Browsing by Author "Mourran, Ahmed"
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- Item4D Printing of a Light-Driven Soft Actuator with Programmed Printing Density(Washington, DC : ACS Publications, 2020) Nishiguchi, Akihiro; Zhang, Hang; Schweizerhof, Sjören; Schulte, Marie Friederike; Mourran, Ahmed; Möller, MartinThere is a growing interest in the concept of four-dimensional (4D) printing that combines a three-dimensional (3D) manufacturing process with dynamic modulation for bioinspired soft materials exhibiting more complex functionality. However, conventional approaches have drawbacks of low resolution, control of internal micro/nanostructure, and creation of fast, complex actuation due to a lack of high-resolution fabrication technology and suitable photoresist for soft materials. Here, we report an approach of 4D printing that develops a bioinspired soft actuator with a defined 3D geometry and programmed printing density. Multiphoton lithography (MPL) allows for controlling printing density in gels at pixel-by-pixel with a resolution of a few hundreds of nanometers, which tune swelling behaviors of gels in response to external stimuli. We printed a 3D soft actuator composed of thermoresponsive poly(N-isopropylacrylamide) (PNIPAm) and gold nanorods (AuNRs). To improve the resolution of printing, we synthesized a functional, thermoresponsive macrocrosslinker. Through plasmonic heating by AuNRs, nanocomposite-based soft actuators undergo nonequilibrium, programmed, and fast actuation. Light-mediated manufacture and manipulation (MPL and photothermal effect) offer the feasibility of 4D printing toward adaptive bioinspired soft materials. Copyright © 2020 American Chemical Society.
- ItemActively Tunable Collective Localized Surface Plasmons by Responsive Hydrogel Membrane(Weinheim : Wiley-VCH, 2019) Quilis, Nestor Gisbert; van Dongen, Marcel; Venugopalan, Priyamvada; Kotlarek, Daria; Petri, Christian; Cencerrado, Alberto Moreno; Stanescu, Sorin; Herrera, Jose Luis Toca; Jonas, Ulrich; Möller, Martin; Mourran, Ahmed; Dostalek, JakubCollective (lattice) localized surface plasmons (cLSP) with actively tunable and extremely narrow spectral characteristics are reported. They are supported by periodic arrays of gold nanoparticles attached to a stimuli-responsive hydrogel membrane, which can on demand swell and collapse to reversibly modulate arrays period and surrounding refractive index. In addition, it features a refractive index-symmetrical geometry that promotes the generation of cLSPs and leads to strong suppression of radiative losses, narrowing the spectral width of the resonance, and increasing of the electromagnetic field intensity. Narrowing of the cLSP spectral band down to 13 nm and its reversible shifting by up to 151 nm is observed in the near infrared part of the spectrum by varying temperature and by solvent exchange for systems with a poly(N-isopropylacrylamide)-based hydrogel membrane that is allowed to reversibly swell and collapse in either one or in three dimensions. The reported structures with embedded periodic gold nanoparticle arrays are particularly attractive for biosensing applications as the open hydrogel structure can be efficiently post-modified with functional moieties, such as specific ligands, and since biomolecules can rapidly diffuse through swollen polymer networks. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemCellular responses to beating hydrogels to investigate mechanotransduction([London] : Nature Publishing Group UK, 2019) Chandorkar, Yashoda; Castro Nava, Arturo; Schweizerhof, Sjören; Van Dongen, Marcel; Haraszti, Tamás; Köhler, Jens; Zhang, Hang; Windoffer, Reinhard; Mourran, Ahmed; Möller, Martin; De Laporte, LauraCells feel the forces exerted on them by the surrounding extracellular matrix (ECM) environment and respond to them. While many cell fate processes are dictated by these forces, which are highly synchronized in space and time, abnormal force transduction is implicated in the progression of many diseases (muscular dystrophy, cancer). However, material platforms that enable transient, cyclic forces in vitro to recreate an in vivo-like scenario remain a challenge. Here, we report a hydrogel system that rapidly beats (actuates) with spatio-temporal control using a near infra-red light trigger. Small, user-defined mechanical forces (~nN) are exerted on cells growing on the hydrogel surface at frequencies up to 10 Hz, revealing insights into the effect of actuation on cell migration and the kinetics of reversible nuclear translocation of the mechanosensor protein myocardin related transcription factor A, depending on the actuation amplitude, duration and frequency.
- ItemCubosomes from hierarchical self-assembly of poly(ionic liquid) block copolymers([London] : Nature Publishing Group UK, 2017) He, Hongkun; Rahimi, Khosrow; Zhong, Mingjiang; Mourran, Ahmed; Luebke, David R.; Nulwala, Hunaid B.; Möller, Martin; Matyjaszewski, KrzysztofCubosomes are micro- and nanoparticles with a bicontinuous cubic two-phase structure, reported for the self-assembly of low molecular weight surfactants, for example, lipids, but rarely formed by polymers. These objects are characterized by a maximum continuous interface and high interface to volume ratio, which makes them promising candidates for efficient adsorbents and host-guest applications. Here we demonstrate self-assembly to nanoscale cuboidal particles with a bicontinuous cubic structure by amphiphilic poly(ionic liquid) diblock copolymers, poly(acrylic acid)-block-poly(4-vinylbenzyl)-3-butyl imidazolium bis(trifluoromethylsulfonyl)imide, in a mixture of tetrahydrofuran and water under optimized conditions. Structure determining parameters include polymer composition and concentration, temperature, and the variation of the solvent mixture. The formation of the cubosomes can be explained by the hierarchical interactions of the constituent components. The lattice structure of the block copolymers can be transferred to the shape of the particle as it is common for atomic and molecular faceted crystals.
- ItemIn-Gel Direct Laser Writing for 3D-Designed Hydrogel Composites That Undergo Complex Self-Shaping(Weinheim : Wiley-VCH, 2017) Nishiguchi, Akihiro; Mourran, Ahmed; Zhang, Hang; Möller, MartinSelf-shaping and actuating materials inspired by biological system have enormous potential for biosensor, microrobotics, and optics. However, the control of 3D-complex microactuation is still challenging due to the difficulty in design of nonuniform internal stress of micro/nanostructures. Here, we develop in-gel direct laser writing (in-gel DLW) procedure offering a high resolution inscription whereby the two materials, resin and hydrogel, are interpenetrated on a scale smaller than the wavelength of the light. The 3D position and mechanical properties of the inscribed structures could be tailored to a resolution better than 100 nm over a wide density range. These provide an unparalleled means of inscribing a freely suspended microstructures of a second material like a skeleton into the hydrogel body and also to direct isotropic volume changes to bending and distortion motions. In the combination with a thermosensitive hydrogel rather small temperature variations could actuate large amplitude motions. This generates complex modes of motion through the rational engineering of the stresses present in the multicomponent material. More sophisticated folding design would realize a multiple, programmable actuation of soft materials. This method inspired by biological system may offer the possibility for functional soft materials capable of biomimetic actuation and photonic crystal application.
- ItemA Light-Driven Microgel Rotor(Weinheim : Wiley-VCH, 2019) Zhang, Hang; Koens, Lyndon; Lauga, Eric; Mourran, Ahmed; Möller, MartinThe current understanding of motility through body shape deformation of micro-organisms and the knowledge of fluid flows at the microscale provides ample examples for mimicry and design of soft microrobots. In this work, a 2D spiral is presented that is capable of rotating by non-reciprocal curling deformations. The body of the microswimmer is a ribbon consisting of a thermoresponsive hydrogel bilayer with embedded plasmonic gold nanorods. Such a system allows fast local photothermal heating and nonreciprocal bending deformation of the hydrogel bilayer under nonequilibrium conditions. It is shown that the spiral acts as a spring capable of large deformations thanks to its low stiffness, which is tunable by the swelling degree of the hydrogel and the temperature. Tethering the ribbon to a freely rotating microsphere enables rotational motion of the spiral by stroboscopic irradiation. The efficiency of the rotor is estimated using resistive force theory for Stokes flow. This research demonstrates microscopic locomotion by the shape change of a spiral and may find applications in the field of microfluidics, or soft microrobotics.
- ItemMicrogel that swims to the beat of light(Berlin ; Heidelberg : Springer, 2021) Mourran, Ahmed; Jung, Oliver; Vinokur, Rostislav; Möller, MartinComplementary to the quickly advancing understanding of the swimming of microorganisms, we demonstrate rather simple design principles for systems that can mimic swimming by body shape deformation. For this purpose, we developed a microswimmer that could be actuated and controlled by fast temperature changes through pulsed infrared light irradiation. The construction of the microswimmer has the following features: (i) it is a bilayer ribbon with a length of 80 or 120 μm, consisting of a thermo-responsive hydrogel of poly-N-isopropylamide coated with a 2-nm layer of gold and equipped with homogeneously dispersed gold nanorods; (ii) the width of the ribbon is linearly tapered with a wider end of 5 μm and a tip of 0.5 μm; (iii) a thickness of only 1 and 2 μm that ensures a maximum variation of the cross section of the ribbon along its length from square to rectangular. These wedge-shaped ribbons form conical helices when the hydrogel is swollen in cold water and extend to a filament-like object when the temperature is raised above the volume phase transition of the hydrogel at 32∘C. The two ends of these ribbons undergo different but coupled modes of motion upon fast temperature cycling through plasmonic heating of the gel-objects from inside. Proper choice of the IR-light pulse sequence caused the ribbons to move at a rate of 6 body length/s (500 μm/s) with the wider end ahead. Within the confinement of rectangular container of 30 μm height and 300 μm width, the different modes can be actuated in a way that the movement is directed by the energy input between spinning on the spot and fast forward locomotion.
- ItemPolymers Diffusivity Encoded by Stimuli-Induced Phase Transition: Theory and Application to Poly(N-Isopropylacrylamide) with Hydrophilic and Hydrophobic End Groups(Weinheim : Wiley-VCH, 2018) Schweizerhof, Sjören; Demco, Dan Eugen; Mourran, Ahmed; Fechete, Radu; Möller, MartinThe self-diffusion of various nano-objects investigated by high-resolution nuclear magnetic resonance diffusometry proves to be an efficient method for the characterization of dynamics, aggregation kinetic, and matrix morphology. This study investigates how the two-state model and Boltzmann function approach can be used for the evaluation of the thermodynamic parameters of temperature-induced phase transition encoded in polymer diffusivity. The characteristics of the phase transition given by the transition temperature, change of entropy, and width of transition are obtained for poly(N-isopropylacrylamide) (PNIPAm) linear polymers with hydrophilic and hydrophobic end-group functionalization. The effect of end groups upon the polymer diffusivity is investigated as a function of molecular weight (M n), from which fractal dimensions and hydrodynamic drag coefficients are obtained. The PNIPAm diffusivity is affected strongly by the end groups, and it is reflected in the hydrodynamic radius dependence upon molecular weight that obeys different power-law relations. In this study, the synthesis of α-ω-heterotelechelic PNIPAm of different molecular weights with a thiol end group and a hydrophilic NIPAm-like as well as a hydrophobic benzyl end group are described by reversible addition–fragmentation chain-transfer polymerization.
- ItemSoft Microrobots Employing Nonequilibrium Actuation via Plasmonic Heating(Weinheim : Wiley-VCH, 2017) Mourran, Ahmed; Zhang, Hang; Vinokur, Rostislav; Möller, MartinA soft microrobot composed of a microgel and driven by the light-controlled nonequilibrium dynamics of volume changes is presented. The photothermal response of the microgel, containing plasmonic gold nanorods, enables fast heating/cooling dynamics. Mastering the nonequilibrium response provides control of the complex motion, which goes beyond what has been so far reported for hydrophilic microgels.
- ItemStiffness Tomography of Ultra-Soft Nanogels by Atomic Force Microscopy(Weinheim : Wiley-VCH, 2020) Schulte, M. Friederike; Bochenek, Steffen; Brugnoni, Monia; Scotti, Andrea; Mourran, Ahmed; Richtering, WalterThe softness of nanohydrogels results in unique properties and recently attracted tremendous interest due to the multi-functionalization of interfaces. Herein, we study extremely soft temperature-sensitive ultra-low cross-linked (ULC) nanogels adsorbed to the solid/water interface by atomic force microscopy (AFM). The ultra-soft nanogels seem to disappear in classical imaging modes since a sharp tip fully penetrates these porous networks with very low forces in the range of steric interactions (ca. 100 pN). However, the detailed evaluation of Force Volume mode measurements allows us to resolve their overall shape and at the same time their internal structure in all three dimensions. The nanogels exhibit an extraordinary disk-like and entirely homogeneous but extremely soft structure—even softer than polymer brushes. Moreover, the temperature-sensitive nanogels can be switched on demand between the ultra-soft and a very stiff state. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemThe swimming of a deforming helix(Berlin ; Heidelberg : Springer, 2018) Koens, Lyndon; Zhang, Hang; Moeller, Martin; Mourran, Ahmed; Lauga, EricMany microorganisms and artificial microswimmers use helical appendages in order to generate locomotion. Though often rotated so as to produce thrust, some species of bacteria such Spiroplasma, Rhodobacter sphaeroides and Spirochetes induce movement by deforming a helical-shaped body. Recently, artificial devices have been created which also generate motion by deforming their helical body in a non-reciprocal way (A. Mourran et al. Adv. Mater. 29, 1604825, 2017). Inspired by these systems, we investigate the transport of a deforming helix within a viscous fluid. Specifically, we consider a swimmer that maintains a helical centreline and a single handedness while changing its helix radius, pitch and wavelength uniformly across the body. We first discuss how a deforming helix can create a non-reciprocal translational and rotational swimming stroke and identify its principle direction of motion. We then determine the leading-order physics for helices with small helix radius before considering the general behaviour for different configuration parameters and how these swimmers can be optimised. Finally, we explore how the presence of walls, gravity, and defects in the centreline allow the helical device to break symmetries, increase its speed, and generate transport in directions not available to helices in bulk fluids.
- ItemThermodynamic Parameters of Temperature-Induced Phase Transition for Brushes onto Nanoparticles: Hydrophilic versus Hydrophobic End-Groups Functionalization(Weinheim : Wiley-VCH, 2017) Schweizerhof, Sjören; Demco, Dan Eugen; Mourran, Ahmed; Keul, Helmut; Fechete, Radu; Möller, MartinQuantification of the stimuli-responsive phase transition in polymers is topical and important for the understanding and development of novel stimuli-responsive materials. The temperature-induced phase transition of poly(N-isopropylacrylamide) (PNIPAm) with one thiol end group depends on the confinement—free polymer or polymer brush—on the molecular weight and on the nature of the second end. This paper describes the synthesis of heterotelechelic PNIPAm of different molecular weights with a thiol end group—that specifically binds to gold nanorods and a hydrophilic NIPAm end group by reversible addition-fragmentation chain-transfer polymerization. Proton high-resolution magic angle sample spinning NMR spectra are used as an indicator of the polymer chain conformations. The characteristics of phase transition given by the transition temperature, entropy, and width of transition are obtained by a two-state model. The dependence of thermodynamic parameters on molecular weight is compared for hydrophilic and hydrophobic end functional-free polymers and brushes.