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2015


Scalable Robust Principal Component Analysis using {Grassmann} Averages
Scalable Robust Principal Component Analysis using Grassmann Averages

Hauberg, S., Feragen, A., Enficiaud, R., Black, M.

IEEE Trans. Pattern Analysis and Machine Intelligence (PAMI), December 2015 (article)

Abstract
In large datasets, manual data verification is impossible, and we must expect the number of outliers to increase with data size. While principal component analysis (PCA) can reduce data size, and scalable solutions exist, it is well-known that outliers can arbitrarily corrupt the results. Unfortunately, state-of-the-art approaches for robust PCA are not scalable. We note that in a zero-mean dataset, each observation spans a one-dimensional subspace, giving a point on the Grassmann manifold. We show that the average subspace corresponds to the leading principal component for Gaussian data. We provide a simple algorithm for computing this Grassmann Average (GA), and show that the subspace estimate is less sensitive to outliers than PCA for general distributions. Because averages can be efficiently computed, we immediately gain scalability. We exploit robust averaging to formulate the Robust Grassmann Average (RGA) as a form of robust PCA. The resulting Trimmed Grassmann Average (TGA) is appropriate for computer vision because it is robust to pixel outliers. The algorithm has linear computational complexity and minimal memory requirements. We demonstrate TGA for background modeling, video restoration, and shadow removal. We show scalability by performing robust PCA on the entire Star Wars IV movie; a task beyond any current method. Source code is available online.

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preprint pdf from publisher supplemental Project Page [BibTex]

2015


preprint pdf from publisher supplemental Project Page [BibTex]


Enzymatically active biomimetic micropropellers for the penetration of mucin gels
Enzymatically active biomimetic micropropellers for the penetration of mucin gels

Walker (Schamel), D., Käsdorf, B. T., Jeong, H. H., Lieleg, O., Fischer, P.

Science Advances, 1(11):e1500501, December 2015 (article)

Abstract
In the body, mucus provides an important defense mechanism by limiting the penetration of pathogens. It is therefore also a major obstacle for the efficient delivery of particle-based drug carriers. The acidic stomach lining in particular is difficult to overcome because mucin glycoproteins form viscoelastic gels under acidic conditions. The bacterium Helicobacter pylori has developed a strategy to overcome the mucus barrier by producing the enzyme urease, which locally raises the pH and consequently liquefies the mucus. This allows the bacteria to swim through mucus and to reach the epithelial surface. We present an artificial system of reactive magnetic micropropellers that mimic this strategy to move through gastric mucin gels by making use of surface-immobilized urease. The results demonstrate the validity of this biomimetic approach to penetrate biological gels, and show that externally propelled microstructures can actively and reversibly manipulate the physical state of their surroundings, suggesting that such particles could potentially penetrate native mucus.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


{SMPL}: A Skinned Multi-Person Linear Model
SMPL: A Skinned Multi-Person Linear Model

Loper, M., Mahmood, N., Romero, J., Pons-Moll, G., Black, M. J.

ACM Trans. Graphics (Proc. SIGGRAPH Asia), 34(6):248:1-248:16, ACM, New York, NY, October 2015 (article)

Abstract
We present a learned model of human body shape and pose-dependent shape variation that is more accurate than previous models and is compatible with existing graphics pipelines. Our Skinned Multi-Person Linear model (SMPL) is a skinned vertex-based model that accurately represents a wide variety of body shapes in natural human poses. The parameters of the model are learned from data including the rest pose template, blend weights, pose-dependent blend shapes, identity-dependent blend shapes, and a regressor from vertices to joint locations. Unlike previous models, the pose-dependent blend shapes are a linear function of the elements of the pose rotation matrices. This simple formulation enables training the entire model from a relatively large number of aligned 3D meshes of different people in different poses. We quantitatively evaluate variants of SMPL using linear or dual-quaternion blend skinning and show that both are more accurate than a Blend-SCAPE model trained on the same data. We also extend SMPL to realistically model dynamic soft-tissue deformations. Because it is based on blend skinning, SMPL is compatible with existing rendering engines and we make it available for research purposes.

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pdf video code/model errata DOI Project Page Project Page [BibTex]

pdf video code/model errata DOI Project Page Project Page [BibTex]


The EChemPen: A Guiding Hand To Learn Electrochemical Surface Modifications
The EChemPen: A Guiding Hand To Learn Electrochemical Surface Modifications

Valetaud, M., Loget, G., Roche, J., Hueken, N., Fattah, Z., Badets, V., Fontaine, O., Zigah, D.

J. of Chem. Ed., 92(10):1700-1704, September 2015 (article)

Abstract
The Electrochemical Pen (EChemPen) was developed as an attractive tool for learning electrochemistry. The fabrication, principle, and operation of the EChemPen are simple and can be easily performed by students in practical classes. It is based on a regular fountain pen principle, where the electrolytic solution is dispensed at a tip to locally modify a conductive surface by triggering a localized electrochemical reaction. Three simple model reactions were chosen to demonstrate the versatility of the EChemPen for teaching various electrochemical processes. We describe first the reversible writing/erasing of metal letters, then the electrodeposition of a black conducting polymer "ink", and finally the colorful writings that can be generated by titanium anodization and that can be controlled by the applied potential. These entertaining and didactic experiments are adapted for teaching undergraduate students that start to study electrochemistry by means of surface modification reactions.

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DOI [BibTex]

DOI [BibTex]


Dyna: A Model of Dynamic Human Shape in Motion
Dyna: A Model of Dynamic Human Shape in Motion

Pons-Moll, G., Romero, J., Mahmood, N., Black, M. J.

ACM Transactions on Graphics, (Proc. SIGGRAPH), 34(4):120:1-120:14, ACM, August 2015 (article)

Abstract
To look human, digital full-body avatars need to have soft tissue deformations like those of real people. We learn a model of soft-tissue deformations from examples using a high-resolution 4D capture system and a method that accurately registers a template mesh to sequences of 3D scans. Using over 40,000 scans of ten subjects, we learn how soft tissue motion causes mesh triangles to deform relative to a base 3D body model. Our Dyna model uses a low-dimensional linear subspace to approximate soft-tissue deformation and relates the subspace coefficients to the changing pose of the body. Dyna uses a second-order auto-regressive model that predicts soft-tissue deformations based on previous deformations, the velocity and acceleration of the body, and the angular velocities and accelerations of the limbs. Dyna also models how deformations vary with a person’s body mass index (BMI), producing different deformations for people with different shapes. Dyna realistically represents the dynamics of soft tissue for previously unseen subjects and motions. We provide tools for animators to modify the deformations and apply them to new stylized characters.

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pdf preprint video data DOI Project Page Project Page [BibTex]

pdf preprint video data DOI Project Page Project Page [BibTex]


Linking Objects to Actions: Encoding of Target Object and Grasping Strategy in Primate Ventral Premotor Cortex
Linking Objects to Actions: Encoding of Target Object and Grasping Strategy in Primate Ventral Premotor Cortex

Vargas-Irwin, C. E., Franquemont, L., Black, M. J., Donoghue, J. P.

Journal of Neuroscience, 35(30):10888-10897, July 2015 (article)

Abstract
Neural activity in ventral premotor cortex (PMv) has been associated with the process of matching perceived objects with the motor commands needed to grasp them. It remains unclear how PMv networks can flexibly link percepts of objects affording multiple grasp options into a final desired hand action. Here, we use a relational encoding approach to track the functional state of PMv neuronal ensembles in macaque monkeys through the process of passive viewing, grip planning, and grasping movement execution. We used objects affording multiple possible grip strategies. The task included separate instructed delay periods for object presentation and grip instruction. This approach allowed us to distinguish responses elicited by the visual presentation of the objects from those associated with selecting a given motor plan for grasping. We show that PMv continuously incorporates information related to object shape and grip strategy as it becomes available, revealing a transition from a set of ensemble states initially most closely related to objects, to a new set of ensemble patterns reflecting unique object-grip combinations. These results suggest that PMv dynamically combines percepts, gradually navigating toward activity patterns associated with specific volitional actions, rather than directly mapping perceptual object properties onto categorical grip representations. Our results support the idea that PMv is part of a network that dynamically computes motor plans from perceptual information. Significance Statement: The present work demonstrates that the activity of groups of neurons in primate ventral premotor cortex reflects information related to visually presented objects, as well as the motor strategy used to grasp them, linking individual objects to multiple possible grips. PMv could provide useful control signals for neuroprosthetic assistive devices designed to interact with objects in a flexible way.

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publisher link DOI Project Page [BibTex]

publisher link DOI Project Page [BibTex]


Optimal Length of Low Reynolds Number Nanopropellers
Optimal Length of Low Reynolds Number Nanopropellers

Walker (Schamel), D., Kuebler, M., Morozov, K. I., Fischer, P., Leshansky, A. M.

Nano Letters, 15(7):4412-4416, June 2015 (article)

Abstract
Locomotion in fluids at the nanoscale is dominated by viscous drag. One efficient propulsion scheme is to use a weak rotating magnetic field that drives a chiral object. Froth bacterial flagella to artificial drills, the corkscrew is a universally useful chiral shape for propulsion in viscous environments. Externally powered magnetic micro- and nanomotors have been recently developed that allow for precise fuel-free propulsion in complex media. Here, we combine analytical and numerical theory with experiments on nanostructured screw-propellers to show that the optimal length is surprisingly short only about one helical turn, which is shorter than most of the structures in use to date. The results have important implications for the design of artificial actuated nano- and micropropellers and can dramatically reduce fabrication times, while ensuring optimal performance.

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DOI [BibTex]

DOI [BibTex]


A theoretical study of potentially observable chirality-sensitive NMR effects in molecules
A theoretical study of potentially observable chirality-sensitive NMR effects in molecules

Garbacz, P., Cukras, J., Jaszunski, M.

Phys. Chem. Chem. Phys., 17(35):22642-22651, May 2015 (article)

Abstract
Two recently predicted nuclear magnetic resonance effects, the chirality-induced rotating electric polarization and the oscillating magnetization, are examined for several experimentally available chiral molecules. We discuss in detail the requirements for experimental detection of chirality-sensitive NMR effects of the studied molecules. These requirements are related to two parameters: the shielding polarizability and the antisymmetric part of the nuclear magnetic shielding tensor. The dominant second contribution has been computed for small molecules at the coupled cluster and density functional theory levels. It was found that DFT calculations using the KT2 functional and the aug-cc-pCVTZ basis set adequately reproduce the CCSD(T) values obtained with the same basis set. The largest values of parameters, thus most promising from the experimental point of view, were obtained for the fluorine nuclei in 1,3-difluorocyclopropene and 1,3-diphenyl-2-fluoro-3-trifluoromethylcyclopropene.

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DOI [BibTex]

DOI [BibTex]


Dynamic Inclusion Complexes of Metal Nanoparticles Inside Nanocups
Dynamic Inclusion Complexes of Metal Nanoparticles Inside Nanocups

Alarcon-Correa, M., Lee, T. C., Fischer, P.

Angew. Chem. Int. Ed., 54(23):6730-6734, May 2015, Featured cover article. (article)

Abstract
Host-guest inclusion complexes are abundant in molecular systems and of fundamental importance in living organisms. Realizing a colloidal analogue of a molecular dynamic inclusion complex is challenging because inorganic nanoparticles (NPs) with a well-defined cavity and portal are difficult to synthesize in high yield and with good structural fidelity. Herein, a generic strategy towards the fabrication of dynamic 1: 1 inclusion complexes of metal nanoparticles inside oxide nanocups with high yield (> 70%) and regiospecificity (> 90%) by means of a reactive double Janus nanoparticle intermediate is reported. Experimental evidence confirms that the inclusion complexes are formed by a kinetically controlled mechanism involving a delicate interplay between bipolar galvanic corrosion and alloying-dealloying oxidation. Release of the NP guest from the nanocups can be efficiently triggered by an external stimulus. Featured cover article.

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DOI [BibTex]

DOI [BibTex]


Surface roughness-induced speed increase for active Janus micromotors
Surface roughness-induced speed increase for active Janus micromotors

Choudhury, U., Soler, L., Gibbs, J. G., Sanchez, S., Fischer, P.

Chem. Comm., 51(41):8660-8663, April 2015 (article)

Abstract
We demonstrate a simple physical fabrication method to control surface roughness of Janus micromotors and fabricate self-propelled active Janus microparticles with rough catalytic platinum surfaces that show a four-fold increase in their propulsion speed compared to conventional Janus particles coated with a smooth Pt layer.

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DOI [BibTex]

DOI [BibTex]


Multi-view and 3D Deformable Part Models
Multi-view and 3D Deformable Part Models

Pepik, B., Stark, M., Gehler, P., Schiele, B.

Pattern Analysis and Machine Intelligence, 37(11):14, IEEE, March 2015 (article)

Abstract
As objects are inherently 3-dimensional, they have been modeled in 3D in the early days of computer vision. Due to the ambiguities arising from mapping 2D features to 3D models, 3D object representations have been neglected and 2D feature-based models are the predominant paradigm in object detection nowadays. While such models have achieved outstanding bounding box detection performance, they come with limited expressiveness, as they are clearly limited in their capability of reasoning about 3D shape or viewpoints. In this work, we bring the worlds of 3D and 2D object representations closer, by building an object detector which leverages the expressive power of 3D object representations while at the same time can be robustly matched to image evidence. To that end, we gradually extend the successful deformable part model [1] to include viewpoint information and part-level 3D geometry information, resulting in several different models with different level of expressiveness. We end up with a 3D object model, consisting of multiple object parts represented in 3D and a continuous appearance model. We experimentally verify that our models, while providing richer object hypotheses than the 2D object models, provide consistently better joint object localization and viewpoint estimation than the state-of-the-art multi-view and 3D object detectors on various benchmarks (KITTI [2], 3D object classes [3], Pascal3D+ [4], Pascal VOC 2007 [5], EPFL multi-view cars [6]).

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DOI Project Page [BibTex]

DOI Project Page [BibTex]


Active colloidal microdrills
Active colloidal microdrills

Gibbs, J. G., Fischer, P.

Chem. Comm., 51(20):4192-4195, Febuary 2015 (article)

Abstract
We demonstrate a chemically driven, autonomous catalytic microdrill. An asymmetric distribution of catalyst causes the helical swimmer to twist while it undergoes directed propulsion. A driving torque and hydrodynamic coupling between translation and rotation at low Reynolds number leads to drill-like swimming behaviour.

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DOI [BibTex]

DOI [BibTex]


{Spike train SIMilarity Space} ({SSIMS}): A framework for single neuron and ensemble data analysis
Spike train SIMilarity Space (SSIMS): A framework for single neuron and ensemble data analysis

Vargas-Irwin, C. E., Brandman, D. M., Zimmermann, J. B., Donoghue, J. P., Black, M. J.

Neural Computation, 27(1):1-31, MIT Press, January 2015 (article)

Abstract
We present a method to evaluate the relative similarity of neural spiking patterns by combining spike train distance metrics with dimensionality reduction. Spike train distance metrics provide an estimate of similarity between activity patterns at multiple temporal resolutions. Vectors of pair-wise distances are used to represent the intrinsic relationships between multiple activity patterns at the level of single units or neuronal ensembles. Dimensionality reduction is then used to project the data into concise representations suitable for clustering analysis as well as exploratory visualization. Algorithm performance and robustness are evaluated using multielectrode ensemble activity data recorded in behaving primates. We demonstrate how Spike train SIMilarity Space (SSIMS) analysis captures the relationship between goal directions for an 8-directional reaching task and successfully segregates grasp types in a 3D grasping task in the absence of kinematic information. The algorithm enables exploration of virtually any type of neural spiking (time series) data, providing similarity-based clustering of neural activity states with minimal assumptions about potential information encoding models.

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pdf: publisher site pdf: author's proof DOI Project Page [BibTex]

pdf: publisher site pdf: author's proof DOI Project Page [BibTex]


Metric Regression Forests for Correspondence Estimation
Metric Regression Forests for Correspondence Estimation

Pons-Moll, G., Taylor, J., Shotton, J., Hertzmann, A., Fitzgibbon, A.

International Journal of Computer Vision, pages: 1-13, 2015 (article)

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springer PDF Project Page [BibTex]

springer PDF Project Page [BibTex]


Selectable Nanopattern Arrays for Nanolithographic Imprint and Etch-Mask Applications
Selectable Nanopattern Arrays for Nanolithographic Imprint and Etch-Mask Applications

Jeong, H. H., Mark, A. G., Lee, T., Son, K., Chen, W., Alarcon-Correa, M., Kim, I., Schütz, G., Fischer, P.

Adv. Science, 2(7):1500016, 2015, Featured cover article. (article)

Abstract
A parallel nanolithographic patterning method is presented that can be used to obtain arrays of multifunctional nanoparticles. These patterns can simply be converted into a variety of secondary nanopatterns that are useful for nanolithographic imprint, plasmonic, and etch-mask applications.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


{MoSh}: Motion and Shape Capture from Sparse Markers
MoSh: Motion and Shape Capture from Sparse Markers

Loper, M. M., Mahmood, N., Black, M. J.

ACM Transactions on Graphics, (Proc. SIGGRAPH Asia), 33(6):220:1-220:13, ACM, New York, NY, USA, November 2014 (article)

Abstract
Marker-based motion capture (mocap) is widely criticized as producing lifeless animations. We argue that important information about body surface motion is present in standard marker sets but is lost in extracting a skeleton. We demonstrate a new approach called MoSh (Motion and Shape capture), that automatically extracts this detail from mocap data. MoSh estimates body shape and pose together using sparse marker data by exploiting a parametric model of the human body. In contrast to previous work, MoSh solves for the marker locations relative to the body and estimates accurate body shape directly from the markers without the use of 3D scans; this effectively turns a mocap system into an approximate body scanner. MoSh is able to capture soft tissue motions directly from markers by allowing body shape to vary over time. We evaluate the effect of different marker sets on pose and shape accuracy and propose a new sparse marker set for capturing soft-tissue motion. We illustrate MoSh by recovering body shape, pose, and soft-tissue motion from archival mocap data and using this to produce animations with subtlety and realism. We also show soft-tissue motion retargeting to new characters and show how to magnify the 3D deformations of soft tissue to create animations with appealing exaggerations.

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pdf video data pdf from publisher link (url) DOI Project Page Project Page Project Page [BibTex]

pdf video data pdf from publisher link (url) DOI Project Page Project Page Project Page [BibTex]


Can I recognize my body’s weight? The influence of shape and texture on the perception of self
Can I recognize my body’s weight? The influence of shape and texture on the perception of self

Piryankova, I., Stefanucci, J., Romero, J., de la Rosa, S., Black, M., Mohler, B.

ACM Transactions on Applied Perception for the Symposium on Applied Perception, 11(3):13:1-13:18, September 2014 (article)

Abstract
The goal of this research was to investigate women’s sensitivity to changes in their perceived weight by altering the body mass index (BMI) of the participants’ personalized avatars displayed on a large-screen immersive display. We created the personalized avatars with a full-body 3D scanner that records both the participants’ body geometry and texture. We altered the weight of the personalized avatars to produce changes in BMI while keeping height, arm length and inseam fixed and exploited the correlation between body geometry and anthropometric measurements encapsulated in a statistical body shape model created from thousands of body scans. In a 2x2 psychophysical experiment, we investigated the relative importance of visual cues, namely shape (own shape vs. an average female body shape with equivalent height and BMI to the participant) and texture (own photo-realistic texture or checkerboard pattern texture) on the ability to accurately perceive own current body weight (by asking them ‘Is the avatar the same weight as you?’). Our results indicate that shape (where height and BMI are fixed) had little effect on the perception of body weight. Interestingly, the participants perceived their body weight veridically when they saw their own photo-realistic texture and significantly underestimated their body weight when the avatar had a checkerboard patterned texture. The range that the participants accepted as their own current weight was approximately a 0.83 to −6.05 BMI% change tolerance range around their perceived weight. Both the shape and the texture had an effect on the reported similarity of the body parts and the whole avatar to the participant’s body. This work has implications for new measures for patients with body image disorders, as well as researchers interested in creating personalized avatars for games, training applications or virtual reality.

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pdf DOI Project Page Project Page [BibTex]

pdf DOI Project Page Project Page [BibTex]


Breathing Life into Shape: Capturing, Modeling and Animating {3D} Human Breathing
Breathing Life into Shape: Capturing, Modeling and Animating 3D Human Breathing

Tsoli, A., Mahmood, N., Black, M. J.

ACM Transactions on Graphics, (Proc. SIGGRAPH), 33(4):52:1-52:11, ACM, New York, NY, July 2014 (article)

Abstract
Modeling how the human body deforms during breathing is important for the realistic animation of lifelike 3D avatars. We learn a model of body shape deformations due to breathing for different breathing types and provide simple animation controls to render lifelike breathing regardless of body shape. We capture and align high-resolution 3D scans of 58 human subjects. We compute deviations from each subject’s mean shape during breathing, and study the statistics of such shape changes for different genders, body shapes, and breathing types. We use the volume of the registered scans as a proxy for lung volume and learn a novel non-linear model relating volume and breathing type to 3D shape deformations and pose changes. We then augment a SCAPE body model so that body shape is determined by identity, pose, and the parameters of the breathing model. These parameters provide an intuitive interface with which animators can synthesize 3D human avatars with realistic breathing motions. We also develop a novel interface for animating breathing using a spirometer, which measures the changes in breathing volume of a “breath actor.”

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pdf video link (url) DOI Project Page Project Page Project Page [BibTex]


Nanopropellers and Their Actuation in Complex Viscoelastic Media
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]


Convertor
Convertor

Fischer, P., Mark, A.

May 2014 (patent)

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[BibTex]

[BibTex]


3D Traffic Scene Understanding from Movable Platforms
3D Traffic Scene Understanding from Movable Platforms

Geiger, A., Lauer, M., Wojek, C., Stiller, C., Urtasun, R.

IEEE Transactions on Pattern Analysis and Machine Intelligence (PAMI), 36(5):1012-1025, published, IEEE, Los Alamitos, CA, May 2014 (article)

Abstract
In this paper, we present a novel probabilistic generative model for multi-object traffic scene understanding from movable platforms which reasons jointly about the 3D scene layout as well as the location and orientation of objects in the scene. In particular, the scene topology, geometry and traffic activities are inferred from short video sequences. Inspired by the impressive driving capabilities of humans, our model does not rely on GPS, lidar or map knowledge. Instead, it takes advantage of a diverse set of visual cues in the form of vehicle tracklets, vanishing points, semantic scene labels, scene flow and occupancy grids. For each of these cues we propose likelihood functions that are integrated into a probabilistic generative model. We learn all model parameters from training data using contrastive divergence. Experiments conducted on videos of 113 representative intersections show that our approach successfully infers the correct layout in a variety of very challenging scenarios. To evaluate the importance of each feature cue, experiments using different feature combinations are conducted. Furthermore, we show how by employing context derived from the proposed method we are able to improve over the state-of-the-art in terms of object detection and object orientation estimation in challenging and cluttered urban environments.

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pdf link (url) [BibTex]

pdf link (url) [BibTex]


Adaptive Offset Correction for Intracortical Brain Computer Interfaces
Adaptive Offset Correction for Intracortical Brain Computer Interfaces

Homer, M. L., Perge, J. A., Black, M. J., Harrison, M. T., Cash, S. S., Hochberg, L. R.

IEEE Transactions on Neural Systems and Rehabilitation Engineering, 22(2):239-248, March 2014 (article)

Abstract
Intracortical brain computer interfaces (iBCIs) decode intended movement from neural activity for the control of external devices such as a robotic arm. Standard approaches include a calibration phase to estimate decoding parameters. During iBCI operation, the statistical properties of the neural activity can depart from those observed during calibration, sometimes hindering a user’s ability to control the iBCI. To address this problem, we adaptively correct the offset terms within a Kalman filter decoder via penalized maximum likelihood estimation. The approach can handle rapid shifts in neural signal behavior (on the order of seconds) and requires no knowledge of the intended movement. The algorithm, called MOCA, was tested using simulated neural activity and evaluated retrospectively using data collected from two people with tetraplegia operating an iBCI. In 19 clinical research test cases, where a nonadaptive Kalman filter yielded relatively high decoding errors, MOCA significantly reduced these errors (10.6 ± 10.1\%; p < 0.05, pairwise t-test). MOCA did not significantly change the error in the remaining 23 cases where a nonadaptive Kalman filter already performed well. These results suggest that MOCA provides more robust decoding than the standard Kalman filter for iBCIs.

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pdf DOI Project Page [BibTex]

pdf DOI Project Page [BibTex]


Circular polarization interferometry: circularly polarized modes of cholesteric liquid crystals
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]


Self-Propelling Nanomotors in the Presence of Strong Brownian Forces
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]


Shape control in wafer-based aperiodic 3D nanostructures
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]


A freely-moving monkey treadmill model
A freely-moving monkey treadmill model

Foster, J., Nuyujukian, P., Freifeld, O., Gao, H., Walker, R., Ryu, S., Meng, T., Murmann, B., Black, M., Shenoy, K.

J. of Neural Engineering, 11(4):046020, 2014 (article)

Abstract
Objective: Motor neuroscience and brain-machine interface (BMI) design is based on examining how the brain controls voluntary movement, typically by recording neural activity and behavior from animal models. Recording technologies used with these animal models have traditionally limited the range of behaviors that can be studied, and thus the generality of science and engineering research. We aim to design a freely-moving animal model using neural and behavioral recording technologies that do not constrain movement. Approach: We have established a freely-moving rhesus monkey model employing technology that transmits neural activity from an intracortical array using a head-mounted device and records behavior through computer vision using markerless motion capture. We demonstrate the excitability and utility of this new monkey model, including the fi rst recordings from motor cortex while rhesus monkeys walk quadrupedally on a treadmill. Main results: Using this monkey model, we show that multi-unit threshold-crossing neural activity encodes the phase of walking and that the average ring rate of the threshold crossings covaries with the speed of individual steps. On a population level, we find that neural state-space trajectories of walking at diff erent speeds have similar rotational dynamics in some dimensions that evolve at the step rate of walking, yet robustly separate by speed in other state-space dimensions. Significance: Freely-moving animal models may allow neuroscientists to examine a wider range of behaviors and can provide a flexible experimental paradigm for examining the neural mechanisms that underlie movement generation across behaviors and environments. For BMIs, freely-moving animal models have the potential to aid prosthetic design by examining how neural encoding changes with posture, environment, and other real-world context changes. Understanding this new realm of behavior in more naturalistic settings is essential for overall progress of basic motor neuroscience and for the successful translation of BMIs to people with paralysis.

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pdf Supplementary DOI Project Page [BibTex]

pdf Supplementary DOI Project Page [BibTex]


Swimming by reciprocal motion at low Reynolds number
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]


Nanohelices by shadow growth
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]


Chiral Nanomagnets
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]


Wireless powering of e-swimmers
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]


Swelling and shrinking behaviour of photoresponsive phosphonium-based ionogel microstructures
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]


A Quantitative Analysis of Current Practices in Optical Flow Estimation and the Principles behind Them
A Quantitative Analysis of Current Practices in Optical Flow Estimation and the Principles behind Them

Sun, D., Roth, S., Black, M. J.

International Journal of Computer Vision (IJCV), 106(2):115-137, 2014 (article)

Abstract
The accuracy of optical flow estimation algorithms has been improving steadily as evidenced by results on the Middlebury optical flow benchmark. The typical formulation, however, has changed little since the work of Horn and Schunck. We attempt to uncover what has made recent advances possible through a thorough analysis of how the objective function, the optimization method, and modern implementation practices influence accuracy. We discover that "classical'' flow formulations perform surprisingly well when combined with modern optimization and implementation techniques. One key implementation detail is the median filtering of intermediate flow fields during optimization. While this improves the robustness of classical methods it actually leads to higher energy solutions, meaning that these methods are not optimizing the original objective function. To understand the principles behind this phenomenon, we derive a new objective function that formalizes the median filtering heuristic. This objective function includes a non-local smoothness term that robustly integrates flow estimates over large spatial neighborhoods. By modifying this new term to include information about flow and image boundaries we develop a method that can better preserve motion details. To take advantage of the trend towards video in wide-screen format, we further introduce an asymmetric pyramid downsampling scheme that enables the estimation of longer range horizontal motions. The methods are evaluated on Middlebury, MPI Sintel, and KITTI datasets using the same parameter settings.

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pdf full text code [BibTex]

pdf full text code [BibTex]

2011


Loose-limbed People: Estimating {3D} Human Pose and Motion Using Non-parametric Belief Propagation
Loose-limbed People: Estimating 3D Human Pose and Motion Using Non-parametric Belief Propagation

Sigal, L., Isard, M., Haussecker, H., Black, M. J.

International Journal of Computer Vision, 98(1):15-48, Springer Netherlands, May 2011 (article)

Abstract
We formulate the problem of 3D human pose estimation and tracking as one of inference in a graphical model. Unlike traditional kinematic tree representations, our model of the body is a collection of loosely-connected body-parts. In particular, we model the body using an undirected graphical model in which nodes correspond to parts and edges to kinematic, penetration, and temporal constraints imposed by the joints and the world. These constraints are encoded using pair-wise statistical distributions, that are learned from motion-capture training data. Human pose and motion estimation is formulated as inference in this graphical model and is solved using Particle Message Passing (PaMPas). PaMPas is a form of non-parametric belief propagation that uses a variation of particle filtering that can be applied over a general graphical model with loops. The loose-limbed model and decentralized graph structure allow us to incorporate information from "bottom-up" visual cues, such as limb and head detectors, into the inference process. These detectors enable automatic initialization and aid recovery from transient tracking failures. We illustrate the method by automatically tracking people in multi-view imagery using a set of calibrated cameras and present quantitative evaluation using the HumanEva dataset.

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pdf publisher's site link (url) Project Page Project Page [BibTex]

2011


pdf publisher's site link (url) Project Page Project Page [BibTex]


Point-and-Click Cursor Control With an Intracortical Neural Interface System by Humans With Tetraplegia
Point-and-Click Cursor Control With an Intracortical Neural Interface System by Humans With Tetraplegia

Kim, S., Simeral, J. D., Hochberg, L. R., Donoghue, J. P., Friehs, G. M., Black, M. J.

IEEE Transactions on Neural Systems and Rehabilitation Engineering, 19(2):193-203, April 2011 (article)

Abstract
We present a point-and-click intracortical neural interface system (NIS) that enables humans with tetraplegia to volitionally move a 2D computer cursor in any desired direction on a computer screen, hold it still and click on the area of interest. This direct brain-computer interface extracts both discrete (click) and continuous (cursor velocity) signals from a single small population of neurons in human motor cortex. A key component of this system is a multi-state probabilistic decoding algorithm that simultaneously decodes neural spiking activity and outputs either a click signal or the velocity of the cursor. The algorithm combines a linear classifier, which determines whether the user is intending to click or move the cursor, with a Kalman filter that translates the neural population activity into cursor velocity. We present a paradigm for training the multi-state decoding algorithm using neural activity observed during imagined actions. Two human participants with tetraplegia (paralysis of the four limbs) performed a closed-loop radial target acquisition task using the point-and-click NIS over multiple sessions. We quantified point-and-click performance using various human-computer interaction measurements for pointing devices. We found that participants were able to control the cursor motion accurately and click on specified targets with a small error rate (< 3% in one participant). This study suggests that signals from a small ensemble of motor cortical neurons (~40) can be used for natural point-and-click 2D cursor control of a personal computer.

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pdf publishers's site pub med link (url) Project Page [BibTex]

pdf publishers's site pub med link (url) Project Page [BibTex]


A Database and Evaluation Methodology for Optical Flow
A Database and Evaluation Methodology for Optical Flow

Baker, S., Scharstein, D., Lewis, J. P., Roth, S., Black, M. J., Szeliski, R.

International Journal of Computer Vision, 92(1):1-31, March 2011 (article)

Abstract
The quantitative evaluation of optical flow algorithms by Barron et al. (1994) led to significant advances in performance. The challenges for optical flow algorithms today go beyond the datasets and evaluation methods proposed in that paper. Instead, they center on problems associated with complex natural scenes, including nonrigid motion, real sensor noise, and motion discontinuities. We propose a new set of benchmarks and evaluation methods for the next generation of optical flow algorithms. To that end, we contribute four types of data to test different aspects of optical flow algorithms: (1) sequences with nonrigid motion where the ground-truth flow is determined by tracking hidden fluorescent texture, (2) realistic synthetic sequences, (3) high frame-rate video used to study interpolation error, and (4) modified stereo sequences of static scenes. In addition to the average angular error used by Barron et al., we compute the absolute flow endpoint error, measures for frame interpolation error, improved statistics, and results at motion discontinuities and in textureless regions. In October 2007, we published the performance of several well-known methods on a preliminary version of our data to establish the current state of the art. We also made the data freely available on the web at http://vision.middlebury.edu/flow/ . Subsequently a number of researchers have uploaded their results to our website and published papers using the data. A significant improvement in performance has already been achieved. In this paper we analyze the results obtained to date and draw a large number of conclusions from them.

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pdf pdf from publisher Middlebury Flow Evaluation Website [BibTex]

pdf pdf from publisher Middlebury Flow Evaluation Website [BibTex]


Quantum-Cascade Laser-Based Vibrational Circular Dichroism
Quantum-Cascade Laser-Based Vibrational Circular Dichroism

Luedeke, S., Pfeifer, M., Fischer, P.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 133(15):5704-5707, 2011 (article)

Abstract
Vibrational circular dichroism (VCD) spectra were recorded with a tunable external-cavity quantum-cascade laser (QCL). In comparison with standard thermal light sources in the IR, QCLs provide orders of magnitude more power and are therefore promising for VCD studies in strongly absorbing solvents. The brightness of this novel light source is demonstrated with VCD and IR absorption measurements of a number of compounds, including proline in water.

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DOI [BibTex]

DOI [BibTex]


Actively coupled cavity ringdown spectroscopy with low-power broadband sources
Actively coupled cavity ringdown spectroscopy with low-power broadband sources

Petermann, C., Fischer, P.

OPTICS EXPRESS, 19(11):10164-10173, 2011 (article)

Abstract
We demonstrate a coupling scheme for cavity enhanced absorption spectroscopy that makes use of an intracavity acousto-optical modulator to actively switch light into (and out of) a resonator. This allows cavity ringdown spectroscopy (CRDS) to be implemented with broadband nonlaser light sources with spectral power densities of less than 30 mu W/nm. Although the acousto-optical element reduces the ultimate detection limit by introducing additional losses, it permits absorptivities to be measured with a high dynamic range, especially in lossy environments. Absorption measurements for the forbidden transition of gaseous oxygen in air at similar to 760nm are presented using a low-coherence cw-superluminescent diode. The same setup was electronically configured to cover absorption losses from 1.8 x 10(-8)cm(-1) to 7.5\% per roundtrip. This could be of interest in process analytical applications. (C) 2011 Optical Society of America

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DOI [BibTex]

DOI [BibTex]


Magnetically actuated propulsion at low Reynolds numbers: towards nanoscale control
Magnetically actuated propulsion at low Reynolds numbers: towards nanoscale control

Fischer, P., Ghosh, A.

NANOSCALE, 3(2):557-563, 2011 (article)

Abstract
Significant progress has been made in the fabrication of micron and sub-micron structures whose motion can be controlled in liquids under ambient conditions. The aim of many of these engineering endeavors is to be able to build and propel an artificial micro-structure that rivals the versatility of biological swimmers of similar size, e. g. motile bacterial cells. Applications for such artificial ``micro-bots'' are envisioned to range from microrheology to targeted drug delivery and microsurgery, and require full motion-control under ambient conditions. In this Mini-Review we discuss the construction, actuation, and operation of several devices that have recently been reported, especially systems that can be controlled by and propelled with homogenous magnetic fields. We describe the fabrication and associated experimental challenges and discuss potential applications.

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Video - Nanospropellers DOI [BibTex]


Weak value amplified optical activity measurements
Weak value amplified optical activity measurements

Pfeifer, M., Fischer, P.

Opt. Express, 19(17):16508-16517, OSA, 2011 (article)

Abstract
We present a new form of optical activity measurement based on a modified weak value amplification scheme. It has recently been shown experimentally that the left- and right-circular polarization components refract with slightly different angles of refraction at a chiral interface causing a linearly polarized light beam to split into two. By introducing a polarization modulation that does not give rise to a change in the optical rotation it is possible to differentiate between the two circular polarization components even after post-selection with a linear polarizer. We show that such a modified weak value amplification measurement permits the sign of the splitting and thus the handedness of the optically active medium to be determined. Angular beam separations of Δθ ∼ 1 nanoradian, which corresponds to a circular birefringence of Δn ∼ 1 × 10−9, could be measured with a relative error of less than 1%.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


Neural control of cursor trajectory and click by a human with tetraplegia 1000 days after implant of an intracortical microelectrode array
Neural control of cursor trajectory and click by a human with tetraplegia 1000 days after implant of an intracortical microelectrode array

(J. Neural Engineering Highlights of 2011 Collection. JNE top 10 cited papers of 2010-2011.)

Simeral, J. D., Kim, S., Black, M. J., Donoghue, J. P., Hochberg, L. R.

J. of Neural Engineering, 8(2):025027, 2011 (article)

Abstract
The ongoing pilot clinical trial of the BrainGate neural interface system aims in part to assess the feasibility of using neural activity obtained from a small-scale, chronically implanted, intracortical microelectrode array to provide control signals for a neural prosthesis system. Critical questions include how long implanted microelectrodes will record useful neural signals, how reliably those signals can be acquired and decoded, and how effectively they can be used to control various assistive technologies such as computers and robotic assistive devices, or to enable functional electrical stimulation of paralyzed muscles. Here we examined these questions by assessing neural cursor control and BrainGate system characteristics on five consecutive days 1000 days after implant of a 4 × 4 mm array of 100 microelectrodes in the motor cortex of a human with longstanding tetraplegia subsequent to a brainstem stroke. On each of five prospectively-selected days we performed time-amplitude sorting of neuronal spiking activity, trained a population-based Kalman velocity decoding filter combined with a linear discriminant click state classifier, and then assessed closed-loop point-and-click cursor control. The participant performed both an eight-target center-out task and a random target Fitts metric task which was adapted from a human-computer interaction ISO standard used to quantify performance of computer input devices. The neural interface system was further characterized by daily measurement of electrode impedances, unit waveforms and local field potentials. Across the five days, spiking signals were obtained from 41 of 96 electrodes and were successfully decoded to provide neural cursor point-and-click control with a mean task performance of 91.3% ± 0.1% (mean ± s.d.) correct target acquisition. Results across five consecutive days demonstrate that a neural interface system based on an intracortical microelectrode array can provide repeatable, accurate point-and-click control of a computer interface to an individual with tetraplegia 1000 days after implantation of this sensor.

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pdf pdf from publisher link (url) Project Page [BibTex]

2010


Magnetic Nanostructured Propellers
Magnetic Nanostructured Propellers

Fischer, P., Ghosh, A.

July 2010 (patent)

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[BibTex]

2010


[BibTex]


Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field
Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field

Fischer, P., Salam, A.

MOLECULAR PHYSICS, 108(14):1857-1868, 2010 (article)

Abstract
Coherent second-order nonlinear optical processes are symmetry forbidden in centrosymmetric environments in the electric-dipole approximation. In liquids that contain chiral molecules, however, and which therefore lack mirror image symmetry, coherent sum-frequency generation is possible, whereas second-harmonic generation remains forbidden. Here we apply the theory of molecular quantum electrodynamics to the calculation of the matrix element, transition rate, and integrated signal intensity for sum-frequency and second-harmonic generation taking place in a chiral liquid in the presence and absence of a static electric field, to examine which coherent and incoherent processes exist in the electric-dipole approximation in liquids. Third- and fourth-order time-dependent perturbation theory is employed in combination with single-sided Feynman diagrams to evaluate two contributions arising from static field-free and field-induced processes. It is found that, in addition to the coherent term, an incoherent process exists for sum-frequency generation in liquids. Surprisingly, in the case of dc-field-induced second-harmonic generation, the incoherent contribution is found to always vanish for isotropic chiral liquids even though hyper-Rayleigh second-harmonic generation and electric-field-induced second-harmonic generation are both independently symmetry allowed in any liquid.

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DOI [BibTex]


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]

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]