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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]


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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]


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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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Chapter 8 - Micro- and nanorobots in Newtonian and biological viscoelastic fluids

Palagi, S., (Walker) Schamel, D., Qiu, T., Fischer, P.

In Microbiorobotics, pages: 133 - 162, 8, Micro and Nano Technologies, Second edition, Elsevier, Boston, March 2017 (incollection)

Abstract
Swimming microorganisms are a source of inspiration for small scale robots that are intended to operate in fluidic environments including complex biomedical fluids. Nature has devised swimming strategies that are effective at small scales and at low Reynolds number. These include the rotary corkscrew motion that, for instance, propels a flagellated bacterial cell, as well as the asymmetric beat of appendages that sperm cells or ciliated protozoa use to move through fluids. These mechanisms can overcome the reciprocity that governs the hydrodynamics at small scale. The complex molecular structure of biologically important fluids presents an additional challenge for the effective propulsion of microrobots. In this chapter it is shown how physical and chemical approaches are essential in realizing engineered abiotic micro- and nanorobots that can move in biomedically important environments. Interestingly, we also describe a microswimmer that is effective in biological viscoelastic fluids that does not have a natural analogue.

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link (url) DOI [BibTex]

link (url) DOI [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]


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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]


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Convertor

Fischer, P., Mark, A.

May 2014 (patent)

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[BibTex]

[BibTex]


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3D nanofabrication on complex seed shapes using glancing angle deposition

Hyeon-Ho, J., Mark, A. G., Gibbs, J. G., Reindl, T., Waizmann, U., Weis, J., Fischer, P.

In 2014 IEEE 27th International Conference on Micro Electro Mechanical Systems (MEMS), pages: 437-440, January 2014 (inproceedings)

Abstract
Three-dimensional (3D) fabrication techniques promise new device architectures and enable the integration of more components, but fabricating 3D nanostructures for device applications remains challenging. Recently, we have performed glancing angle deposition (GLAD) upon a nanoscale hexagonal seed array to create a variety of 3D nanoscale objects including multicomponent rods, helices, and zigzags [1]. Here, in an effort to generalize our technique, we present a step-by-step approach to grow 3D nanostructures on more complex nanoseed shapes and configurations than before. This approach allows us to create 3D nanostructures on nanoseeds regardless of seed sizes and shapes.

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DOI [BibTex]

DOI [BibTex]


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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]


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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]


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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]


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Active Microrheology of the Vitreous of the Eye applied to Nanorobot Propulsion

Qiu, T., Schamel, D., Mark, A. G., Fischer, P.

In 2014 IEEE INTERNATIONAL CONFERENCE ON ROBOTICS AND AUTOMATION (ICRA), pages: 3801-3806, IEEE International Conference on Robotics and Automation ICRA, 2014, Best Automation Paper Award – Finalist. (inproceedings)

Abstract
Biomedical applications of micro or nanorobots require active movement through complex biological fluids. These are generally non-Newtonian (viscoelastic) fluids that are characterized by complicated networks of macromolecules that have size-dependent rheological properties. It has been suggested that an untethered microrobot could assist in retinal surgical procedures. To do this it must navigate the vitreous humor, a hydrated double network of collagen fibrils and high molecular-weight, polyanionic hyaluronan macromolecules. Here, we examine the characteristic size that potential robots must have to traverse vitreous relatively unhindered. We have constructed magnetic tweezers that provide a large gradient of up to 320 T/m to pull sub-micron paramagnetic beads through biological fluids. A novel two-step electrical discharge machining (EDM) approach is used to construct the tips of the magnetic tweezers with a resolution of 30 mu m and high aspect ratio of similar to 17:1 that restricts the magnetic field gradient to the plane of observation. We report measurements on porcine vitreous. In agreement with structural data and passive Brownian diffusion studies we find that the unhindered active propulsion through the eye calls for nanorobots with cross-sections of less than 500 nm.

Best Automation Paper Award – Finalist.

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[BibTex]

[BibTex]


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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]


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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]


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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]


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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]


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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]


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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]


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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]


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NONLINEAR OPTICAL PROPERTIES OF CHIRAL LIQUIDS Electric-dipolar pseudoscalars in nonlinear optics

Fischer, P., Champagne, B.

In NON-LINEAR OPTICAL PROPERTIES OF MATTER: FROM MOLECULES TO CONDENSED PHASES, 1, pages: 359-381, Challenges and Advances in Computational Chemistry and Physics, 2006 (incollection)

Abstract
We give all overview of linear and nonlinear optical processes that can be specific to chiral molecules in isotropic media. Specifically, we discuss the pseudoscalars that underlie nonlinear optical activity and chiral frequency conversion processes in fluids. We show that nonlinear optical techniques open entirely new ways of exploring chirality: Sum-frequency-generation (SFG) at second-order and BioCARS at fourth-order arise in the electric-dipole approximation and do not require circularly polarized light to detect chiral molecules in solution. Here the frequency conversion in itself is a measure of chirality. This is in contrast to natural optical activity phenomena which are based on the interference of radiation from induced oscillating electric and magnetic dipoles, and which are observed as a differential response to right and left circularly polarized light. We give examples from our SFG experiments in optically active solutions and show how the application of an additional static electric field to sum-frequency generation allows the absolute configuration of the chiral solute to be determined via all electric-dipolar process. Results from ab initio calculations of the SFG pseudoscalar are presented for a number of chiral molecules

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[BibTex]

[BibTex]


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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]


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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]

2002


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Chirality-specific nonlinear spectroscopies in isotropic media

Fischer, P., Albrecht, A.

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

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

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DOI [BibTex]

2002


DOI [BibTex]


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The chiral specificity of sum-frequency generation in solutions

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

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

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

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DOI [BibTex]

DOI [BibTex]


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On optical rectification in isotropic media

Fischer, P., Albrecht, A.

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

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

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[BibTex]

[BibTex]