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2020


Chiroptical spectroscopy of a freely diffusing single nanoparticle
Chiroptical spectroscopy of a freely diffusing single nanoparticle

Sachs, J., Günther, J., Mark, A. G., Fischer, P.

Nature Communications, 11(4513), September 2020 (article)

Abstract
Chiral plasmonic nanoparticles can exhibit strong chiroptical signals compared to the corresponding molecular response. Observations are, however, generally restricted to measurements on stationary single particles with a fixed orientation, which complicates the spectral analysis. Here, we report the spectroscopic observation of a freely diffusing single chiral nanoparticle in solution. By acquiring time-resolved circular differential scattering signals we show that the spectral interpretation is significantly simplified. We experimentally demonstrate the equivalence between time-averaged chiral spectra observed for an individual nanostructure and the corresponding ensemble spectra, and thereby demonstrate the ergodic principle for chiroptical spectroscopy. We also show how it is possible for an achiral particle to yield an instantaneous chiroptical response, whereas the time-averaged signals are an unequivocal measure of chirality. Time-resolved chiroptical spectroscopy on a freely moving chiral nanoparticle advances the field of single-particle spectroscopy, and is a means to obtain the true signature of the nanoparticle’s chirality.

link (url) DOI [BibTex]


Microchannels with Self-Pumping Walls
Microchannels with Self-Pumping Walls

Yu, T., Athanassiadis, A., Popescu, M., Chikkadi, V., Güth, A., Singh, D., Qiu, T., Fischer, P.

ACS Nano, September 2020 (article)

Abstract
When asymmetric Janus micromotors are immobilized on a surface, they act as chemically powered micropumps, turning chemical energy from the fluid into a bulk flow. However, such pumps have previously produced only localized recirculating flows, which cannot be used to pump fluid in one direction. Here, we demonstrate that an array of three-dimensional, photochemically active Au/TiO2 Janus pillars can pump water. Upon UV illumination, a water-splitting reaction rapidly creates a directional bulk flow above the active surface. By lining a 2D microchannel with such active surfaces, various flow profiles are created within the channels. Analytical and numerical models of a channel with active surfaces predict flow profiles that agree very well with the experimental results. The light-driven active surfaces provide a way to wirelessly pump fluids at small scales and could be used for real-time, localized flow control in complex microfluidic networks.

link (url) DOI [BibTex]


Scalable Fabrication of Molybdenum Disulfide Nanostructures and their Assembly
Scalable Fabrication of Molybdenum Disulfide Nanostructures and their Assembly

Huang, Y., Yu, K., Li, H., Liang, Z., Walker, D., Ferreira, P., Fischer, P., Fan, D.

Adv. Mat., (2003439), September 2020 (article)

Abstract
Molybdenum disulfide (MoS2) is a multifunctional material that can be used for various applications. In the single‐crystalline form, MoS2 shows superior electronic properties. It is also an exceptionally useful nanomaterial in its polycrystalline form with applications in catalysis, energy storage, water treatment, and gas sensing. Here, the scalable fabrication of longitudinal MoS2 nanostructures, i.e., nanoribbons, and their oxide hybrids with tunable dimensions in a rational and well‐reproducible fashion, is reported. The nanoribbons, obtained at different reaction stages, that is, MoO3, MoS2/MoO2 hybrid, and MoS2, are fully characterized. The growth method presented herein has a high yield and is particularly robust. The MoS2 nanoribbons can readily be removed from its substrate and dispersed in solution. It is shown that functionalized MoS2 nanoribbons can be manipulated in solution and assembled in controlled patterns and directly on microelectrodes with UV‐click‐chemistry. Owing to the high chemical purity and polycrystalline nature, the MoS2 nanostructures demonstrate rapid optoelectronic response to wavelengths from 450 to 750 nm, and successfully remove mercury contaminants from water. The scalable fabrication and manipulation followed by light‐directed assembly of MoS2 nanoribbons, and their unique properties, will be inspiring for device fabrication and applications of the transition metal dichalcogenides.

link (url) [BibTex]

link (url) [BibTex]


Spatial ultrasound modulation by digitally controlling microbubble arrays
Spatial ultrasound modulation by digitally controlling microbubble arrays

Ma, Z., Melde, K., Athanassiadis, A. G., Schau, M., Richter, H., Qiu, T., Fischer, P.

Nature Communications, 11(4537), September 2020 (article)

Abstract
Acoustic waves, capable of transmitting through optically opaque objects, have been widely used in biomedical imaging, industrial sensing and particle manipulation. High-fidelity wavefront shaping is essential to further improve performance in these applications. An acoustic analog to the successful spatial light modulator (SLM) in optics would be highly desirable. To date there have been no techniques shown that provide effective and dynamic modulation of a sound wave and which also support scale-up to a high number of individually addressable pixels. In the present study, we introduce a dynamic spatial ultrasound modulator (SUM),which dynamically reshapes incident plane waves into complex acoustic images. Its trans-mission function is set with a digitally generated pattern of microbubbles controlled by a complementary metal–oxide–semiconductor (CMOS) chip, which results in a binary amplitude acoustic hologram. We employ this device to project sequentially changing acoustic images and demonstrate the first dynamic parallel assembly of microparticles using a SUM.

link (url) DOI [BibTex]


Characterization of active matter in dense suspensions with heterodyne laser Doppler velocimetry
Characterization of active matter in dense suspensions with heterodyne laser Doppler velocimetry

Sachs, J., Kottapalli, S. N., Fischer, P., Botin, D., Palberg, T.

Colloid and Polymer Science, August 2020 (article)

Abstract
We present a novel approach for characterizing the properties and performance of active matter in dilute suspension as well as in crowded environments. We use Super-Heterodyne Laser-Doppler-Velocimetry (SH-LDV) to study large ensembles of catalytically active Janus particles moving under UV illumination. SH-LDV facilitates a model-free determination of the swimming speed and direction, with excellent ensemble averaging. In addition, we obtain information on the distribution of the catalytic activity. Moreover, SH-LDV operates away from walls and permits a facile correction for multiple scattering contributions. It thus allows for studies of concentrated suspensions of swimmers or of systems where swimmers propel actively in an environment crowded by passive particles. We demonstrate the versatility and the scope of the method with a few selected examples. We anticipate that SH-LDV complements established methods and paves the way for systematic measurements at previously inaccessible boundary conditions.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Biocompatible magnetic micro‐ and nanodevices: Fabrication of FePt nanopropellers and cell transfection
Biocompatible magnetic micro‐ and nanodevices: Fabrication of FePt nanopropellers and cell transfection

Kadiri, V. M., Bussi, C., Holle, A. W., Son, K., Kwon, H., Schütz, G., Gutierrez, M. G., Fischer, P.

Adv. Mat., 32(2001114), May 2020 (article)

Abstract
The application of nanoparticles for drug or gene delivery promises benefits in the form of single‐cell‐specific therapeutic and diagnostic capabilities. Many methods of cell transfection rely on unspecific means to increase the transport of genetic material into cells. Targeted transport is in principle possible with magnetically propelled micromotors, which allow responsive nanoscale actuation and delivery. However, many commonly used magnetic materials (e.g., Ni and Co) are not biocompatible, possess weak magnetic remanence (Fe3O4), or cannot be implemented in nanofabrication schemes (NdFeB). Here, it is demonstrated that co‐depositing iron (Fe) and platinum (Pt) followed by one single annealing step, without the need for solution processing, yields ferromagnetic FePt nanomotors that are noncytotoxic, biocompatible, and possess a remanence and magnetization that rival those of permanent NdFeB micromagnets. Active cell targeting and magnetic transfection of lung carcinoma cells are demonstrated using gradient‐free rotating millitesla fields to drive the FePt nanopropellers. The carcinoma cells express enhanced green fluorescent protein after internalization and cell viability is unaffected by the presence of the FePt nanopropellers. The results establish FePt, prepared in the L10 phase, as a promising magnetic material for biomedical applications with superior magnetic performance, especially for micro‐ and nanodevices.

link (url) DOI [BibTex]


Interface-mediated spontaneous symmetry breaking and mutual communication between drops containing chemically active particles
Interface-mediated spontaneous symmetry breaking and mutual communication between drops containing chemically active particles

Singh, D., Domínguez, A., Choudhury, U., Kottapalli, S., Popescu, M., Dietrich, S., Fischer, P.

Nature Communications, 11(2210), May 2020 (article)

Abstract
Symmetry breaking and the emergence of self-organized patterns is the hallmark of com- plexity. Here, we demonstrate that a sessile drop, containing titania powder particles with negligible self-propulsion, exhibits a transition to collective motion leading to self-organized flow patterns. This phenomenology emerges through a novel mechanism involving the interplay between the chemical activity of the photocatalytic particles, which induces Mar- angoni stresses at the liquid–liquid interface, and the geometrical confinement provided by the drop. The response of the interface to the chemical activity of the particles is the source of a significantly amplified hydrodynamic flow within the drop, which moves the particles. Furthermore, in ensembles of such active drops long-ranged ordering of the flow patterns within the drops is observed. We show that the ordering is dictated by a chemical com- munication between drops, i.e., an alignment of the flow patterns is induced by the gradients of the chemicals emanating from the active particles, rather than by hydrodynamic interactions.

link (url) DOI [BibTex]


Spectrally selective and highly-sensitive UV photodetection with UV-A, C band specific polarity switching in silver plasmonic nanoparticle enhanced gallium oxide thin-film
Spectrally selective and highly-sensitive UV photodetection with UV-A, C band specific polarity switching in silver plasmonic nanoparticle enhanced gallium oxide thin-film

Arora, K., Singh, D., Fischer, P., Kumar, M.

Adv. Opt. Mat., March 2020 (article)

Abstract
Traditional photodetectors generally show a unipolar photocurrent response when illuminated with light of wavelength equal or shorter than the optical bandgap. Here, we report that a thin film of gallium oxide (GO) decorated with plasmonic nanoparticles, surprisingly, exhibits a change in the polarity of the photocurrent for different UV bands. Silver (Ag) nanoparticles are vacuum-deposited onto β-Ga2O3 and the AgNP@GO thin films show a record responsivity of 250 A/W, which significantly outperforms bare GO planar photodetectors. The photoresponsivity reverses sign from +157 µA/W in the UV-C band under unbiased operation to -353 µA/W in the UV-A band. The current reversal is rationalized by considering the charge dynamics stemming from hot electrons generated when the incident light excites a local surface plasmon resonance (LSPR) in the Ag nanoparticles. The Ag nanoparticles improve the external quantum efficiency and detectivity by nearly one order of magnitude with high values of 1.2×105 and 3.4×1014 Jones, respectively. This plasmon-enhanced solar blind GO detector allows UV regions to be spectrally distinguished, which is useful for the development of sensitive dynamic imaging photodetectors.

link (url) DOI [BibTex]


Investigating photoresponsivity of graphene-silver hybrid nanomaterials in the ultraviolet
Investigating photoresponsivity of graphene-silver hybrid nanomaterials in the ultraviolet

Deshpande, P., Suri, P., Jeong, H., Fischer, P., Ghosh, A., Ghosh, G.

J. Chem. Phys., 152, pages: 044709, January 2020 (article)

Abstract
There have been several reports of plasmonically enhanced graphene photodetectors in the visible and the near infrared regime but rarely in the ultraviolet. In a previous work, we have reported that a graphene-silver hybrid structure shows a high photoresponsivity of 13 A/W at 270 nm. Here, we consider the likely mechanisms that underlie this strong photoresponse. We investigate the role of the plasmonic layer and examine the response using silver and gold nanoparticles of similar dimensions and spatial arrangement. The effect on local doping, strain, and absorption properties of the hybrid is also probed by photocurrent measurements and Raman and UV-visible spectroscopy. We find that the local doping from the silver nanoparticles is stronger than that from gold and correlates with a measured photosensitivity that is larger in devices with a higher contact area between the plasmonic nanomaterials and the graphene layer.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


A High-Fidelity Phantom for the Simulation and Quantitative Evaluation of Transurethral Resection of the Prostate
A High-Fidelity Phantom for the Simulation and Quantitative Evaluation of Transurethral Resection of the Prostate

Choi, E., Adams, F., Gengenbacher, A., Schlager, D., Palagi, S., Müller, P., Wetterauer, U., Miernik, A., Fischer, P., Qiu, T.

Annals of Biomed. Eng., 48, pages: 437-446, January 2020 (article)

Abstract
Transurethral resection of the prostate (TURP) is a minimally invasive endoscopic procedure that requires experience and skill of the surgeon. To permit surgical training under realistic conditions we report a novel phantom of the human prostate that can be resected with TURP. The phantom mirrors the anatomy and haptic properties of the gland and permits quantitative evaluation of important surgical performance indicators. Mixtures of soft materials are engineered to mimic the physical properties of the human tissue, including the mechanical strength, the electrical and thermal conductivity, and the appearance under an endoscope. Electrocautery resection of the phantom closely resembles the procedure on human tissue. Ultrasound contrast agent was applied to the central zone, which was not detectable by the surgeon during the surgery but showed high contrast when imaged after the surgery, to serve as a label for the quantitative evaluation of the surgery. Quantitative criteria for performance assessment are established and evaluated by automated image analysis. We present the workflow of a surgical simulation on a prostate phantom followed by quantitative evaluation of the surgical performance. Surgery on the phantom is useful for medical training, and enables the development and testing of endoscopic and minimally invasive surgical instruments.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Interactive Materials – Drivers of Future Robotic Systems
Interactive Materials – Drivers of Future Robotic Systems

Fischer, P.

Adv. Mat., January 2020 (article)

Abstract
A robot senses its environment, processes the sensory information, acts in response to these inputs, and possibly communicates with the outside world. Robots generally achieve these tasks with electronics-based hardware or by receiving inputs from some external hardware. In contrast, simple microorganisms can autonomously perceive, act, and communicate via purely physicochemical processes in soft material systems. A key property of biological systems is that they are built from energy-consuming ‘active’ units. Exciting developments in material science show that even very simple artificial active building blocks can show surprisingly rich emergent behaviors. Active non-equilibrium systems are therefore predicted to play an essential role to realize interactive materials. A major challenge is to find robust ways to couple and integrate the energy-consuming building blocks to the mechanical structure of the material. However, success in this endeavor will lead to a new generation of sophisticated micro- and soft-robotic systems that can operate autonomously.

link (url) DOI [BibTex]

2019


Soft-magnetic coatings as possible sensors for magnetic imaging of superconductors
Soft-magnetic coatings as possible sensors for magnetic imaging of superconductors

Ionescu, A., Simmendinger, J., Bihler, M., Miksch, C., Fischer, P., Soltan, S., Schütz, G., Albrecht, J.

Supercond. Sci. and Tech., 33, pages: 015002, IOP, December 2019 (article)

Abstract
Magnetic imaging of superconductors typically requires a soft-magnetic material placed on top of the superconductor to probe local magnetic fields. For reasonable results the influence of the magnet onto the superconductor has to be small. Thin YBCO films with soft-magnetic coatings are investigated using SQUID magnetometry. Detailed measurements of the magnetic moment as a function of temperature, magnetic field and time have been performed for different heterostructures. It is found that the modification of the superconducting transport in these heterostructures strongly depends on the magnetic and structural properties of the soft-magnetic material. This effect is especially pronounced for an inhomogeneous coating consisting of ferromagnetic nanoparticles.

link (url) DOI [BibTex]

2019

link (url) DOI [BibTex]


HPLC of monolayer-protected Gold clusters with baseline separation
HPLC of monolayer-protected Gold clusters with baseline separation

Knoppe, S., Vogt, P.

Analytical Chemistry, 91, pages: 1603, December 2019 (article)

Abstract
The properties of ultrasmall metal nanoparticles (ca. 10–200 metal atoms), or monolayer-protected metal clusters (MPCs), drastically depend on their atomic structure. For systematic characterization and application, assessment of their purity is of high importance. Currently, the gold standard for purity control of MPCs is mass spectrometry (MS). Mass spectrometry, however, cannot always detect small impurities; MS of certain clusters, for example, ESI-TOF of Au40(SR)24, is not successful at all. We here present a simple reversed-phase HPLC method for purity control of a series of small alkanethiolate-protected gold clusters. The method allows the detection of small impurities with high sensitivity. Linear correlation between alkyl chain length of Au25(SC_n H_(2n+1))18 clusters (n = 6, 8, 10, 12) and their retention time was noticed.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Acoustic hologram enhanced phased arrays for ultrasonic particle manipulation
Acoustic hologram enhanced phased arrays for ultrasonic particle manipulation

Cox, L., Melde, K., Croxford, A., Fischer, P., Drinkwater, B.

Phys. Rev. Applied, 12, pages: 064055, November 2019 (article)

Abstract
The ability to shape ultrasound fields is important for particle manipulation, medical therapeutics and imaging applications. If the amplitude and/or phase is spatially varied across the wavefront then it is possible to project ‘acoustic images’. When attempting to form an arbitrary desired static sound field, acoustic holograms are superior to phased arrays due to their significantly higher phase fidelity. However, they lack the dynamic flexibility of phased arrays. Here, we demonstrate how to combine the high-fidelity advantages of acoustic holograms with the dynamic control of phased arrays in the ultrasonic frequency range. Holograms are used with a 64-element phased array, driven with continuous excitation. Moving the position of the projected hologram via phase delays which steer the output beam is demonstrated experimentally. This allows the creation of a much more tightly focused point than with the phased array alone, whilst still being reconfigurable. It also allows the complex movement at a water-air interface of a “phase surfer” along a phase track or the manipulation of a more arbitrarily shaped particle via amplitude traps. Furthermore, a particle manipulation device with two emitters and a single split hologram is demonstrated that allows the positioning of a “phase surfer” along a 1D axis. This paper opens the door for new applications with complex manipulation of ultrasound whilst minimising the complexity and cost of the apparatus.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


A Helical Microrobot with an Optimized Propeller-Shape for Propulsion in Viscoelastic Biological Media
A Helical Microrobot with an Optimized Propeller-Shape for Propulsion in Viscoelastic Biological Media

Li., D., Jeong, M., Oren, E., Yu, T., Qiu, T.

Robotics, 8, pages: 87, MDPI, October 2019 (article)

Abstract
One major challenge for microrobots is to penetrate and effectively move through viscoelastic biological tissues. Most existing microrobots can only propel in viscous liquids. Recent advances demonstrate that sub-micron robots can actively penetrate nanoporous biological tissue, such as the vitreous of the eye. However, it is still difficult to propel a micron-sized device through dense biological tissue. Here, we report that a special twisted helical shape together with a high aspect ratio in cross-section permit a microrobot with a diameter of hundreds-of-micrometers to move through mouse liver tissue. The helical microrobot is driven by a rotating magnetic field and localized by ultrasound imaging inside the tissue. The twisted ribbon is made of molybdenum and a sharp tip is chemically etched to generate a higher pressure at the edge of the propeller to break the biopolymeric network of the dense tissue.

link (url) DOI [BibTex]


Acoustic Holographic Cell Patterning in a Biocompatible Hydrogel
Acoustic Holographic Cell Patterning in a Biocompatible Hydrogel

Ma, Z., Holle, A., Melde, K., Qiu, T., Poeppel, K., Kadiri, V., Fischer, P.

Adv. Mat., 32(1904181), October 2019 (article)

Abstract
Acoustophoresis is promising as a rapid, biocompatible, non-contact cell manipulation method, where cells are arranged along the nodes or antinodes of the acoustic field. Typically, the acoustic field is formed in a resonator, which results in highly symmetric regular patterns. However, arbitrary, non-symmetrically shaped cell assemblies are necessary to obtain the irregular cellular arrangements found in biological tissues. We show that arbitrarily shaped cell patterns can be obtained from the complex acoustic field distribution defined by an acoustic hologram. Attenuation of the sound field induces localized acoustic streaming and the resultant convection flow gently delivers the suspended cells to the image plane where they form the designed pattern. We show that the process can be implemented in a biocompatible collagen solution, which can then undergo gelation to immobilize the cell pattern inside the viscoelastic matrix. The patterned cells exhibit F-actin-based protrusions, which indicates that the cells grow and thrive within the matrix. Cell viability assays and brightfield imaging after one week confirm cell survival and that the patterns persist. Acoustophoretic cell manipulation by holographic fields thus holds promise for non-contact, long-range, long-term cellular pattern formation, with a wide variety of potential applications in tissue engineering and mechanobiology.

link (url) DOI [BibTex]


Arrays of plasmonic nanoparticle dimers with defined nanogap spacers
Arrays of plasmonic nanoparticle dimers with defined nanogap spacers

Jeong, H., Adams, M. C., Guenther, J., Alarcon-Correa, M., Kim, I., Choi, E., Miksch, C., Mark, A. F. M., Mark, A. G., Fischer, P.

ACS Nano, 13, pages: 11453-11459, September 2019 (article)

Abstract
Plasmonic molecules are building blocks of metallic nanostructures that give rise to intriguing optical phenomena with similarities to those seen in molecular systems. The ability to design plasmonic hybrid structures and molecules with nanometric resolution would enable applications in optical metamaterials and sensing that presently cannot be demonstrated, because of a lack of suitable fabrication methods allowing the structural control of the plasmonic atoms on a large scale. Here we demonstrate a wafer-scale “lithography-free” parallel fabrication scheme to realize nanogap plasmonic meta-molecules with precise control over their size, shape, material, and orientation. We demonstrate how we can tune the corresponding coupled resonances through the entire visible spectrum. Our fabrication method, based on glancing angle physical vapor deposition with gradient shadowing, permits critical parameters to be varied across the wafer and thus is ideally suited to screen potential structures. We obtain billions of aligned dimer structures with controlled variation of the spectral properties across the wafer. We spectroscopically map the plasmonic resonances of gold dimer structures and show that they not only are in good agreement with numerically modeled spectra, but also remain functional, at least for a year, in ambient conditions.

link (url) DOI [BibTex]


Genetically modified M13 bacteriophage nanonets for enzyme catalysis and recovery
Genetically modified M13 bacteriophage nanonets for enzyme catalysis and recovery

Kadiri, V. M., Alarcon-Correa, M., Guenther, J. P., Ruppert, J., Bill, J., Rothenstein, D., Fischer, P.

Catalysts, 9, pages: 723, August 2019 (article)

Abstract
Enzyme-based biocatalysis exhibits multiple advantages over inorganic catalysts, including the biocompatibility and the unchallenged specificity of enzymes towards their substrate. The recovery and repeated use of enzymes is essential for any realistic application in biotechnology, but is not easily achieved with current strategies. For this purpose, enzymes are often immobilized on inorganic scaffolds, which could entail a reduction of the enzymes’ activity. Here, we show that immobilization to a nano-scaled biological scaffold, a nanonetwork of end-to-end cross-linked M13 bacteriophages, ensures high enzymatic activity and at the same time allows for the simple recovery of the enzymes. The bacteriophages have been genetically engineered to express AviTags at their ends, which permit biotinylation and their specific end-to-end self-assembly while allowing space on the major coat protein for enzyme coupling. We demonstrate that the phages form nanonetwork structures and that these so-called nanonets remain highly active even after re-using the nanonets multiple times in a flow-through reactor.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Light-controlled micromotors and soft microrobots
Light-controlled micromotors and soft microrobots

Palagi, S., Singh, D. P., Fischer, P.

Adv. Opt. Mat., 7, pages: 1900370, August 2019 (article)

Abstract
Mobile microscale devices and microrobots can be powered by catalytic reactions (chemical micromotors) or by external fields. This report is focused on the role of light as a versatile means for wirelessly powering and controlling such microdevices. Recent advances in the development of autonomous micromotors are discussed, where light permits their actuation with unprecedented control and thereby enables advances in the field of active matter. In addition, structuring the light field is a new means to drive soft microrobots that are based on (photo‐) responsive polymers. The behavior of the two main classes of thermo‐ and photoresponsive polymers adopted in microrobotics (poly(N‐isopropylacrylamide) and liquid‐crystal elastomers) is analyzed, and recent applications are reported. The advantages and limitations of controlling micromotors and microrobots by light are reviewed, and some of the remaining challenges in the development of novel photo‐active materials for micromotors and microrobots are discussed.

link (url) DOI [BibTex]


Superior Magnetic Performance in FePt L1_0 Nanomaterials
Superior Magnetic Performance in FePt L1_0 Nanomaterials

Son, K., Ryu, G. H., Jeong, H., Fink, L., Merz, M., Nagel, P., Schuppler, S., Richter, G., Goering, E., Schütz, G.

Small, 15(1902353), July 2019 (article)

Abstract
The discovery of the high maximum energy product of 59 MGOe for NdFeB magnets is a breakthrough in the development of permanent magnets with a tremendous impact in many fields of technology. This value is still the world record, for 40 years. This work reports on a reliable and robust route to realize nearly perfectly ordered L1_0-phase FePt nanoparticles, leading to an unprecedented energy product of 80 MGOe at room temperature. Furthermore, with a 3 nm Au coverage, the magnetic polarization of these nanomagnets can be enhanced by 25% exceeding 1.8 T. This exceptional magnetization and anisotropy is confirmed by using multiple imaging and spectroscopic methods, which reveal highly consistent results. Due to the unprecedented huge energy product, this material can be envisaged as a new advanced basic magnetic component in modern micro and nanosized devices.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Recent advances in gold nanoparticles forbiomedical applications: from hybrid structuresto multi-functionality
Recent advances in gold nanoparticles forbiomedical applications: from hybrid structuresto multi-functionality

Jeong, H., Choi, E., Ellis, E., Lee, T.

J. of Mat. Chem. B, 7, pages: 3480, May 2019 (article)

Abstract
Gold nanoparticles (Au NPs) are arguably the most versatile nanomaterials reported to date. Recentadvances in nanofabrication and chemical synthesis have expanded the scope of Au NPs from classicalhomogeneous nanospheres to a wide range of hybrid nanostructures with programmable size, shapeand composition. Novel physiochemical properties can be achievedviadesign and engineering of thehybrid nanostructures. In this review we discuss the recent progress in the development of complexhybrid Au NPs and propose a classification framework based on three fundamental structuraldimensions (length scale, complexity and symmetry) to aid categorising, comparing and designingvarious types of Au NPs. Their novel functions and potential for biomedical applications will also bediscussed, featuring point-of-care diagnostics by advanced optical spectroscopy and assays, as well asminimally invasive surgeries and targeted drug delivery using multifunctional nano-robot

link (url) DOI [BibTex]


Self-Assembled Phage-Based Colloids for High Localized Enzymatic Activity
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, 13, pages: 5810–5815, 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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Absolute diffusion measurements of active enzyme solutions by NMR
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.

link (url) DOI [BibTex]


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

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

Adv. Mat., 31(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.

link (url) DOI [BibTex]


First Observation of Optical Activity in Hyper-Rayleigh Scattering
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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]

2018


Role of symmetry in driven propulsion at low Reynolds number
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.

link (url) DOI Project Page [BibTex]

2018

link (url) DOI Project Page [BibTex]


Optical and Thermophoretic Control of Janus Nanopen Injection into Living Cells
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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


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

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

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


Nanoscale robotic agents in biological fluids and tissues
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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Fast spatial scanning of 3D ultrasound fields via thermography
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.

link (url) DOI Project Page [BibTex]


Diffusion Measurements of Swimming Enzymes with Fluorescence Correlation Spectroscopy
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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


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

link (url) DOI [BibTex]

link (url) DOI [BibTex]


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

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Chemotaxis of Active Janus Nanoparticles
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.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Bioinspired microrobots
Bioinspired microrobots

Palagi, S., Fischer, P.

Nature Reviews Materials, 3, pages: 113–124, May 2018 (article)

Abstract
Microorganisms can move in complex media, respond to the environment and self-organize. The field of microrobotics strives to achieve these functions in mobile robotic systems of sub-millimetre size. However, miniaturization of traditional robots and their control systems to the microscale is not a viable approach. A promising alternative strategy in developing microrobots is to implement sensing, actuation and control directly in the materials, thereby mimicking biological matter. In this Review, we discuss design principles and materials for the implementation of robotic functionalities in microrobots. We examine different biological locomotion strategies, and we discuss how they can be artificially recreated in magnetic microrobots and how soft materials improve control and performance. We show that smart, stimuli-responsive materials can act as on-board sensors and actuators and that ‘active matter’ enables autonomous motion, navigation and collective behaviours. Finally, we provide a critical outlook for the field of microrobotics and highlight the challenges that need to be overcome to realize sophisticated microrobots, which one day might rival biological machines.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Graphene-silver hybrid devices for sensitive photodetection in the ultraviolet
Graphene-silver hybrid devices for sensitive photodetection in the ultraviolet

Paria, D., Jeong, H. H., Vadakkumbatt, V., Deshpande, P., Fischer, P., Ghosh, A., Ghosh, A.

Nanoscale, 10, pages: 7685-7693, April 2018 (article)

Abstract
The weak light-matter interaction in graphene can be enhanced with a number of strategies, among which sensitization with plasmonic nanostructures is particularly attractive. This has resulted in the development of graphene-plasmonic hybrid systems with strongly enhanced photodetection efficiencies in the visible and the IR, but none in the UV. Here, we describe a silver nanoparticle-graphene stacked optoelectronic device that shows strong enhancement of its photoresponse across the entire UV spectrum. The device fabrication strategy is scalable and modular. Self-assembly techniques are combined with physical shadow growth techniques to fabricate a regular large-area array of 50 nm silver nanoparticles onto which CVD graphene is transferred. The presence of the silver nanoparticles resulted in a plasmonically enhanced photoresponse as high as 3.2 A W-1 in the wavelength range from 330 nm to 450 nm. At lower wavelengths, close to the Van Hove singularity of the density of states in graphene, we measured an even higher responsivity of 14.5 A W-1 at 280 nm, which corresponds to a more than 10 000-fold enhancement over the photoresponse of native graphene.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Nanoparticles on the move for medicine
Nanoparticles on the move for medicine

Fischer, P.

Physics World Focus on Nanotechnology, pages: 26028, (Editors: Margaret Harris), IOP Publishing Ltd and individual contributors, April 2018 (article)

Abstract
Peer Fischer outlines the prospects for creating “nanoswimmers” that can be steered through the body to deliver drugs directly to their targets Molecules don’t move very fast on their own. If they had to rely solely on diffusion – a slow and inefficient process linked to the Brownian motion of small particles and molecules in solution – then a protein mole­cule, for instance, would take around three weeks to travel a single centimetre down a nerve fibre. This is why active transport mechanisms exist in cells and in the human body: without them, all the processes of life would happen at a pace that would make snails look speedy.

link (url) [BibTex]

link (url) [BibTex]


Photogravitactic Microswimmers
Photogravitactic Microswimmers

Singh, D. P., Uspal, W. E., Popescu, M. N., Wilson, L. G., Fischer, P.

Adv. Func. Mat., 28, pages: 1706660, Febuary 2018 (article)

Abstract
Abstract Phototactic microorganisms are commonly observed to respond to natural sunlight by swimming upward against gravity. This study demonstrates that synthetic photochemically active microswimmers can also swim against gravity. The particles initially sediment and, when illuminated at low light intensities exhibit wall‐bound states of motion near the bottom surface. Upon increasing the intensity of light, the artificial swimmers lift off from the wall and swim against gravity and away from the light source. This motion in the bulk has been further confirmed using holographic microscopy. A theoretical model is presented within the framework of self‐diffusiophoresis, which allows to unequivocally identify the photochemical activity and the phototactic response as key mechanisms in the observed phenomenology. Since the lift‐off threshold intensity depends on the particle size, it can be exploited to selectively address particles with the same density from a polydisperse mixture of active particles and move them in or out of the boundary region. This study provides a simple design strategy to fabricate artificial microswimmers whose two‐ or three‐dimensional swimming behavior can be controlled with light.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Chiral Plasmonic Hydrogen Sensors
Chiral Plasmonic Hydrogen Sensors

Matuschek, M., Singh, D. P., Hyeon-Ho, J., Nesterov, M., Weiss, T., Fischer, P., Neubrech, F., Na Liu, L.

Small, 14(7):1702990, Febuary 2018 (article)

Abstract
In this article, a chiral plasmonic hydrogen‐sensing platform using palladium‐based nanohelices is demonstrated. Such 3D chiral nanostructures fabricated by nanoglancing angle deposition exhibit strong circular dichroism both experimentally and theoretically. The chiroptical properties of the palladium nanohelices are altered upon hydrogen uptake and sensitively depend on the hydrogen concentration. Such properties are well suited for remote and spark‐free hydrogen sensing in the flammable range. Hysteresis is reduced, when an increasing amount of gold is utilized in the palladium‐gold hybrid helices. As a result, the linearity of the circular dichroism in response to hydrogen is significantly improved. The chiral plasmonic sensor scheme is of potential interest for hydrogen‐sensing applications, where good linearity and high sensitivity are required.

link (url) DOI [BibTex]

link (url) DOI [BibTex]


Acoustic Fabrication via the Assembly and Fusion of Particles
Acoustic Fabrication via the Assembly and Fusion of Particles

Melde, K., Choi, E., Wu, Z., Palagi, S., Qiu, T., Fischer, P.

Advanced Materials, 30(3):1704507, January 2018 (article)

Abstract
Acoustic assembly promises a route toward rapid parallel fabrication of whole objects directly from solution. This study reports the contact-free and maskless assembly, and fixing of silicone particles into arbitrary 2D shapes using ultrasound fields. Ultrasound passes through an acoustic hologram to form a target image. The particles assemble from a suspension along lines of high pressure in the image due to acoustic radiation forces and are then fixed (crosslinked) in a UV-triggered reaction. For this, the particles are loaded with a photoinitiator by solvent-induced swelling. This localizes the reaction and allows the bulk suspension to be reused. The final fabricated parts are mechanically stable and self-supporting.

link (url) DOI Project Page [BibTex]


The grand challenges of Science Robotics
The grand challenges of Science Robotics

Yang, G., Bellingham, J., Dupont, P., Fischer, P., Floridi, L., Full, R., Jacobstein, N., Kumar, V., McNutt, M., Merrifield, R., Nelson, B., Scassellati, B., Taddeo, M., Taylor, R., Veloso, M., Wang, Z. L., Wood, R.

Science Robotics, 3(eaar7650), January 2018 (article)

Abstract
One of the ambitions of Science Robotics is to deeply root robotics research in science while developing novel robotic platforms that will enable new scientific discoveries. Of our 10 grand challenges, the first 7 represent underpinning technologies that have a wider impact on all application areas of robotics. For the next two challenges, we have included social robotics and medical robotics as application-specific areas of development to highlight the substantial societal and health impacts that they will bring. Finally, the last challenge is related to responsible innovation and how ethics and security should be carefully considered as we develop the technology further.

link (url) DOI [BibTex]

link (url) DOI [BibTex]

2001


Isotropic second-order nonlinear optical susceptibilities
Isotropic second-order nonlinear optical susceptibilities

Fischer, P., Buckingham, A., Albrecht, A.

PHYSICAL REVIEW A, 64(5), 2001 (article)

Abstract
The second-order nonlinear optical susceptibility, in the electric dipole approximation, is only nonvanishing for materials that are noncentrosymmetric. Should the medium be isotropic, then only a chiral system. such as an optically active liquid, satisfies this symmetry requirement. We derive the quantum-mechanical form of the isotropic component of the sum- and difference-frequency susceptibility and discuss its unusual spectral properties. We show that any coherent second-order nonlinear optical process in a system of randomly oriented molecules requires the medium to be chiral. and the incident frequencies to be different and nonzero. Furthermore, a minimum of two nondegenerate excited molecular states are needed for the isotropic part of the susceptibility to be nonvanishing. The rotationally invariant susceptibility is zero in the static field limit and shows exceptionally sensitive resonance and dephasing effects that are particular to chiral centers.

DOI [BibTex]

2001

DOI [BibTex]


Reply to ``Comment on `Phenomenological damping in optical response tensors'{''}
Reply to “Comment on ‘Phenomenological damping in optical response tensors’”

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 63(4), 2001 (article)

Abstract
We show that damping factors must not be incorporated in the perturbation of the ground state by a static electric field. If they are included, as in the theory of Stedman et al. {[}preceding Comment. Phys. Rev. A 63, 047801 (2001)], then there would be an electric dipole in the y direction induced in a hydrogen atom in the M-s = + 1/2 state by a static electric field in the x direction. Such a dipole is excluded by symmetry.

DOI [BibTex]

2000


Phenomenological damping in optical response tensors
Phenomenological damping in optical response tensors

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 61(3), 2000 (article)

Abstract
Although perturbation theory applied to the optical response of a molecule or material system is only strictly valid far from resonances, it is often applied to ``near-resonance{''} conditions by means of complex energies incorporating damping. Inconsistent signs of the damping in optical response tensors have appeared in the recent literature, as have errors in the treatment of the perturbation by a static held. The ``equal-sign{''} convention used in a recent publication yields an unphysical material response, and Koroteev's intimation that linear electro-optical circular dichroism may exist in an optically active liquid under resonance conditions is also flawed. We show that the isotropic part of the Pockels tensor vanishes.

DOI [BibTex]

2000

DOI [BibTex]


Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules
Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules

Champagne, B., Fischer, P., Buckingham, A.

CHEMICAL PHYSICS LETTERS, 331(1):83-88, 2000 (article)

Abstract
Using a sum-over-states procedure based on configuration interaction singles /6-311++G{*}{*}, we have computed the sum-frequency hyperpolarizability beta (ijk)(-3 omega; 2 omega, omega) Of two small chiral molecules, R-monofluoro-oxirane and R-(+)-propylene oxide. Excitation energies were scaled to fit experimental UV-absorption data and checked with ab initio values from time-dependent density functional theory. The isotropic part of the computed hyperpolarizabilities, beta(-3 omega; 2 omega, omega), is much smaller than that reported previously from sum-frequency generation experiments on aqueous solutions of arabinose. Comparison is made with a single-centre chiral model. (C) 2000 Elsevier Science B.V. All rights reserved.

DOI [BibTex]

DOI [BibTex]


Three-wave mixing in chiral liquids
Three-wave mixing in chiral liquids

Fischer, P., Wiersma, D., Righini, R., Champagne, B., Buckingham, A.

PHYSICAL REVIEW LETTERS, 85(20):4253-4256, 2000 (article)

Abstract
Second-order nonlinear optical frequency conversion in isotropic systems is only dipole allowed for sum- and difference-frequency generation in chiral media. We develop a single-center chiral model of the three-wave mixing (sum:frequency generation) nonlinearity and estimate its magnitude. We also report results from ab initio calculations and from three- and four-wave mixing experiments in support of the theoretical estimates. We show that the second-order susceptibility in chiral liquids is much smaller than previously thought.

DOI [BibTex]

DOI [BibTex]