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2019


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An ACT-R approach to investigating mechanisms of performance-related changes in an interrupted learning task

Wirzberger, M., Borst, J. P., Krems, J. F., Rey, G. D.

41st Annual Meeting of the Cognitive Science Society., July 2019 (conference)

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[BibTex]

2019


[BibTex]


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What’s in the Adaptive Toolbox and How Do People Choose From It? Rational Models of Strategy Selection in Risky Choice

Mohnert, F., Pachur, T., Lieder, F.

41st Annual Meeting of the Cognitive Science Society, July 2019 (conference)

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[BibTex]


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Measuring how people learn how to plan

Jain, Y. R., Callaway, F., Lieder, F.

RLDM 2019, July 2019 (conference)

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[BibTex]

[BibTex]


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Measuring how people learn how to plan

Jain, Y. R., Callaway, F., Lieder, F.

41st Annual Meeting of the Cognitive Science Society, July 2019 (conference)

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[BibTex]

[BibTex]


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A model-based explanation of performance related changes in abstract stimulus-response learning

Wirzberger, M., Borst, J. P., Krems, J. F., Rey, G. D.

52nd Annual Meeting of the Society for Mathematical Psychology, July 2019 (conference)

Abstract
Stimulus-response learning constitutes an important part of human experience over the life course. Independent of the domain, it is characterized by changes in performance with increasing task progress. But what cognitive mechanisms are responsible for these changes and how do additional task requirements affect the related dynamics? To inspect that in more detail, we introduce a computational modeling approach that investigates performance-related changes in learning situations with reference to chunk activation patterns. It leverages the cognitive architecture ACT-R to model learner behavior in abstract stimulus-response learning in two conditions of task complexity. Additional situational demands are reflected in embedded secondary tasks that interrupt participants during the learning process. Our models apply an activation equation that also takes into account the association between related nodes of information and the similarity between potential responses. Model comparisons with two human datasets (N = 116 and N = 123 participants) indicate a good fit in terms of both accuracy and reaction times. Based on the existing neurophysiological mapping of ACT-R modules on defined human brain areas, we convolve recorded module activity into simulated BOLD responses to investigate underlying cognitive mechanisms in more detail. The resulting evidence supports the connection of learning effects in both task conditions with activation-related patterns to explain changes in performance.

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[BibTex]

[BibTex]


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A cognitive tutor for helping people overcome present bias

Lieder, F., Callaway, F., Jain, Y., Krueger, P., Das, P., Gul, S., Griffiths, T.

RLDM 2019, July 2019 (conference)

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[BibTex]

[BibTex]


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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.

pf

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.

pf

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)

mms pi

[BibTex]

[BibTex]


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Spatial Continuity Effect vs. Spatial Contiguity Failure. Revising the Effects of Spatial Proximity Between Related and Unrelated Representations

Beege, M., Wirzberger, M., Nebel, S., Schneider, S., Schmidt, N., Rey, G. D.

Frontiers in Education, 4:86, 2019 (article)

Abstract
The split-attention effect refers to learning with related representations in multimedia. Spatial proximity and integration of these representations are crucial for learning processes. The influence of varying amounts of proximity between related and unrelated information has not yet been specified. In two experiments (N1 = 98; N2 = 85), spatial proximity between a pictorial presentation and text labels was manipulated (high vs. medium vs. low). Additionally, in experiment 1, a control group with separated picture and text presentation was implemented. The results revealed a significant effect of spatial proximity on learning performance. In contrast to previous studies, the medium condition leads to the highest transfer, and in experiment 2, the highest retention score. These results are interpreted considering cognitive load and instructional efficiency. Findings indicate that transfer efficiency is optimal at a medium distance between representations in experiment 1. Implications regarding the spatial contiguity principle and the spatial contiguity failure are discussed.

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link (url) 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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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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Doing more with less: Meta-reasoning and meta-learning in humans and machines

Griffiths, T., Callaway, F., Chang, M., Grant, E., Krueger, P. M., Lieder, F.

Current Opinion in Behavioral Sciences, 2019 (article)

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DOI [BibTex]

DOI [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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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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Cognitive Prostheses for Goal Achievement

Lieder, F., Chen, O. X., Krueger, P. M., Griffiths, T.

Nature Human Behavior, 2019 (article)

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DOI [BibTex]

DOI [BibTex]


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Remediating cognitive decline with cognitive tutors

Das, P., Callaway, F., Griffiths, T., Lieder, F.

RLDM 2019, 2019 (conference)

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[BibTex]

[BibTex]


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Effects of system response delays on elderly humans’ cognitive performance in a virtual training scenario

Wirzberger, M., Schmidt, R., Georgi, M., Hardt, W., Brunnett, G., Rey, G. D.

Scientific Reports, 9:8291, 2019 (article)

Abstract
Observed influences of system response delay in spoken human-machine dialogues are rather ambiguous and mainly focus on perceived system quality. Studies that systematically inspect effects on cognitive performance are still lacking, and effects of individual characteristics are also often neglected. Building on benefits of cognitive training for decelerating cognitive decline, this Wizard-of-Oz study addresses both issues by testing 62 elderly participants in a dialogue-based memory training with a virtual agent. Participants acquired the method of loci with fading instructional guidance and applied it afterward to memorizing and recalling lists of German nouns. System response delays were randomly assigned, and training performance was included as potential mediator. Participants’ age, gender, and subscales of affinity for technology (enthusiasm, competence, positive and negative perception of technology) were inspected as potential moderators. The results indicated positive effects on recall performance with higher training performance, female gender, and less negative perception of technology. Additionally, memory retention and facets of affinity for technology moderated increasing system response delays. Participants also provided higher ratings in perceived system quality with higher enthusiasm for technology but reported increasing frustration with a more positive perception of technology. Potential explanations and implications for the design of spoken dialogue systems are discussed.

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link (url) DOI [BibTex]

link (url) 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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A rational reinterpretation of dual process theories

Milli, S., Lieder, F., Griffiths, T.

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.

pf

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.

pf

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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Gait learning for soft microrobots controlled by light fields

Rohr, A. V., Trimpe, S., Marco, A., Fischer, P., Palagi, S.

In International Conference on Intelligent Robots and Systems (IROS) 2018, pages: 6199-6206, International Conference on Intelligent Robots and Systems 2018, October 2018 (inproceedings)

Abstract
Soft microrobots based on photoresponsive materials and controlled by light fields can generate a variety of different gaits. This inherent flexibility can be exploited to maximize their locomotion performance in a given environment and used to adapt them to changing environments. However, because of the lack of accurate locomotion models, and given the intrinsic variability among microrobots, analytical control design is not possible. Common data-driven approaches, on the other hand, require running prohibitive numbers of experiments and lead to very sample-specific results. Here we propose a probabilistic learning approach for light-controlled soft microrobots based on Bayesian Optimization (BO) and Gaussian Processes (GPs). The proposed approach results in a learning scheme that is highly data-efficient, enabling gait optimization with a limited experimental budget, and robust against differences among microrobot samples. These features are obtained by designing the learning scheme through the comparison of different GP priors and BO settings on a semisynthetic data set. The developed learning scheme is validated in microrobot experiments, resulting in a 115% improvement in a microrobot’s locomotion performance with an experimental budget of only 20 tests. These encouraging results lead the way toward self-adaptive microrobotic systems based on lightcontrolled soft microrobots and probabilistic learning control.

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arXiv IEEE Xplore DOI Project Page [BibTex]

arXiv IEEE Xplore DOI Project Page [BibTex]


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Nanoscale robotic agents in biological fluids and tissues

Palagi, S., Walker, D. Q. T., Fischer, P.

In The Encyclopedia of Medical Robotics, 2, pages: 19-42, 2, (Editors: Desai, J. P. and Ferreira, A.), World Scientific, October 2018 (inbook)

Abstract
Nanorobots are untethered structures of sub-micron size that can be controlled in a non-trivial way. Such nanoscale robotic agents are envisioned to revolutionize medicine by enabling minimally invasive diagnostic and therapeutic procedures. To be useful, nanorobots must be operated in complex biological fluids and tissues, which are often difficult to penetrate. In this chapter, we first discuss potential medical applications of motile nanorobots. We briefly present the challenges related to swimming at such small scales and we survey the rheological properties of some biological fluids and tissues. We then review recent experimental results in the development of nanorobots and in particular their design, fabrication, actuation, and propulsion in complex biological fluids and tissues. Recent work shows that their nanoscale dimension is a clear asset for operation in biological tissues, since many biological tissues consist of networks of macromolecules that prevent the passage of larger micron-scale structures, but contain dynamic pores through which nanorobots can move.

pf

link (url) DOI [BibTex]

link (url) 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.

pf

link (url) DOI Project Page [BibTex]


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Discovering and Teaching Optimal Planning Strategies

Lieder, F., Callaway, F., Krueger, P. M., Das, P., Griffiths, T. L., Gul, S.

In The 14th biannual conference of the German Society for Cognitive Science, GK, September 2018 (inproceedings)

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Project Page [BibTex]

Project Page [BibTex]


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Discovering Rational Heuristics for Risky Choice

Gul, S., Krueger, P. M., Callaway, F., Griffiths, T. L., Lieder, F.

The 14th biannual conference of the German Society for Cognitive Science, GK, The 14th biannual conference of the German Society for Cognitive Science, GK, September 2018 (conference)

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Project Page [BibTex]

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.

pf

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.

pf

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.

pf

link (url) DOI [BibTex]

link (url) DOI [BibTex]


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A machine from machines

Fischer, P.

Nature Physics, 14, pages: 1072–1073, July 2018 (misc)

Abstract
Building spinning microrotors that self-assemble and synchronize to form a gear sounds like an impossible feat. However, it has now been achieved using only a single type of building block -- a colloid that self-propels.

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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]