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2013


Quasi-Newton Methods: A New Direction
Quasi-Newton Methods: A New Direction

Hennig, P., Kiefel, M.

Journal of Machine Learning Research, 14(1):843-865, March 2013 (article)

Abstract
Four decades after their invention, quasi-Newton methods are still state of the art in unconstrained numerical optimization. Although not usually interpreted thus, these are learning algorithms that fit a local quadratic approximation to the objective function. We show that many, including the most popular, quasi-Newton methods can be interpreted as approximations of Bayesian linear regression under varying prior assumptions. This new notion elucidates some shortcomings of classical algorithms, and lights the way to a novel nonparametric quasi-Newton method, which is able to make more efficient use of available information at computational cost similar to its predecessors.

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website+code pdf link (url) [BibTex]

2013


website+code pdf link (url) [BibTex]


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Analytical probabilistic modeling for radiation therapy treatment planning

Bangert, M., Hennig, P., Oelfke, U.

Physics in Medicine and Biology, 58(16):5401-5419, 2013 (article)

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PDF DOI [BibTex]

PDF DOI [BibTex]


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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Optimal distribution of contact forces with inverse-dynamics control

Righetti, L., Buchli, J., Mistry, M., Kalakrishnan, M., Schaal, S.

The International Journal of Robotics Research, 32(3):280-298, March 2013 (article)

Abstract
The development of legged robots for complex environments requires controllers that guarantee both high tracking performance and compliance with the environment. More specifically the control of the contact interaction with the environment is of crucial importance to ensure stable, robust and safe motions. In this contribution we develop an inverse-dynamics controller for floating-base robots under contact constraints that can minimize any combination of linear and quadratic costs in the contact constraints and the commands. Our main result is the exact analytical derivation of the controller. Such a result is particularly relevant for legged robots as it allows us to use torque redundancy to directly optimize contact interactions. For example, given a desired locomotion behavior, we can guarantee the minimization of contact forces to reduce slipping on difficult terrains while ensuring high tracking performance of the desired motion. The main advantages of the controller are its simplicity, computational efficiency and robustness to model inaccuracies. We present detailed experimental results on simulated humanoid and quadruped robots as well as a real quadruped robot. The experiments demonstrate that the controller can greatly improve the robustness of locomotion of the robots.1

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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]


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Controlled Reduction with Unactuated Cyclic Variables: Application to 3D Bipedal Walking with Passive Yaw Rotation

Gregg, R., Righetti, L.

IEEE Transactions on Automatic Control, 58(10):2679-2685, October 2013 (article)

Abstract
This technical note shows that viscous damping can shape momentum conservation laws in a manner that stabilizes yaw rotation and enables steering for underactuated 3D walking. We first show that unactuated cyclic variables can be controlled by passively shaped conservation laws given a stabilizing controller in the actuated coordinates. We then exploit this result to realize controlled geometric reduction with multiple unactuated cyclic variables. We apply this underactuated control strategy to a five-link 3D biped to produce exponentially stable straight-ahead walking and steering in the presence of passive yawing.

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link (url) DOI [BibTex]

link (url) 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



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Frequency analysis with coupled nonlinear oscillators

Buchli, J., Righetti, L., Ijspeert, A.

Physica D: Nonlinear Phenomena, 237(13):1705-1718, August 2008 (article)

Abstract
We present a method to obtain the frequency spectrum of a signal with a nonlinear dynamical system. The dynamical system is composed of a pool of adaptive frequency oscillators with negative mean-field coupling. For the frequency analysis, the synchronization and adaptation properties of the component oscillators are exploited. The frequency spectrum of the signal is reflected in the statistics of the intrinsic frequencies of the oscillators. The frequency analysis is completely embedded in the dynamics of the system. Thus, no pre-processing or additional parameters, such as time windows, are needed. Representative results of the numerical integration of the system are presented. It is shown, that the oscillators tune to the correct frequencies for both discrete and continuous spectra. Due to its dynamic nature the system is also capable to track non-stationary spectra. Further, we show that the system can be modeled in a probabilistic manner by means of a nonlinear Fokker–Planck equation. The probabilistic treatment is in good agreement with the numerical results, and provides a useful tool to understand the underlying mechanisms leading to convergence.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]

2005


Nonlinear optical spectroscopy of chiral molecules
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]

2005


DOI [BibTex]


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

1998


Surface second-order nonlinear optical activity
Surface second-order nonlinear optical activity

Fischer, P., Buckingham, A.

JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 15(12):2951-2957, 1998 (article)

Abstract
Following the recent observation of a large second-harmonic intensity difference from a monolayer of chiral molecules with left and right circularly polarized light, the scattering theory is generalized and extended to predict linear and circular intensity differences for the more Versatile sum-frequency spectroscopy. Estimates indicate that intensity differences should be detectable for a typical experimental arrangement. The second-order nonlinear surface susceptibility tensor is given for different surface point groups in the electric dipole approximation; it is shown that nonlinear optical activity phenomena unambiguously probe molecular chirality only for molecular monolayers that are symmetric about the normal. Other surface symmetries can give rise to intensity differences from monolayers composed of achiral molecules. A water surface is predicted to show Linear and nonlinear optical activity in the presence of an electric field parallel to the surface. (C) 1998 Optical Society of America {[}S0740-3224(98)01311-3] OCIS codes: 190.0190, 190.4350, 240.6490.

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DOI [BibTex]

1998


DOI [BibTex]


Linear electro-optic effect in optically active liquids
Linear electro-optic effect in optically active liquids

Buckingham, A., Fischer, P.

CHEMICAL PHYSICS LETTERS, 297(3-4):239-246, 1998 (article)

Abstract
A linear effect of an electrostatic field F on the intensity of sum- and difference-frequency generation in a chiral liquid is predicted. It arises in the electric dipole approximation. The effect changes sign with the enantiomer and on reversing the direction of the electrostatic field. The sum-frequency generator chi(alpha beta gamma)((2)) (-omega(3);omega(1),omega(2)), where omega(3) = omega(1) + omega(2), and the electric field-induced sum-frequency generator chi(alpha beta gamma delta)((3))(-omega(3);omega(1),omega(2),0)F-delta interfere and their contributions to the scattering power can be distinguished. Encouraging predictions are given for a typical experimental arrangement. (C) 1998 Elsevier Science B.V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]


Monolayers of hexadecyltrimethylammonium p-tosylate at the air-water interface. 1. Sum-frequency spectroscopy
Monolayers of hexadecyltrimethylammonium p-tosylate at the air-water interface. 1. Sum-frequency spectroscopy

Bell, G., Li, Z., Bain, C., Fischer, P., Duffy, D.

JOURNAL OF PHYSICAL CHEMISTRY B, 102(47):9461-9472, 1998 (article)

Abstract
Sum-frequency vibrational spectroscopy has been used to determine the structure of monolayers of the cationic surfactant, hexadecyltrimethylammonium p-tosylate (C(16)TA(+)Ts(-)), at the surface of water. Selective deuteration of the cation or the anion allowed the separate detection of sum-frequency spectra of the surfactant and of counterions that are bound to the monolayer. The p-tosylate ions an oriented with their methyl groups pointing away from the aqueous subphase and with the C-2 axis tilted, on average, by 30-40 degrees from the surface normal. The vibrational spectra of C(16)TA(+) indicate that the number of gauche defects in the monolayer does not change dramatically when bromide counterions are replaced by p-tosylate. The ends of the hydrocarbon chains of C16TA+ are, however, tilted much further from the surface normal in the presence of p-tosylate than in the presence of bromide. A quantitative analysis of the sum-frequency spectra requires a knowledge of the molecular hyperpolarizability tensor: the role of ab initio calculations and Raman spectroscopy in determining the components of this tensor is discussed.

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DOI [BibTex]

DOI [BibTex]


Ultraviolet resonance Raman study of drug binding in dihydrofolate reductase, gyrase, and catechol O-methyltransferase
Ultraviolet resonance Raman study of drug binding in dihydrofolate reductase, gyrase, and catechol O-methyltransferase

Couling, V., Fischer, P., Klenerman, D., Huber, W.

BIOPHYSICAL JOURNAL, 75(2):1097-1106, 1998 (article)

Abstract
This paper presents a study of the use of ultraviolet resonance Raman (UVRR) spectroscopic methods as a means of elucidating aspects of drug-protein interactions. Some of the RR vibrational bands of the aromatic amino acids tyrosine and tryptophan are sensitive to the microenvironment, and the use of UV excitation radiation allows selective enhancement of the spectral features of the aromatic amino acids, enabling observation specifically of their change in microenvironment upon drug binding. The three drug-protein systems investigated in this study are dihydrofolate reductase with its inhibitor trimethoprim, gyrase with novobiocin, and catechol O-methyltransferase with dinitrocatechol. It is demonstrated that UVRR spectroscopy has adequate sensitivity to be a useful means of detecting drug-protein interactions in those systems for which the electronic absorption of the aromatic amino acids changes because of hydrogen bonding and/or possible dipole-dipole and dipole-polarizability interactions with the ligand.

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DOI [BibTex]

DOI [BibTex]