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2020


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Fabrication and temperature-dependent magnetic properties of large-area L10-FePt/Co exchange-spring magnet nanopatterns

Son, K., Schütz, G.

{Physica E: Low-Dimensional Systems And Nanostructures}, 115, North-Holland, Amsterdam, 2020 (article)

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DOI [BibTex]

2020


DOI [BibTex]

2019


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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]


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Microrobotics and Microorganisms: Biohybrid Autonomous Cellular Robots

Alapan, Y., Yasa, O., Yigit, B., Yasa, I. C., Erkoc, P., Sitti, M.

Annual Review of Control, Robotics, and Autonomous Systems, 2019 (article)

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[BibTex]

[BibTex]


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X-ray Optics Fabrication Using Unorthodox Approaches

Sanli, U., Baluktsian, M., Ceylan, H., Sitti, M., Weigand, M., Schütz, G., Keskinbora, K.

Bulletin of the American Physical Society, APS, 2019 (article)

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[BibTex]

[BibTex]


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Nanoscale detection of spin wave deflection angles in permalloy

Gross, F., Träger, N., Förster, J., Weigand, M., Schütz, G., Gräfe, J.

{Applied Physics Letters}, 114(1), American Institute of Physics, Melville, NY, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Extracting the dynamic magnetic contrast in time-resolved X-ray transmission microscopy

Schaffers, T., Feggeler, T., Pile, S., Meckenstock, R., Buchner, M., Spoddig, D., Ney, V., Farle, M., Wende, H., Wintz, S., Weigand, M., Ohldag, H., Ollefs, K, Ney, A.

{Nanomaterials}, 9(7), MDPI, Basel, Schweiz, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Generation of switchable singular beams with dynamic metasurfaces

Yu, P., Li, J., Li, X., Schütz, G., Hirscher, M., Zhang, S., Liu, N.

{ACS Nano}, 13(6):7100-7106, American Chemical Society, Washington, DC, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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The near and far of a pair of magnetic capillary disks

Koens, L., Wang, W., Sitti, M., Lauga, E.

Soft Matter, 2019 (article)

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[BibTex]

[BibTex]


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Coherent excitation of heterosymmetric spin waves with ultrashort wavelengths

Dieterle, G., Förster, J., Stoll, H., Semisalova, A. S., Finizio, S., Gangwar, A., Weigand, M., Noske, M., Fähnle, M., Bykova, I., Gräfe, J., Bozhko, D. A., Musiienko-Shmarova, H. Y., Tiberkevich, V., Slavin, A. N., Back, C. H., Raabe, J., Schütz, G., Wintz, S.

{Physical Review Letters}, 122(11), American Physical Society, Woodbury, N.Y., 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Reprogrammability and Scalability of Magnonic Fibonacci Quasicrystals

Lisiecki, F., Rychły, J., Kuświk, P., Głowiński, H., Kłos, J. W., Groß, F., Bykova, I., Weigand, M., Zelent, M., Goering, E. J., Schütz, G., Gubbiotti, G., Krawczyk, M., Stobiecki, F., Dubowik, J., Gräfe, J.

Physical Review Applied, 11, pages: 054003, 2019 (article)

Abstract
Magnonic crystals are systems that can be used to design and tune the dynamic properties of magnetization. Here, we focus on one-dimensional Fibonacci magnonic quasicrystals. We confirm the existence of collective spin waves propagating through the structure as well as dispersionless modes; the reprogammability of the resonance frequencies, dependent on the magnetization order; and dynamic spin-wave interactions. With the fundamental understanding of these properties, we lay a foundation for the scalable and advanced design of spin-wave band structures for spintronic, microwave, and magnonic applications.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Coordinated molecule-modulated magnetic phase with metamagnetism in metal-organic frameworks

Son, K., Kim, J. Y., Schütz, G., Kang, S. G., Moon, H. R., Oh, H.

{Inorganic Chemistry}, 58(14):8895-8899, American Chemical Society, Washington, DC, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Review of emerging concepts in nanotoxicology: opportunities and challenges for safer nanomaterial design

Singh, A. V., Laux, P., Luch, A., Sudrik, C., Wiehr, S., Wild, A., Santamauro, G., Bill, J., Sitti, M.

Toxicology Mechanisms and Methods, 2019 (article)

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[BibTex]

[BibTex]


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Graphene oxide synergistically enhances antibiotic efficacy in Vancomycin resistance Staphylococcus aureus

Singh, V., Kumar, V., Kashyap, S., Singh, A. V., Kishore, V., Sitti, M., Saxena, P. S., Srivastava, A.

ACS Applied Bio Materials, ACS Publications, 2019 (article)

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[BibTex]

[BibTex]


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Magnons in a Quasicrystal: Propagation, Extinction, and Localization of Spin Waves in Fibonacci Structures

Lisiecki, F., Rychły, J., Kuświk, P., Głowiński, H., Kłos, J. W., Groß, F., Träger, N., Bykova, I., Weigand, M., Zelent, M., Goering, E. J., Schütz, G., Krawczyk, M., Stobiecki, F., Dubowik, J., Gräfe, J.

Physical Review Applied, 11, pages: 054061, 2019 (article)

Abstract
Magnonic quasicrystals exceed the possibilities of spin-wave (SW) manipulation offered by regular magnonic crystals, because of their more complex SW spectra with fractal characteristics. Here, we report the direct x-ray microscopic observation of propagating SWs in a magnonic quasicrystal, consisting of dipolar coupled permalloy nanowires arranged in a one-dimensional Fibonacci sequence. SWs from the first and second band as well as evanescent waves from the band gap between them are imaged. Moreover, additional mini band gaps in the spectrum are demonstrated, directly indicating an influence of the quasiperiodicity of the system. Finally, the localization of SW modes within the Fibonacci crystal is shown. The experimental results are interpreted using numerical calculations and we deduce a simple model to estimate the frequency position of the magnonic gaps in quasiperiodic structures. The demonstrated features of SW spectra in one-dimensional magnonic quasicrystals allow utilizing this class of metamaterials for magnonics and make them an ideal basis for future applications.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Microfluidics Integrated Lithography‐Free Nanophotonic Biosensor for the Detection of Small Molecules

Sreekanth, K. V., Sreejith, S., Alapan, Y., Sitti, M., Lim, C. T., Singh, R.

Advanced Optical Materials, 2019 (article)

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[BibTex]

[BibTex]


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Mobile microrobots for active therapeutic delivery

Erkoc, P., Yasa, I. C., Ceylan, H., Yasa, O., Alapan, Y., Sitti, M.

Advanced Therapeutics, Wiley Online Library, 2019 (article)

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[BibTex]

[BibTex]


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Interpreting first-order reversal curves beyond the Preisach model: An experimental permalloy microarray investigation

Groß, F., Ilse, S. E., Schütz, G., Gräfe, J., Goering, E.

{Physical Review B}, 99(6), American Physical Society, Woodbury, NY, 2019 (article)

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DOI [BibTex]


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Bistability of magnetic states in Fe-Pd nanocap arrays

Aravind, P. B., Heigl, M., Fix, M., Groß, F., Gräfe, J., Mary, A., Rajgowrav, C. R., Krupiński, M., Marszałek, M., Thomas, S., Anantharaman, M. R., Albrecht, M.

Nanotechnology, 30, pages: 405705, 2019 (article)

Abstract
Magnetic bistability between vortex and single domain states in nanostructures are of great interest from both fundamental and technological perspectives. In soft magnetic nanostructures, the transition from a uniform collinear magnetic state to a vortex state (or vice versa) induced by a magnetic field involves an energy barrier. If the thermal energy is large enough for overcoming this energy barrier, magnetic bistability with a hysteresis-free switching occurs between the two magnetic states. In this work, we tune this energy barrier by tailoring the composition of FePd alloys, which were deposited onto self-assembled particle arrays forming magnetic vortex structures on top of the particles. The bifurcation temperature, where a hysteresis-free transition occurs, was extracted from the temperature dependence of the annihilation and nucleation field which increases almost linearly with Fe content of the magnetic alloy. This study provides insights into the magnetization reversal process associated with magnetic bistability, which allows adjusting the bifurcation temperature range by the material properties of the nanosystem.

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link (url) [BibTex]

link (url) [BibTex]


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An international laboratory comparison study of volumetric and gravimetric hydrogen adsorption measurements

Hurst, K. E., Gennett, T., Adams, J., Allendorf, M. D., Balderas-Xicohténcatl, R., Bielewski, M., Edwards, B., Espinal, L., Fultz, B., Hirscher, M., Hudson, M. S. L., Hulvey, Z., Latroche, M., Liu, D., Kapelewski, M., Napolitano, E., Perry, Z. T., Purewal, J., Stavila, V., Veenstra, M., White, J. L., Yuan, Y., Zhou, H., Zlotea, C., Parilla, P.

{ChemPhysChem}, 20(15):1997-2009, Wiley-VCH, Weinheim, Germany, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Electromechanical actuation of dielectric liquid crystal elastomers for soft robotics

Davidson, Z., Shahsavan, H., Guo, Y., Hines, L., Xia, Y., Yang, S., Sitti, M.

Bulletin of the American Physical Society, APS, 2019 (article)

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[BibTex]

[BibTex]


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The route to supercurrent transparent ferromagnetic barriers in superconducting matrix

Ivanov, Y. P., Soltan, S., Albrecht, J., Goering, E., Schütz, G., Zhang, Z., Chuvilin, A.

{ACS Nano}, 13(5):5655-5661, American Chemical Society, Washington, DC, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Systematic experimental study on quantum sieving of hydrogen isotopes in metal-amide-imidazolate frameworks with narrow 1-D channels

Mondal, S. S., Kreuzer, A., Behrens, K., Schütz, G., Holdt, H., Hirscher, M.

{ChemPhysChem}, 20(10):1311-1315, Wiley-VCH, Weinheim, Germany, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Artifacts from manganese reduction in rock samples prepared by focused ion beam (FIB) slicing for X-ray microspectroscopy

Macholdt, D. S., Förster, J., Müller, M., Weber, B., Kappl, M., Kilcoyne, A. L. D., Weigand, M., Leitner, J., Jochum, K. P., Pöhlker, C., Andreae, M. O.

{Geoscientific instrumentation, methods and data systems}, 8(1):97-111, Copernicus Publ., Göttingen, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Mixed-state magnetotransport properties of MgB2 thin film prepared by pulsed laser deposition on an Al2O3 substrate

Alzayed, N. S., Shahabuddin, M., Ramey, S. M., Soltan, S.

{Journal of Materials Science: Materials in Electronics}, 30(2):1547-1552, Springer, Norwell, MA, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Comparison of theories of fast and ultrafast magnetization dynamics

Fähnle, M.

{Journal of Magnetism and Magnetic Materials}, 469, pages: 28-29, NH, Elsevier, Amsterdam, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Concepts for improving hydrogen storage in nanoporous materials

Broom, D. P., Webb, C. J., Fanourgakis, G. S., Froudakis, G. E., Trikalitis, P. N., Hirscher, M.

{International Journal of Hydrogen Energy}, 44(15):7768-7779, Elsevier, Amsterdam, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Controlling dislocation nucleation-mediatd plasticity in nanostructures via surface modification

Shin, J., Chen, L. Y., Sanli, U. T., Richter, G., Labat, S., Richard, M., Cornelius, T., Thomas, O., Gianola, D. S.

{Acta Materialia}, 166, pages: 572-586, Elsevier Science, Kidlington, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Reprogrammability and scalability of magnonic Fibonacci quasicrystals

Lisiecki, F., Rychly, J., Kuswik, P., Glowinski, H., Klos, J. W., Groß, F., Bykova, I., Weigand, M., Zelent, M., Goering, E. J., Schütz, G., Gubbiotti, G., Krawczyk, M., Stobiecki, F., Dubowik, J., Gräfe, J.

{Physical Review Applied}, 11(5), American Physical Society, College Park, Md. [u.a.], 2019 (article)

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DOI [BibTex]

DOI [BibTex]

2018


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Role of symmetry in driven propulsion at low Reynolds number

Sachs, J., Morozov, K. I., Kenneth, O., Qiu, T., Segreto, N., Fischer, P., Leshansky, A. M.

Phys. Rev. E, 98(6):063105, American Physical Society, December 2018 (article)

Abstract
We theoretically and experimentally investigate low-Reynolds-number propulsion of geometrically achiral planar objects that possess a dipole moment and that are driven by a rotating magnetic field. Symmetry considerations (involving parity, $\widehat{P}$, and charge conjugation, $\widehat{C}$) establish correspondence between propulsive states depending on orientation of the dipolar moment. Although basic symmetry arguments do not forbid individual symmetric objects to efficiently propel due to spontaneous symmetry breaking, they suggest that the average ensemble velocity vanishes. Some additional arguments show, however, that highly symmetrical ($\widehat{P}$-even) objects exhibit no net propulsion while individual less symmetrical ($\widehat{C}\widehat{P}$-even) propellers do propel. Particular magnetization orientation, rendering the shape $\widehat{C}\widehat{P}$-odd, yields unidirectional motion typically associated with chiral structures, such as helices. If instead of a structure with a permanent dipole we consider a polarizable object, some of the arguments have to be modified. For instance, we demonstrate a truly achiral ($\widehat{P}$- and $\widehat{C}\widehat{P}$-even) planar shape with an induced electric dipole that can propel by electro-rotation. We thereby show that chirality is not essential for propulsion due to rotation-translation coupling at low Reynolds number.

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link (url) DOI Project Page [BibTex]

2018


link (url) DOI Project Page [BibTex]


Thumb xl screenshot 2018 5 9 swimming back and forth using planar flagellar propulsion at low reynolds numbers   khalil   2018   adv ...
Swimming Back and Forth Using Planar Flagellar Propulsion at Low Reynolds Numbers

Khalil, I. S. M., Tabak, A. F., Hamed, Y., Mitwally, M. E., Tawakol, M., Klingner, A., Sitti, M.

Advanced Science, 5(2):1700461, 2018 (article)

Abstract
Abstract Peritrichously flagellated Escherichia coli swim back and forth by wrapping their flagella together in a helical bundle. However, other monotrichous bacteria cannot swim back and forth with a single flagellum and planar wave propagation. Quantifying this observation, a magnetically driven soft two‐tailed microrobot capable of reversing its swimming direction without making a U‐turn trajectory or actively modifying the direction of wave propagation is designed and developed. The microrobot contains magnetic microparticles within the polymer matrix of its head and consists of two collinear, unequal, and opposite ultrathin tails. It is driven and steered using a uniform magnetic field along the direction of motion with a sinusoidally varying orthogonal component. Distinct reversal frequencies that enable selective and independent excitation of the first or the second tail of the microrobot based on their tail length ratio are found. While the first tail provides a propulsive force below one of the reversal frequencies, the second is almost passive, and the net propulsive force achieves flagellated motion along one direction. On the other hand, the second tail achieves flagellated propulsion along the opposite direction above the reversal frequency.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Optical and Thermophoretic Control of Janus Nanopen Injection into Living Cells

Maier, C. M., Huergo, M. A., Milosevic, S., Pernpeintner, C., Li, M., Singh, D. P., Walker, D., Fischer, P., Feldmann, J., Lohmüller, T.

Nano Letters, 18, pages: 7935–7941, November 2018 (article) Accepted

Abstract
Devising strategies for the controlled injection of functional nanoparticles and reagents into living cells paves the way for novel applications in nanosurgery, sensing, and drug delivery. Here, we demonstrate the light-controlled guiding and injection of plasmonic Janus nanopens into living cells. The pens are made of a gold nanoparticle attached to a dielectric alumina shaft. Balancing optical and thermophoretic forces in an optical tweezer allows single Janus nanopens to be trapped and positioned on the surface of living cells. While the optical injection process involves strong heating of the plasmonic side, the temperature of the alumina stays significantly lower, thus allowing the functionalization with fluorescently labeled, single-stranded DNA and, hence, the spatially controlled injection of genetic material with an untethered nanocarrier.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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A swarm of slippery micropropellers penetrates the vitreous body of the eye

Wu, Z., Troll, J., Jeong, H. H., Wei, Q., Stang, M., Ziemssen, F., Wang, Z., Dong, M., Schnichels, S., Qiu, T., Fischer, P.

Science Advances, 4(11):eaat4388, November 2018 (article)

Abstract
The intravitreal delivery of therapeutic agents promises major benefits in the field of ocular medicine. Traditional delivery methods rely on the random, passive diffusion of molecules, which do not allow for the rapid delivery of a concentrated cargo to a defined region at the posterior pole of the eye. The use of particles promises targeted delivery but faces the challenge that most tissues including the vitreous have a tight macromolecular matrix that acts as a barrier and prevents its penetration. Here, we demonstrate novel intravitreal delivery microvehicles slippery micropropellers that can be actively propelled through the vitreous humor to reach the retina. The propulsion is achieved by helical magnetic micropropellers that have a liquid layer coating to minimize adhesion to the surrounding biopolymeric network. The submicrometer diameter of the propellers enables the penetration of the biopolymeric network and the propulsion through the porcine vitreous body of the eye over centimeter distances. Clinical optical coherence tomography is used to monitor the movement of the propellers and confirm their arrival on the retina near the optic disc. Overcoming the adhesion forces and actively navigating a swarm of micropropellers in the dense vitreous humor promise practical applications in ophthalmology.

pf

Video: Nanorobots propel through the eye link (url) DOI [BibTex]

Video: Nanorobots propel through the eye link (url) DOI [BibTex]


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Universal Custom Complex Magnetic Spring Design Methodology

Woodward, M. A., Sitti, M.

IEEE Transactions on Magnetics, 54(1):1-13, October 2018 (article)

Abstract
A design methodology is presented for creating custom complex magnetic springs through the design of force-displacement curves. This methodology results in a magnet configuration, which will produce a desired force-displacement relationship. Initially, the problem is formulated and solved as a system of linear equations. Then, given the limited likelihood of a single solution being feasibly manufactured, key parameters of the solution are extracted and varied to create a family of solutions. Finally, these solutions are refined using numerical optimization. Given the properties of magnets, this methodology can create any well-defined function of force versus displacement and is model-independent. To demonstrate this flexibility, a number of example magnetic springs are designed; one of which, designed for use in a jumping-gliding robot's shape memory alloy actuated clutch, is manufactured and experimentally characterized. Due to the scaling of magnetic forces, the displacement region which these magnetic springs are most applicable is that of millimeters and below. However, this region is well situated for miniature robots and smart material actuators, where a tailored magnetic spring, designed to compliment a component, can enhance its performance while adding new functionality. The methodology is also expendable to variable interactions and multi-dimensional magnetic field design.

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DOI [BibTex]

DOI [BibTex]


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Fast spatial scanning of 3D ultrasound fields via thermography

Melde, K., Qiu, T., Fischer, P.

Applied Physics Letters, 113(13):133503, September 2018 (article)

Abstract
We propose and demonstrate a thermographic method that allows rapid scanning of ultrasound fields in a volume to yield 3D maps of the sound intensity. A thin sound-absorbing membrane is continuously translated through a volume of interest while a thermal camera records the evolution of its surface temperature. The temperature rise is a function of the absorbed sound intensity, such that the thermal image sequence can be combined to reveal the sound intensity distribution in the traversed volume. We demonstrate the mapping of ultrasound fields, which is several orders of magnitude faster than scanning with a hydrophone. Our results are in very good agreement with theoretical simulations.

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link (url) DOI Project Page [BibTex]


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Diffusion Measurements of Swimming Enzymes with Fluorescence Correlation Spectroscopy

Günther, J., Börsch, M., Fischer, P.

Accounts of Chemical Research, 51(9):1911-1920, August 2018 (article)

Abstract
Self-propelled chemical motors are chemically powered micro- or nanosized swimmers. The energy required for these motors’ active motion derives from catalytic chemical reactions and the transformation of a fuel dissolved in the solution. While self-propulsion is now well established for larger particles, it is still unclear if enzymes, nature’s nanometer-sized catalysts, are potentially also self-powered nanomotors. Because of its small size, any increase in an enzyme’s diffusion due to active self-propulsion must be observed on top of the enzyme’s passive Brownian motion, which dominates at this scale. Fluorescence correlation spectroscopy (FCS) is a sensitive method to quantify the diffusion properties of single fluorescently labeled molecules in solution. FCS experiments have shown a general increase in the diffusion constant of a number of enzymes when the enzyme is catalytically active. Diffusion enhancements after addition of the enzyme’s substrate (and sometimes its inhibitor) of up to 80\% have been reported, which is at least 1 order of magnitude higher than what theory would predict. However, many factors contribute to the FCS signal and in particular the shape of the autocorrelation function, which underlies diffusion measurements by fluorescence correlation spectroscopy. These effects need to be considered to establish if and by how much the catalytic activity changes an enzyme’s diffusion.We carefully review phenomena that can play a role in FCS experiments and the determination of enzyme diffusion, including the dissociation of enzyme oligomers upon interaction with the substrate, surface binding of the enzyme to glass during the experiment, conformational changes upon binding, and quenching of the fluorophore. We show that these effects can cause changes in the FCS signal that behave similar to an increase in diffusion. However, in the case of the enzymes F1-ATPase and alkaline phosphatase, we demonstrate that there is no measurable increase in enzyme diffusion. Rather, dissociation and conformational changes account for the changes in the FCS signal in the former and fluorophore quenching in the latter. Within the experimental accuracy of our FCS measurements, we do not observe any change in diffusion due to activity for the enzymes we have investigated.We suggest useful control experiments and additional tests for future FCS experiments that should help establish if the observed diffusion enhancement is real or if it is due to an experimental or data analysis artifact. We show that fluorescence lifetime and mean intensity measurements are essential in order to identify the nature of the observed changes in the autocorrelation function. While it is clear from theory that chemically active enzymes should also act as self-propelled nanomotors, our FCS measurements show that the associated increase in diffusion is much smaller than previously reported. Further experiments are needed to quantify the contribution of the enzymes’ catalytic activity to their self-propulsion. We hope that our findings help to establish a useful protocol for future FCS studies in this field and help establish by how much the diffusion of an enzyme is enhanced through catalytic activity.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Uphill production of dihydrogen by enzymatic oxidation of glucose without an external energy source

Suraniti, E., Merzeau, P., Roche, J., Gounel, S., Mark, A. G., Fischer, P., Mano, N., Kuhn, A.

Nature Communications, 9(1):3229, August 2018 (article)

Abstract
Chemical systems do not allow the coupling of energy from several simple reactions to drive a subsequent reaction, which takes place in the same medium and leads to a product with a higher energy than the one released during the first reaction. Gibbs energy considerations thus are not favorable to drive e.g., water splitting by the direct oxidation of glucose as a model reaction. Here, we show that it is nevertheless possible to carry out such an energetically uphill reaction, if the electrons released in the oxidation reaction are temporarily stored in an electromagnetic system, which is then used to raise the electrons' potential energy so that they can power the electrolysis of water in a second step. We thereby demonstrate the general concept that lower energy delivering chemical reactions can be used to enable the formation of higher energy consuming reaction products in a closed system.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Chemical micromotors self-assemble and self-propel by spontaneous symmetry breaking

Yu, T., Chuphal, P., Thakur, S., Reigh, S. Y., Singh, D. P., Fischer, P.

Chem. Comm., 54, pages: 11933-11936, August 2018 (article)

Abstract
Self-propelling chemical motors have thus far required the fabrication of Janus particles with an asymmetric catalyst distribution. Here, we demonstrate that simple, isotropic colloids can spontaneously assemble to yield dimer motors that self-propel. In a mixture of isotropic titanium dioxide colloids with photo-chemical catalytic activity and passive silica colloids, light illumination causes diffusiophoretic attractions between the active and passive particles and leads to the formation of dimers. The dimers constitute a symmetry-broken motor, whose dynamics can be fully controlled by the illumination conditions. Computer simulations reproduce the dynamics of the colloids and are in good agreement with experiments. The current work presents a simple route to obtain large numbers of self-propelling chemical motors from a dispersion of spherically symmetric colloids through spontaneous symmetry breaking.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Chemotaxis of Active Janus Nanoparticles

Popescu, M. N., Uspal, W. E., Bechinger, C., Fischer, P.

Nano Letters, 18(9):5345–5349, July 2018 (article)

Abstract
While colloids and molecules in solution exhibit passive Brownian motion, particles that are partially covered with a catalyst, which promotes the transformation of a fuel dissolved in the solution, can actively move. These active Janus particles are known as “chemical nanomotors” or self-propelling “swimmers” and have been realized with a range of catalysts, sizes, and particle geometries. Because their active translation depends on the fuel concentration, one expects that active colloidal particles should also be able to swim toward a fuel source. Synthesizing and engineering nanoparticles with distinct chemotactic properties may enable important developments, such as particles that can autonomously swim along a pH gradient toward a tumor. Chemotaxis requires that the particles possess an active coupling of their orientation to a chemical gradient. In this Perspective we provide a simple, intuitive description of the underlying mechanisms for chemotaxis, as well as the means to analyze and classify active particles that can show positive or negative chemotaxis. The classification provides guidance for engineering a specific response and is a useful organizing framework for the quantitative analysis and modeling of chemotactic behaviors. Chemotaxis is emerging as an important focus area in the field of active colloids and promises a number of fascinating applications for nanoparticles and particle-based delivery.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Programmable collective behavior in dynamically self-assembled mobile microrobotic swarms

B Yigit, , Y Alapan, , Sitti, M.

Advanced Science, July 2018 (article)

Abstract
Collective control of mobile microrobotic swarms is indispensable for their potential high-impact applications in targeted drug delivery, medical diagnostics, parallel micromanipulation, and environmental sensing and remediation. Lack of on-board computational and sensing capabilities in current microrobotic systems necessitates use of physical interactions among individual microrobots for local physical communication and cooperation. Here, we show that mobile microrobotic swarms with well-defined collective behavior can be designed by engineering magnetic interactions among individual units. Microrobots, consisting of a linear chain of self-assembled magnetic microparticles, locomote on surfaces in response to a precessing magnetic field. Control over the direction of precessing magnetic field allows engineering attractive and repulsive interactions among microrobots and, thus, collective order with well-defined spatial organization and parallel operation over macroscale distances (~ 1 cm). These microrobotic swarms can be guided through confined spaces, while preserving microrobot morphology and function. These swarms can further achieve directional transport of large cargoes on surfaces and small cargoes in bulk fluids. Described design approach, exploiting physical interactions among individual robots, enables facile and rapid formation of self-organized and reconfigurable microrobotic swarms with programmable collective order.

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link (url) [BibTex]


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3D-Printed Biodegradable Microswimmer for Drug Delivery and Targeted Cell Labeling

Hakan Ceylan, , I. Ceren Yasa, , Oncay Yasa, , Ahmet Fatih Tabak, , Joshua Giltinan, , Sitti, M.

bioRxiv, pages: 379024, July 2018 (article)

Abstract
Miniaturization of interventional medical devices can leverage minimally invasive technologies by enabling operational resolution at cellular length scales with high precision and repeatability. Untethered micron-scale mobile robots can realize this by navigating and performing in hard-to-reach, confined and delicate inner body sites. However, such a complex task requires an integrated design and engineering strategy, where powering, control, environmental sensing, medical functionality and biodegradability need to be considered altogether. The present study reports a hydrogel-based, biodegradable microrobotic swimmer, which is responsive to the changes in its microenvironment for theranostic cargo delivery and release tasks. We design a double-helical magnetic microswimmer of 20 micrometers length, which is 3D-printed with complex geometrical and compositional features. At normal physiological concentrations, matrix metalloproteinase-2 (MMP-2) enzyme can entirely degrade the microswimmer body in 118 h to solubilized non-toxic products. The microswimmer can respond to the pathological concentrations of MMP-2 by swelling and thereby accelerating the release kinetics of the drug payload. Anti-ErbB 2 antibody-tagged magnetic nanoparticles released from the degraded microswimmers serve for targeted labeling of SKBR3 breast cancer cells to realize the potential of medical imaging of local tissue sites following the therapeutic intervention. These results represent a leap forward toward clinical medical microrobots that are capable of sensing, responding to the local pathological information, and performing specific therapeutic and diagnostic tasks as orderly executed operations using their smart composite material architectures.

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DOI Project Page [BibTex]


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Innate turning preference of leaf-cutting ants in the absence of external orientation cues

Endlein, T., Sitti, M.

Journal of Experimental Biology, The Company of Biologists Ltd, June 2018 (article)

Abstract
Many ants use a combination of cues for orientation but how do ants find their way when all external cues are suppressed? Do they walk in a random way or are their movements spatially oriented? Here we show for the first time that leaf-cutting ants (Acromyrmex lundii) have an innate preference of turning counter-clockwise (left) when external cues are precluded. We demonstrated this by allowing individual ants to run freely on the water surface of a newly-developed treadmill. The surface tension supported medium-sized workers but effectively prevented ants from reaching the wall of the vessel, important to avoid wall-following behaviour (thigmotaxis). Most ants ran for minutes on the spot but also slowly turned counter-clockwise in the absence of visual cues. Reconstructing the effectively walked path revealed a looping pattern which could be interpreted as a search strategy. A similar turning bias was shown for groups of ants in a symmetrical Y-maze where twice as many ants chose the left branch in the absence of optical cues. Wall-following behaviour was tested by inserting a coiled tube before the Y-fork. When ants traversed a left-coiled tube, more ants chose the left box and vice versa. Adding visual cues in form of vertical black strips either outside the treadmill or on one branch of the Y-maze led to oriented walks towards the strips. It is suggested that both, the turning bias and the wall-following are employed as search strategies for an unknown environment which can be overridden by visual cues.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]


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Motility and chemotaxis of bacteria-driven microswimmers fabricated using antigen 43-mediated biotin display

Schauer, O., Mostaghaci, B., Colin, R., Hürtgen, D., Kraus, D., Sitti, M., Sourjik, V.

Scientific Reports, 8(1):9801, Nature Publishing Group, June 2018 (article)

Abstract
Bacteria-driven biohybrid microswimmers (bacteriabots) combine synthetic cargo with motile living bacteria that enable propulsion and steering. Although fabrication and potential use of such bacteriabots have attracted much attention, existing methods of fabrication require an extensive sample preparation that can drastically decrease the viability and motility of bacteria. Moreover, chemotactic behavior of bacteriabots in a liquid medium with chemical gradients has remained largely unclear. To overcome these shortcomings, we designed Escherichia coli to autonomously display biotin on its cell surface via the engineered autotransporter antigen 43 and thus to bind streptavidin-coated cargo. We show that the cargo attachment to these bacteria is greatly enhanced by motility and occurs predominantly at the cell poles, which is greatly beneficial for the fabrication of motile bacteriabots. We further performed a systemic study to understand and optimize the ability of these bacteriabots to follow chemical gradients. We demonstrate that the chemotaxis of bacteriabots is primarily limited by the cargo-dependent reduction of swimming speed and show that the fabrication of bacteriabots using elongated E. coli cells can be used to overcome this limitation.

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link (url) DOI [BibTex]

link (url) DOI [BibTex]