of four more detectable than any of its components. However, in contrast-discrimination experiments, with a pedestal or masking grating of the same form and phase as the signal and 15% contrast, the noise did not affect the discrimination performance of the pulse train relative to that obtained with its sinusoidal components. We discuss the implications of these observations for models of early vision in particular the implications for possible sources of internal noise.

ei

PDF [BibTex]

PDF [BibTex]


Chirality-specific nonlinear spectroscopies in isotropic media
Chirality-specific nonlinear spectroscopies in isotropic media

Fischer, P., Albrecht, A.

BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 75(5):1119-1124, 2002, 10th International Conference on Time-Resolved Vibrational Spectroscopy (TRVS 2001), OKAZZAKI, JAPAN, MAY 21-25, 2001 (article)

Abstract
Sum or difference frequency generation (SFG or DFG) in isotropic media is in the electric-dipole approximation only symmetry allowed for optically active systems. The hyperpolarizability giving rise to these three-wave mixing processes features only one isotropic component. It factorizes into two terms, an energy (denominator) factor and a triple product of transition moments. These forbid degenerate SFG, i.e., second harmonic generation, as well as the existence of the linear electrooptic effect (Pockels effect) in isotropic media. This second order response also has no static limit, which leads to particularly strong resonance phenomena that are qualitatively different from those usually seen in the ubiquitous even-wave mixing spectroscopies. In particular, the participation of two (not the usual one) excited states is essential to achieve dramatic resonance enhancement, We report our first efforts to see such resonantly enhanced chirality specific SFG.

pf

DOI [BibTex]

DOI [BibTex]


The chiral specificity of sum-frequency generation in solutions
The chiral specificity of sum-frequency generation in solutions

Fischer, P., Beckwitt, K., Wise, F., Albrecht, A.

CHEMICAL PHYSICS LETTERS, 352(5-6):463-468, 2002 (article)

Abstract
Sum-frequency generation in isotropic media is in the electric-dipole approximation the only symmetry allowed for chiral systems. We demonstrate that the sum-frequency intensity from an optically active liquid depends quadratically on the difference in concentration of the two enantiomers. The dominant contribution to the signal is found to be due to the chirality specific electric-dipolar three-wave mixing nonlinearity. Selecting the polarization of all fields allows the chiral electric-dipolar contributions to the bulk sum-frequency signal to be discerned from any achiral magnetic-dipolar and electric-quadrupolar contributions. (C) 2002 Published by Elsevier Science B.V.

pf

DOI [BibTex]

DOI [BibTex]


On optical rectification in isotropic media
On optical rectification in isotropic media

Fischer, P., Albrecht, A.

LASER PHYSICS, 12(8):1177-1181, 2002 (article)

Abstract
Coherent nonlinear optical processes at second-order are only electric-dipole allowed in isotropic media that are optically active. Sum-frequency generation in chiral liquids has recently been observed, and difference-frequency and optical rectification have been predicted to exist in isotropic chiral media. Both Rayleigh-Schrodinger perturbation theory and the density matrix approach are used to discuss the quantum-chemical basis of optical rectification in optically active liquids. For pinene we compute the corresponding orientationally averaged hyperpolarizability, and estimate the light-induced dc electric polarization and the consequent voltage across a measuring capacitor it may give rise to near resonance.

pf

[BibTex]

[BibTex]