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2019


Soft-magnetic coatings as possible sensors for magnetic imaging of superconductors
Soft-magnetic coatings as possible sensors for magnetic imaging of superconductors

Ionescu, A., Simmendinger, J., Bihler, M., Miksch, C., Fischer, P., Soltan, S., Schütz, G., Albrecht, J.

Supercond. Sci. and Tech., 33, pages: 015002, IOP, December 2019 (article)

Abstract
Magnetic imaging of superconductors typically requires a soft-magnetic material placed on top of the superconductor to probe local magnetic fields. For reasonable results the influence of the magnet onto the superconductor has to be small. Thin YBCO films with soft-magnetic coatings are investigated using SQUID magnetometry. Detailed measurements of the magnetic moment as a function of temperature, magnetic field and time have been performed for different heterostructures. It is found that the modification of the superconducting transport in these heterostructures strongly depends on the magnetic and structural properties of the soft-magnetic material. This effect is especially pronounced for an inhomogeneous coating consisting of ferromagnetic nanoparticles.

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link (url) DOI [BibTex]

2019


link (url) DOI [BibTex]


HPLC of monolayer-protected Gold clusters with baseline separation
HPLC of monolayer-protected Gold clusters with baseline separation

Knoppe, S., Vogt, P.

Analytical Chemistry, 91, pages: 1603, December 2019 (article)

Abstract
The properties of ultrasmall metal nanoparticles (ca. 10–200 metal atoms), or monolayer-protected metal clusters (MPCs), drastically depend on their atomic structure. For systematic characterization and application, assessment of their purity is of high importance. Currently, the gold standard for purity control of MPCs is mass spectrometry (MS). Mass spectrometry, however, cannot always detect small impurities; MS of certain clusters, for example, ESI-TOF of Au40(SR)24, is not successful at all. We here present a simple reversed-phase HPLC method for purity control of a series of small alkanethiolate-protected gold clusters. The method allows the detection of small impurities with high sensitivity. Linear correlation between alkyl chain length of Au25(SC_n H_(2n+1))18 clusters (n = 6, 8, 10, 12) and their retention time was noticed.

pf

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Acoustic hologram enhanced phased arrays for ultrasonic particle manipulation
Acoustic hologram enhanced phased arrays for ultrasonic particle manipulation

Cox, L., Melde, K., Croxford, A., Fischer, P., Drinkwater, B.

Phys. Rev. Applied, 12, pages: 064055, November 2019 (article)

Abstract
The ability to shape ultrasound fields is important for particle manipulation, medical therapeutics and imaging applications. If the amplitude and/or phase is spatially varied across the wavefront then it is possible to project ‘acoustic images’. When attempting to form an arbitrary desired static sound field, acoustic holograms are superior to phased arrays due to their significantly higher phase fidelity. However, they lack the dynamic flexibility of phased arrays. Here, we demonstrate how to combine the high-fidelity advantages of acoustic holograms with the dynamic control of phased arrays in the ultrasonic frequency range. Holograms are used with a 64-element phased array, driven with continuous excitation. Moving the position of the projected hologram via phase delays which steer the output beam is demonstrated experimentally. This allows the creation of a much more tightly focused point than with the phased array alone, whilst still being reconfigurable. It also allows the complex movement at a water-air interface of a “phase surfer” along a phase track or the manipulation of a more arbitrarily shaped particle via amplitude traps. Furthermore, a particle manipulation device with two emitters and a single split hologram is demonstrated that allows the positioning of a “phase surfer” along a 1D axis. This paper opens the door for new applications with complex manipulation of ultrasound whilst minimising the complexity and cost of the apparatus.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


A Helical Microrobot with an Optimized Propeller-Shape for Propulsion in Viscoelastic Biological Media
A Helical Microrobot with an Optimized Propeller-Shape for Propulsion in Viscoelastic Biological Media

Li., D., Jeong, M., Oren, E., Yu, T., Qiu, T.

Robotics, 8, pages: 87, MDPI, October 2019 (article)

Abstract
One major challenge for microrobots is to penetrate and effectively move through viscoelastic biological tissues. Most existing microrobots can only propel in viscous liquids. Recent advances demonstrate that sub-micron robots can actively penetrate nanoporous biological tissue, such as the vitreous of the eye. However, it is still difficult to propel a micron-sized device through dense biological tissue. Here, we report that a special twisted helical shape together with a high aspect ratio in cross-section permit a microrobot with a diameter of hundreds-of-micrometers to move through mouse liver tissue. The helical microrobot is driven by a rotating magnetic field and localized by ultrasound imaging inside the tissue. The twisted ribbon is made of molybdenum and a sharp tip is chemically etched to generate a higher pressure at the edge of the propeller to break the biopolymeric network of the dense tissue.

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link (url) DOI [BibTex]


Acoustic Holographic Cell Patterning in a Biocompatible Hydrogel
Acoustic Holographic Cell Patterning in a Biocompatible Hydrogel

Ma, Z., Holle, A., Melde, K., Qiu, T., Poeppel, K., Kadiri, V., Fischer, P.

Adv. Mat., 32(1904181), October 2019 (article)

Abstract
Acoustophoresis is promising as a rapid, biocompatible, non-contact cell manipulation method, where cells are arranged along the nodes or antinodes of the acoustic field. Typically, the acoustic field is formed in a resonator, which results in highly symmetric regular patterns. However, arbitrary, non-symmetrically shaped cell assemblies are necessary to obtain the irregular cellular arrangements found in biological tissues. We show that arbitrarily shaped cell patterns can be obtained from the complex acoustic field distribution defined by an acoustic hologram. Attenuation of the sound field induces localized acoustic streaming and the resultant convection flow gently delivers the suspended cells to the image plane where they form the designed pattern. We show that the process can be implemented in a biocompatible collagen solution, which can then undergo gelation to immobilize the cell pattern inside the viscoelastic matrix. The patterned cells exhibit F-actin-based protrusions, which indicates that the cells grow and thrive within the matrix. Cell viability assays and brightfield imaging after one week confirm cell survival and that the patterns persist. Acoustophoretic cell manipulation by holographic fields thus holds promise for non-contact, long-range, long-term cellular pattern formation, with a wide variety of potential applications in tissue engineering and mechanobiology.

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link (url) DOI [BibTex]


Arrays of plasmonic nanoparticle dimers with defined nanogap spacers
Arrays of plasmonic nanoparticle dimers with defined nanogap spacers

Jeong, H., Adams, M. C., Guenther, J., Alarcon-Correa, M., Kim, I., Choi, E., Miksch, C., Mark, A. F. M., Mark, A. G., Fischer, P.

ACS Nano, 13, pages: 11453-11459, September 2019 (article)

Abstract
Plasmonic molecules are building blocks of metallic nanostructures that give rise to intriguing optical phenomena with similarities to those seen in molecular systems. The ability to design plasmonic hybrid structures and molecules with nanometric resolution would enable applications in optical metamaterials and sensing that presently cannot be demonstrated, because of a lack of suitable fabrication methods allowing the structural control of the plasmonic atoms on a large scale. Here we demonstrate a wafer-scale “lithography-free” parallel fabrication scheme to realize nanogap plasmonic meta-molecules with precise control over their size, shape, material, and orientation. We demonstrate how we can tune the corresponding coupled resonances through the entire visible spectrum. Our fabrication method, based on glancing angle physical vapor deposition with gradient shadowing, permits critical parameters to be varied across the wafer and thus is ideally suited to screen potential structures. We obtain billions of aligned dimer structures with controlled variation of the spectral properties across the wafer. We spectroscopically map the plasmonic resonances of gold dimer structures and show that they not only are in good agreement with numerically modeled spectra, but also remain functional, at least for a year, in ambient conditions.

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link (url) DOI [BibTex]


Genetically modified M13 bacteriophage nanonets for enzyme catalysis and recovery
Genetically modified M13 bacteriophage nanonets for enzyme catalysis and recovery

Kadiri, V. M., Alarcon-Correa, M., Guenther, J. P., Ruppert, J., Bill, J., Rothenstein, D., Fischer, P.

Catalysts, 9, pages: 723, August 2019 (article)

Abstract
Enzyme-based biocatalysis exhibits multiple advantages over inorganic catalysts, including the biocompatibility and the unchallenged specificity of enzymes towards their substrate. The recovery and repeated use of enzymes is essential for any realistic application in biotechnology, but is not easily achieved with current strategies. For this purpose, enzymes are often immobilized on inorganic scaffolds, which could entail a reduction of the enzymes’ activity. Here, we show that immobilization to a nano-scaled biological scaffold, a nanonetwork of end-to-end cross-linked M13 bacteriophages, ensures high enzymatic activity and at the same time allows for the simple recovery of the enzymes. The bacteriophages have been genetically engineered to express AviTags at their ends, which permit biotinylation and their specific end-to-end self-assembly while allowing space on the major coat protein for enzyme coupling. We demonstrate that the phages form nanonetwork structures and that these so-called nanonets remain highly active even after re-using the nanonets multiple times in a flow-through reactor.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


Light-controlled micromotors and soft microrobots
Light-controlled micromotors and soft microrobots

Palagi, S., Singh, D. P., Fischer, P.

Adv. Opt. Mat., 7, pages: 1900370, August 2019 (article)

Abstract
Mobile microscale devices and microrobots can be powered by catalytic reactions (chemical micromotors) or by external fields. This report is focused on the role of light as a versatile means for wirelessly powering and controlling such microdevices. Recent advances in the development of autonomous micromotors are discussed, where light permits their actuation with unprecedented control and thereby enables advances in the field of active matter. In addition, structuring the light field is a new means to drive soft microrobots that are based on (photo‐) responsive polymers. The behavior of the two main classes of thermo‐ and photoresponsive polymers adopted in microrobotics (poly(N‐isopropylacrylamide) and liquid‐crystal elastomers) is analyzed, and recent applications are reported. The advantages and limitations of controlling micromotors and microrobots by light are reviewed, and some of the remaining challenges in the development of novel photo‐active materials for micromotors and microrobots are discussed.

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link (url) DOI [BibTex]


Series Elastic Behavior of Biarticular Muscle-Tendon Structure in a Robotic Leg
Series Elastic Behavior of Biarticular Muscle-Tendon Structure in a Robotic Leg

Ruppert, F., Badri-Spröwitz, A.

Frontiers in Neurorobotics, 64, pages: 13, 13, August 2019 (article)

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Frontiers YouTube link (url) DOI [BibTex]

Frontiers YouTube link (url) DOI [BibTex]


Beyond Basins of Attraction: Quantifying Robustness of Natural Dynamics
Beyond Basins of Attraction: Quantifying Robustness of Natural Dynamics

Steve Heim, , Spröwitz, A.

IEEE Transactions on Robotics (T-RO) , 35(4), pages: 939-952, August 2019 (article)

Abstract
Properly designing a system to exhibit favorable natural dynamics can greatly simplify designing or learning the control policy. However, it is still unclear what constitutes favorable natural dynamics and how to quantify its effect. Most studies of simple walking and running models have focused on the basins of attraction of passive limit cycles and the notion of self-stability. We instead emphasize the importance of stepping beyond basins of attraction. In this paper, we show an approach based on viability theory to quantify robust sets in state-action space. These sets are valid for the family of all robust control policies, which allows us to quantify the robustness inherent to the natural dynamics before designing the control policy or specifying a control objective. We illustrate our formulation using spring-mass models, simple low-dimensional models of running systems. We then show an example application by optimizing robustness of a simulated planar monoped, using a gradient-free optimization scheme. Both case studies result in a nonlinear effective stiffness providing more robustness.

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arXiv preprint arXiv:1806.08081 T-RO link (url) DOI Project Page [BibTex]

arXiv preprint arXiv:1806.08081 T-RO link (url) DOI Project Page [BibTex]


Superior Magnetic Performance in FePt L1_0 Nanomaterials
Superior Magnetic Performance in FePt L1_0 Nanomaterials

Son, K., Ryu, G. H., Jeong, H., Fink, L., Merz, M., Nagel, P., Schuppler, S., Richter, G., Goering, E., Schütz, G.

Small, 15(1902353), July 2019 (article)

Abstract
The discovery of the high maximum energy product of 59 MGOe for NdFeB magnets is a breakthrough in the development of permanent magnets with a tremendous impact in many fields of technology. This value is still the world record, for 40 years. This work reports on a reliable and robust route to realize nearly perfectly ordered L1_0-phase FePt nanoparticles, leading to an unprecedented energy product of 80 MGOe at room temperature. Furthermore, with a 3 nm Au coverage, the magnetic polarization of these nanomagnets can be enhanced by 25% exceeding 1.8 T. This exceptional magnetization and anisotropy is confirmed by using multiple imaging and spectroscopic methods, which reveal highly consistent results. Due to the unprecedented huge energy product, this material can be envisaged as a new advanced basic magnetic component in modern micro and nanosized devices.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


The acoustic hologram and particle manipulation with structured acoustic fields
The acoustic hologram and particle manipulation with structured acoustic fields

Melde, K.

Karlsruher Institut für Technologie (KIT), May 2019 (phdthesis)

Abstract
This thesis presents holograms as a novel approach to create arbitrary ultrasound fields. It is shown how any wavefront can simply be encoded in the thickness profile of a phase plate. Contemporary 3D-printers enable fabrication of structured surfaces with feature sizes corresponding to wavelengths of ultrasound up to 7.5 MHz in water—covering the majority of medical and industrial applications. The whole workflow for designing and creating acoustic holograms has been developed and is presented in this thesis. To reconstruct the encoded fields a single transducer element is sufficient. Arbitrary fields are demonstrated in transmission and reflection configurations in water and air and validated by extensive hydrophone scans. To complement these time-consuming measurements a new approach, based on thermography, is presented, which enables volumetric sound field scans in just a few seconds. Several original experiments demonstrate the advantages of using acoustic holograms for particle manipulation. Most notably, directed parallel assembly of microparticles in the shape of a projected acoustic image has been shown and extended to a fabrication method by fusing the particles in a polymerization reaction. Further, seemingly dynamic propulsion from a static hologram is demonstrated by controlling the phase gradient along a projected track. The necessary complexity to create ultrasound fields with set amplitude and phase distributions is easily managed using acoustic holograms. The acoustic hologram is a simple and cost-effective tool for shaping ultrasound fields with high-fidelity. It is expected to have an impact in many applications where ultrasound is employed.

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link (url) DOI [BibTex]


Recent advances in gold nanoparticles forbiomedical applications: from hybrid structuresto multi-functionality
Recent advances in gold nanoparticles forbiomedical applications: from hybrid structuresto multi-functionality

Jeong, H., Choi, E., Ellis, E., Lee, T.

J. of Mat. Chem. B, 7, pages: 3480, May 2019 (article)

Abstract
Gold nanoparticles (Au NPs) are arguably the most versatile nanomaterials reported to date. Recentadvances in nanofabrication and chemical synthesis have expanded the scope of Au NPs from classicalhomogeneous nanospheres to a wide range of hybrid nanostructures with programmable size, shapeand composition. Novel physiochemical properties can be achievedviadesign and engineering of thehybrid nanostructures. In this review we discuss the recent progress in the development of complexhybrid Au NPs and propose a classification framework based on three fundamental structuraldimensions (length scale, complexity and symmetry) to aid categorising, comparing and designingvarious types of Au NPs. Their novel functions and potential for biomedical applications will also bediscussed, featuring point-of-care diagnostics by advanced optical spectroscopy and assays, as well asminimally invasive surgeries and targeted drug delivery using multifunctional nano-robot

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link (url) DOI [BibTex]


Self-Assembled Phage-Based Colloids for High Localized Enzymatic Activity
Self-Assembled Phage-Based Colloids for High Localized Enzymatic Activity

Alarcon-Correa, M., Guenther, J., Troll, J., Kadiri, V. M., Bill, J., Fischer, P., Rothenstein, D.

ACS Nano, 13, pages: 5810–5815, March 2019 (article)

Abstract
Catalytically active colloids are model systems for chemical motors and active matter. It is desirable to replace the inorganic catalysts and the toxic fuels that are often used, with biocompatible enzymatic reactions. However, compared to inorganic catalysts, enzyme-coated colloids tend to exhibit less activity. Here, we show that the self-assembly of genetically engineered M13 bacteriophages that bind enzymes to magnetic beads ensures high and localized enzymatic activity. These phage-decorated colloids provide a proteinaceous environment for directed enzyme immobilization. The magnetic properties of the colloidal carrier particle permit repeated enzyme recovery from a reaction solution, while the enzymatic activity is retained. Moreover, localizing the phage-based construct with a magnetic field in a microcontainer allows the enzyme-phage-colloids to function as an enzymatic micropump, where the enzymatic reaction generates a fluid flow. This system shows the fastest fluid flow reported to date by a biocompatible enzymatic micropump. In addition, it is functional in complex media including blood where the enzyme driven micropump can be powered at the physiological blood-urea concentration.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


Absolute diffusion measurements of active enzyme solutions by NMR
Absolute diffusion measurements of active enzyme solutions by NMR

Guenther, J., Majer, G., Fischer, P.

J. Chem. Phys., 150(124201), March 2019 (article)

Abstract
The diffusion of enzymes is of fundamental importance for many biochemical processes. Enhanced or directed enzyme diffusion can alter the accessibility of substrates and the organization of enzymes within cells. Several studies based on fluorescence correlation spectroscopy (FCS) report enhanced diffusion of enzymes upon interaction with their substrate or inhibitor. In this context, major importance is given to the enzyme fructose-bisphosphate aldolase, for which enhanced diffusion has been reported even though the catalysed reaction is endothermic. Additionally, enhanced diffusion of tracer particles surrounding the active aldolase enzymes has been reported. These studies suggest that active enzymes can act as chemical motors that self-propel and give rise to enhanced diffusion. However, fluorescence studies of enzymes can, despite several advantages, suffer from artefacts. Here we show that the absolute diffusion coefficients of active enzyme solutions can be determined with Pulsed Field Gradient Nuclear Magnetic Resonance (PFG-NMR). The advantage of PFG-NMR is that the motion of the molecule of interest is directly observed in its native state without the need for any labelling. Further, PFG-NMR is model-free and thus yields absolute diffusion constants. Our PFG-NMR experiments of solutions containing active fructose-bisphosphate aldolase from rabbit muscle do not show any diffusion enhancement for the active enzymes nor the surrounding molecules. Additionally, we do not observe any diffusion enhancement of aldolase in the presence of its inhibitor pyrophosphate.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


Chemical Nanomotors at the Gram Scale Form a Dense Active Optorheological Medium
Chemical Nanomotors at the Gram Scale Form a Dense Active Optorheological Medium

Choudhury, U., Singh, D. P., Qiu, T., Fischer, P.

Adv. Mat., 31(1807382), Febuary 2019 (article)

Abstract
The rheological properties of a colloidal suspension are a function of the concentration of the colloids and their interactions. While suspensions of passive colloids are well studied and have been shown to form crystals, gels, and glasses, examples of energy‐consuming “active” colloidal suspensions are still largely unexplored. Active suspensions of biological matter, such as motile bacteria or dense mixtures of active actin–motor–protein mixtures have, respectively, reveals superfluid‐like and gel‐like states. Attractive inanimate systems for active matter are chemically self‐propelled particles. It has so far been challenging to use these swimming particles at high enough densities to affect the bulk material properties of the suspension. Here, it is shown that light‐triggered asymmetric titanium dioxide that self‐propel, can be obtained in large quantities, and self‐organize to make a gram‐scale active medium. The suspension shows an activity‐dependent tenfold reversible change in its bulk viscosity.

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link (url) DOI [BibTex]


First Observation of Optical Activity in Hyper-Rayleigh Scattering
First Observation of Optical Activity in Hyper-Rayleigh Scattering

Collins, J., Rusimova, K., Hooper, D., Jeong, H. H., Ohnoutek, L., Pradaux-Caggiano, F., Verbiest, T., Carbery, D., Fischer, P., Valev, V.

Phys. Rev. X, 9(011024), January 2019 (article)

Abstract
Chiral nano- or metamaterials and surfaces enable striking photonic properties, such as negative refractive index and superchiral light, driving promising applications in novel optical components, nanorobotics, and enhanced chiral molecular interactions with light. In characterizing chirality, although nonlinear chiroptical techniques are typically much more sensitive than their linear optical counterparts, separating true chirality from anisotropy is a major challenge. Here, we report the first observation of optical activity in second-harmonic hyper-Rayleigh scattering (HRS). We demonstrate the effect in a 3D isotropic suspension of Ag nanohelices in water. The effect is 5 orders of magnitude stronger than linear optical activity and is well pronounced above the multiphoton luminescence background. Because of its sensitivity, isotropic environment, and straightforward experimental geometry, HRS optical activity constitutes a fundamental experimental breakthrough in chiral photonics for media including nanomaterials, metamaterials, and chemical molecules.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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On the positivity and magnitudes of Bayesian quadrature weights

Karvonen, T., Kanagawa, M., Särkä, S.

Statistics and Computing, 29, pages: 1317-1333, 2019 (article)

pn

DOI [BibTex]

DOI [BibTex]


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Probabilistic solutions to ordinary differential equations as nonlinear Bayesian filtering: a new perspective

Tronarp, F., Kersting, H., Särkkä, S. H. P.

Statistics and Computing, 29(6):1297-1315, 2019 (article)

ei pn

DOI [BibTex]

DOI [BibTex]


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Co-Contraction facilitates Body Stiffness Modulation during Swimming with Sensory Feedback in a Soft Biorobotic Physical Model

Jusufi, A., Vogt, D., Wood, R. J.

Integrative and Comparative Biology, 59(Supplement 1):E116-E116, Society of Integrative and Comparative Biology, McLean, VA, 2019 (article)

bio

DOI [BibTex]

DOI [BibTex]


Dynamics of self-propelled colloids and their application as active matter
Dynamics of self-propelled colloids and their application as active matter

Choudhury, U.

University of Groningen, Zernike Institute for Advanced Materials, 2019 (phdthesis)

Abstract
In this thesis, the behavior of active particles spanning from single particle dynamics to collective behavior of many particles is explored. Active colloids are out-of equilibrium systems that have been studied extensively over the past 15 years. This thesis addresses several phenomena that arise in the field of active colloids.

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link (url) [BibTex]

link (url) [BibTex]


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Dense connectomic reconstruction in layer 4 of the somatosensory cortex

Motta, A., Berning, M., Boergens, K. M., Staffler, B., Beining, M., Loomba, S., Hennig, P., Wissler, H., Helmstaedter, M.

Science, 366(6469):eaay3134, American Association for the Advancement of Science, 2019 (article)

ei pn

DOI [BibTex]

DOI [BibTex]


Probabilistic Linear Solvers: A Unifying View
Probabilistic Linear Solvers: A Unifying View

Bartels, S., Cockayne, J., Ipsen, I., Hennig, P.

Statistics and Computing, 29(6):1249-1263, 2019 (article)

pn

link (url) DOI [BibTex]

link (url) DOI [BibTex]

2015


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]

2015


link (url) DOI [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]


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]


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]


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Probabilistic Interpretation of Linear Solvers

Hennig, P.

SIAM Journal on Optimization, 25(1):234-260, 2015 (article)

ei pn

Web PDF link (url) DOI [BibTex]

Web PDF link (url) DOI [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]


Exciting Engineered Passive Dynamics in a Bipedal Robot
Exciting Engineered Passive Dynamics in a Bipedal Robot

Renjewski, D., Spröwitz, A., Peekema, A., Jones, M., Hurst, J.

{IEEE Transactions on Robotics and Automation}, 31(5):1244-1251, IEEE, New York, NY, 2015 (article)

Abstract
A common approach in designing legged robots is to build fully actuated machines and control the machine dynamics entirely in soft- ware, carefully avoiding impacts and expending a lot of energy. However, these machines are outperformed by their human and animal counterparts. Animals achieve their impressive agility, efficiency, and robustness through a close integration of passive dynamics, implemented through mechanical components, and neural control. Robots can benefit from this same integrated approach, but a strong theoretical framework is required to design the passive dynamics of a machine and exploit them for control. For this framework, we use a bipedal spring–mass model, which has been shown to approximate the dynamics of human locomotion. This paper reports the first implementation of spring–mass walking on a bipedal robot. We present the use of template dynamics as a control objective exploiting the engineered passive spring–mass dynamics of the ATRIAS robot. The results highlight the benefits of combining passive dynamics with dynamics-based control and open up a library of spring–mass model-based control strategies for dynamic gait control of robots.

dlg

link (url) DOI Project Page [BibTex]

link (url) DOI Project Page [BibTex]


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Probabilistic numerics and uncertainty in computations

Hennig, P., Osborne, M. A., Girolami, M.

Proceedings of the Royal Society of London A: Mathematical, Physical and Engineering Sciences, 471(2179), 2015 (article)

Abstract
We deliver a call to arms for probabilistic numerical methods: algorithms for numerical tasks, including linear algebra, integration, optimization and solving differential equations, that return uncertainties in their calculations. Such uncertainties, arising from the loss of precision induced by numerical calculation with limited time or hardware, are important for much contemporary science and industry. Within applications such as climate science and astrophysics, the need to make decisions on the basis of computations with large and complex data have led to a renewed focus on the management of numerical uncertainty. We describe how several seminal classic numerical methods can be interpreted naturally as probabilistic inference. We then show that the probabilistic view suggests new algorithms that can flexibly be adapted to suit application specifics, while delivering improved empirical performance. We provide concrete illustrations of the benefits of probabilistic numeric algorithms on real scientific problems from astrometry and astronomical imaging, while highlighting open problems with these new algorithms. Finally, we describe how probabilistic numerical methods provide a coherent framework for identifying the uncertainty in calculations performed with a combination of numerical algorithms (e.g. both numerical optimizers and differential equation solvers), potentially allowing the diagnosis (and control) of error sources in computations.

ei pn

PDF DOI [BibTex]

PDF DOI [BibTex]

2011


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.

pf

DOI [BibTex]

2011


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

pf

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.

pf

Video - Nanospropellers DOI [BibTex]


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Aerial righting reflexes in flightless animals

Jusufi, A., Zeng, Y., Full, R., Dudley, R.

Integ. Comp. Biol. , 2011 (article)

bio

[BibTex]

[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%.

pf

link (url) DOI [BibTex]

link (url) DOI [BibTex]

2006


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

Ghosh, A., Fischer, P.

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

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

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

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DOI [BibTex]

2006


DOI [BibTex]


Direct chiral discrimination in NMR spectroscopy
Direct chiral discrimination in NMR spectroscopy

Buckingham, A., Fischer, P.

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

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

pf

DOI [BibTex]

DOI [BibTex]


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

Vollmer, F., Fischer, P.

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

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

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DOI [BibTex]


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

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

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

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

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DOI [BibTex]

DOI [BibTex]