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2019


Thumb xl m13 bacteriophages
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, 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]


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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]


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

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

Adv. Mat., (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]


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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]

2017


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Active colloidal propulsion over a crystalline surface

Choudhury, U., Straube, A., Fischer, P., Gibbs, J., Höfling, F.

New Journal of Physics, 19, pages: 125010, December 2017 (article)

Abstract
We study both experimentally and theoretically the dynamics of chemically self-propelled Janus colloids moving atop a two-dimensional crystalline surface. The surface is a hexagonally close-packed monolayer of colloidal particles of the same size as the mobile one. The dynamics of the self-propelled colloid reflects the competition between hindered diffusion due to the periodic surface and enhanced diffusion due to active motion. Which contribution dominates depends on the propulsion strength, which can be systematically tuned by changing the concentration of a chemical fuel. The mean-square displacements obtained from the experiment exhibit enhanced diffusion at long lag times. Our experimental data are consistent with a Langevin model for the effectively two-dimensional translational motion of an active Brownian particle in a periodic potential, combining the confining effects of gravity and the crystalline surface with the free rotational diffusion of the colloid. Approximate analytical predictions are made for the mean-square displacement describing the crossover from free Brownian motion at short times to active diffusion at long times. The results are in semi-quantitative agreement with numerical results of a refined Langevin model that treats translational and rotational degrees of freedom on the same footing.

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link (url) DOI [BibTex]

2017


link (url) DOI [BibTex]


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Wireless Acoustic-Surface Actuators for Miniaturized Endoscopes

Qiu, T., Adams, F., Palagi, S., Melde, K., Mark, A. G., Wetterauer, U., Miernik, A., Fischer, P.

ACS Applied Materials & Interfaces, 9(49):42536 - 42543, November 2017 (article)

Abstract
Endoscopy enables minimally invasive procedures in many medical fields, such as urology. However, current endoscopes are normally cable-driven, which limits their dexterity and makes them hard to miniaturize. Indeed current urological endoscopes have an outer diameter of about 3 mm and still only possess one bending degree of freedom. In this paper, we report a novel wireless actuation mechanism that increases the dexterity and that permits the miniaturization of a urological endoscope. The novel actuator consists of thin active surfaces that can be readily attached to any device and are wirelessly powered by ultrasound. The surfaces consist of two-dimensional arrays of micro-bubbles, which oscillate under ultrasound excitation and thereby generate an acoustic streaming force. Bubbles of different sizes are addressed by their unique resonance frequency, thus multiple degrees of freedom can readily be incorporated. Two active miniaturized devices (with a side length of around 1 mm) are demonstrated: a miniaturized mechanical arm that realizes two degrees of freedom, and a flexible endoscope prototype equipped with a camera at the tip. With the flexible endoscope, an active endoscopic examination is successfully performed in a rabbit bladder. This results show the potential medical applicability of surface actuators wirelessly powered by ultrasound penetrating through biological tissues.

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link (url) DOI Project Page [BibTex]

link (url) DOI Project Page [BibTex]


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Active Acoustic Surfaces Enable the Propulsion of a Wireless Robot

Qiu, T., Palagi, S., Mark, A. G., Melde, K., Adams, F., Fischer, P.

Advanced Materials Interfaces, 4(21):1700933, September 2017 (article)

Abstract
A major challenge that prevents the miniaturization of mechanically actuated systems is the lack of suitable methods that permit the efficient transfer of power to small scales. Acoustic energy holds great potential, as it is wireless, penetrates deep into biological tissues, and the mechanical vibrations can be directly converted into directional forces. Recently, active acoustic surfaces are developed that consist of 2D arrays of microcavities holding microbubbles that can be excited with an external acoustic field. At resonance, the surfaces give rise to acoustic streaming and thus provide a highly directional propulsive force. Here, this study advances these wireless surface actuators by studying their force output as the size of the bubble-array is increased. In particular, a general method is reported to dramatically improve the propulsive force, demonstrating that the surface actuators are actually able to propel centimeter-scale devices. To prove the flexibility of the functional surfaces as wireless ready-to-attach actuator, a mobile mini-robot capable of propulsion in water along multiple directions is presented. This work paves the way toward effectively exploiting acoustic surfaces as a novel wireless actuation scheme at small scales.

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link (url) DOI Project Page [BibTex]


Thumb xl jeong et al 2017 advanced science
Corrosion-Protected Hybrid Nanoparticles

Jeong, H. H., Alarcon-Correa, M., Mark, A. G., Son, K., Lee, T., Fischer, P.

Advanced Science, 4(12):1700234, September 2017 (article)

Abstract
Nanoparticles composed of functional materials hold great promise for applications due to their unique electronic, optical, magnetic, and catalytic properties. However, a number of functional materials are not only difficult to fabricate at the nanoscale, but are also chemically unstable in solution. Hence, protecting nanoparticles from corrosion is a major challenge for those applications that require stability in aqueous solutions and biological fluids. Here, this study presents a generic scheme to grow hybrid 3D nanoparticles that are completely encapsulated by a nm thick protective shell. The method consists of vacuum-based growth and protection, and combines oblique physical vapor deposition with atomic layer deposition. It provides wide flexibility in the shape and composition of the nanoparticles, and the environments against which particles are protected. The work demonstrates the approach with multifunctional nanoparticles possessing ferromagnetic, plasmonic, and chiral properties. The present scheme allows nanocolloids, which immediately corrode without protection, to remain functional, at least for a week, in acidic solutions.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Locomotion of light-driven soft microrobots through a hydrogel via local melting

Palagi, S., Mark, A. G., Melde, K., Qiu, T., Zeng, H., Parmeggiani, C., Martella, D., Wiersma, D. S., Fischer, P.

In 2017 International Conference on Manipulation, Automation and Robotics at Small Scales (MARSS), pages: 1-5, July 2017 (inproceedings)

Abstract
Soft mobile microrobots whose deformation can be directly controlled by an external field can adapt to move in different environments. This is the case for the light-driven microrobots based on liquid-crystal elastomers (LCEs). Here we show that the soft microrobots can move through an agarose hydrogel by means of light-controlled travelling-wave motions. This is achieved by exploiting the inherent rise of the LCE temperature above the melting temperature of the agarose gel, which facilitates penetration of the microrobot through the hydrogel. The locomotion performance is investigated as a function of the travelling-wave parameters, showing that effective propulsion can be obtained by adapting the generated motion to the specific environmental conditions.

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DOI [BibTex]

DOI [BibTex]


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Non-Equilibrium Assembly of Light-Activated Colloidal Mixtures

Singh, D. P., Choudhury, U., Fischer, P., Mark, A. G.

Advanced Materials, 29, pages: 1701328, June 2017, 32 (article)

Abstract
The collective phenomena exhibited by artificial active matter systems present novel routes to fabricating out-of-equilibrium microscale assemblies. Here, the crystallization of passive silica colloids into well-controlled 2D assemblies is shown, which is directed by a small number of self-propelled active colloids. The active colloids are titania–silica Janus particles that are propelled when illuminated by UV light. The strength of the attractive interaction and thus the extent of the assembled clusters can be regulated by the light intensity. A remarkably small number of the active colloids is sufficient to induce the assembly of the dynamic crystals. The approach produces rationally designed colloidal clusters and crystals with controllable sizes, shapes, and symmetries. This multicomponent active matter system offers the possibility of obtaining structures and assemblies that cannot be found in equilibrium systems.

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link (url) DOI [BibTex]


Thumb xl kim et al 2017 advanced materials
Nanodiamonds That Swim

Kim, J. T., Choudhury, U., Hyeon-Ho, J., Fischer, P.

Advanced Materials, 29(30):1701024, June 2017, Back Cover (article)

Abstract
Nanodiamonds are emerging as nanoscale quantum probes for bio-sensing and imaging. This necessitates the development of new methods to accurately manipulate their position and orientation in aqueous solutions. The realization of an “active” nanodiamond (ND) swimmer in fluids, composed of a ND crystal containing nitrogen vacancy centers and a light-driven self-thermophoretic micromotor, is reported. The swimmer is propelled by a local temperature gradient created by laser illumination on its metal-coated side. Its locomotion—from translational to rotational motion—is successfully controlled by shape-dependent hydrodynamic interactions. The precise engineering of the swimmer's geometry is achieved by self-assembly combined with physical vapor shadow growth. The optical addressability of the suspended ND swimmers is demonstrated by observing the electron spin resonance in the presence of magnetic fields. Active motion at the nanoscale enables new sensing capabilities combined with active transport including, potentially, in living organisms.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Soft 3D-Printed Phantom of the Human Kidney with Collecting System

Adams, F., Qiu, T., Mark, A., Fritz, B., Kramer, L., Schlager, D., Wetterauer, U., Miernik, A., Fischer, P.

Ann. of Biomed. Eng., 45(4):963-972, April 2017 (article)

Abstract
Organ models are used for planning and simulation of operations, developing new surgical instruments, and training purposes. There is a substantial demand for in vitro organ phantoms, especially in urological surgery. Animal models and existing simulator systems poorly mimic the detailed morphology and the physical properties of human organs. In this paper, we report a novel fabrication process to make a human kidney phantom with realistic anatomical structures and physical properties. The detailed anatomical structure was directly acquired from high resolution CT data sets of human cadaveric kidneys. The soft phantoms were constructed using a novel technique that combines 3D wax printing and polymer molding. Anatomical details and material properties of the phantoms were validated in detail by CT scan, ultrasound, and endoscopy. CT reconstruction, ultrasound examination, and endoscopy showed that the designed phantom mimics a real kidney's detailed anatomy and correctly corresponds to the targeted human cadaver's upper urinary tract. Soft materials with a tensile modulus of 0.8-1.5 MPa as well as biocompatible hydrogels were used to mimic human kidney tissues. We developed a method of constructing 3D organ models from medical imaging data using a 3D wax printing and molding process. This method is cost-effective means for obtaining a reproducible and robust model suitable for surgical simulation and training purposes.

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DOI Project Page [BibTex]

DOI Project Page [BibTex]


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Wireless micro-robots for endoscopic applications in urology

Adams, F., Qiu, T., Mark, A. G., Melde, K., Palagi, S., Miernik, A., Fischer, P.

In Eur Urol Suppl, 16(3):e1914, March 2017 (inproceedings)

Abstract
Endoscopy is an essential and common method for both diagnostics and therapy in Urology. Current flexible endoscope is normally cable-driven, thus it is hard to be miniaturized and its reachability is restricted as only one bending section near the tip with one degree of freedom (DoF) is allowed. Recent progresses in micro-robotics offer a unique opportunity for medical inspections in minimally invasive surgery. Micro-robots are active devices that has a feature size smaller than one millimeter and can normally be actuated and controlled wirelessly. Magnetically actuated micro-robots have been demonstrated to propel through biological fluids.Here, we report a novel micro robotic arm, which is actuated wirelessly by ultrasound. It works as a miniaturized endoscope with a side length of ~1 mm, which fits through the 3 Fr. tool channel of a cystoscope, and successfully performs an active cystoscopy in a rabbit bladder.

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link (url) DOI [BibTex]


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Pattern formation and collective effects in populations of magnetic microswimmers

Vach, P. J., (Walker) Schamel, D., Fischer, P., Fratzl, P., Faivre, D.

J. of Phys. D: Appl. Phys., 50(11):11LT03, Febuary 2017 (article)

Abstract
Self-propelled particles are one prototype of synthetic active matter used to understand complex biological processes, such as the coordination of movement in bacterial colonies or schools of fishes. Collective patterns such as clusters were observed for such systems, reproducing features of biological organization. However, one limitation of this model is that the synthetic assemblies are made of identical individuals. Here we introduce an active system based on magnetic particles at colloidal scales. We use identical but also randomly-shaped magnetic micropropellers and show that they exhibit dynamic and reversible pattern formation.

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DOI [BibTex]

DOI [BibTex]


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On-chip enzymatic microbiofuel cell-powered integrated circuits

Mark, A. G., Suraniti, E., Roche, J., Richter, H., Kuhn, A., Mano, N., Fischer, P.

Lab on a Chip, 17(10):1761-1768, Febuary 2017, Recent HOT Article (article)

Abstract
A variety of diagnostic and therapeutic medical technologies rely on long term implantation of an electronic device to monitor or regulate a patient's condition. One proposed approach to powering these devices is to use a biofuel cell to convert the chemical energy from blood nutrients into electrical current to supply the electronics. We present here an enzymatic microbiofuel cell whose electrodes are directly integrated into a digital electronic circuit. Glucose oxidizing and oxygen reducing enzymes are immobilized on microelectrodes of an application specific integrated circuit (ASIC) using redox hydrogels to produce an enzymatic biofuel cell, capable of harvesting electrical power from just a single droplet of 5 mM glucose solution. Optimisation of the fuel cell voltage and power to match the requirements of the electronics allow self-powered operation of the on-board digital circuitry. This study represents a step towards implantable self-powered electronic devices that gather their energy from physiological fluids.

Recent HOT Article.

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DOI [BibTex]

DOI [BibTex]


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Strong Rotational Anisotropies Affect Nonlinear Chiral Metamaterials

Hooper, D. C., Mark, A. G., Kuppe, C., Collins, J. T., Fischer, P., Valev, V. K.

Advanced Materials, 29(13):1605110, January 2017 (article)

Abstract
Masked by rotational anisotropies, the nonlinear chiroptical response of a metamaterial is initially completely inaccessible. Upon rotating the sample the chiral information emerges. These results highlight the need for a general method to extract the true chiral contributions to the nonlinear optical signal, which would be hugely valuable in the present context of increasingly complex chiral meta/nanomaterials.

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DOI [BibTex]

DOI [BibTex]

2008


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Voltage-Controllable Magnetic Composite Based on Multifunctional Polyethylene Microparticles

Ghosh, A., Sheridon, N. K., Fischer, P.

SMALL, 4(11):1956-1958, 2008 (article)

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DOI [BibTex]

2008


2005


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Nonlinear optical spectroscopy of chiral molecules

Fischer, P., Hache, F.

CHIRALITY, 17(8):421-437, 2005 (article)

Abstract
We review nonlinear optical processes that are specific to chiral molecules in solution and on surfaces. In contrast to conventional natural optical activity phenomena, which depend linearly on the electric field strength of the optical field, we discuss how optical processes that are nonlinear (quadratic, cubic, and quartic) functions of the electromagnetic field strength may probe optically active centers and chiral vibrations. We show that nonlinear techniques open entirely new ways of exploring chirality in chemical and biological systems: The cubic processes give rise to nonlinear circular dichroism and nonlinear optical rotation and make it possible to observe dynamic chiral processes at ultrafast time scales. The quadratic second-harmonic and sum-frequency-generation phenomena and the quartic processes may arise entirely in the electric-dipole approximation and do not require the use of circularly polarized light to detect chirality: They provide surface selectivity and their observables can be relatively much larger than in linear optical activity. These processes also give rise to the generation of light at a new color, and in liquids this frequency conversion only occurs if the solution is optically active. We survey recent chiral nonlinear optical experiments and give examples of their application to problems of biophysical interest. (C) 2005 Wiley-Liss, Inc.

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DOI [BibTex]

2005


DOI [BibTex]


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

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

PHYSICAL REVIEW LETTERS, 95(6), 2005 (article)

Abstract
There is significant motivation to develop media with negative refractive indices at optical frequencies, but efforts in this direction are hampered by the weakness of the magnetic response at such frequencies. We show theoretically that a nonmagnetic medium with two atomic or molecular constituents can exhibit a negative refractive index. A negative index is possible even when the real parts of both the permittivity and permeability are positive. This surprising result provides a route to isotropic negative-index media at optical frequencies.

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DOI [BibTex]

DOI [BibTex]