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2020


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.

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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.

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[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.

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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.

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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.

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link (url) DOI [BibTex]

2013


Hybrid nanocolloids with programmed three-dimensional shape and material composition
Hybrid nanocolloids with programmed three-dimensional shape and material composition

Mark, A. G., Gibbs, J. G., Lee, T., Fischer, P.

NATURE MATERIALS, 12(9):802-807, 2013, Max Planck Press Release. (article)

Abstract
Tuning the optical(1,2), electromagnetic(3,4) and mechanical properties of a material requires simultaneous control over its composition and shape(5). This is particularly challenging for complex structures at the nanoscale because surface-energy minimization generally causes small structures to be highly symmetric(5). Here we combine low-temperature shadow deposition with nanoscale patterning to realize nanocolloids with anisotropic three-dimensional shapes, feature sizes down to 20 nm and a wide choice of materials. We demonstrate the versatility of the fabrication scheme by growing three-dimensional hybrid nanostructures that contain several functional materials with the lowest possible symmetry, and by fabricating hundreds of billions of plasmonic nanohelices, which we use as chiral metafluids with record circular dichroism and tunable chiroptical properties.

Max Planck Press Release.

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Video - Fabrication of Designer Nanostructures DOI [BibTex]


Chiral Colloidal Molecules And Observation of The Propeller Effect
Chiral Colloidal Molecules And Observation of The Propeller Effect

Schamel, D., Pfeifer, M., Gibbs, J. G., Miksch, B., Mark, A. G., Fischer, P.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 135(33):12353-12359, 2013 (article)

Abstract
Chiral molecules play an important role in biological and chemical processes, but physical effects due to their symmetry-breaking are generally weak. Several physical chiral separation schemes which could potentially be useful, including the propeller effect, have therefore not yet been demonstrated at the molecular scale. However, it has been proposed that complex nonspherical colloidal particles could act as ``colloidal molecules{''} in mesoscopic model systems to permit the visualization of molecular phenomena that are otherwise difficult to observe. Unfortunately, it is difficult to synthesize such colloids because surface minimization generally favors the growth of symmetric particles. Here we demonstrate the production of large numbers of complex colloids with glancing angle physical vapor deposition. We use chiral colloids to demonstrate the Baranova and Zel'dovich (Baranova, N. B.; Zel'dovich, B. Y. Chem. Phys. Lett. 1978, 57, 435) propeller effect: the separation of a racemic mixture by application of a rotating field that couples to the dipole moment of the enantiomers and screw propels them in opposite directions. The handedness of the colloidal suspensions is monitored with circular differential light scattering. An exact solution for the colloid's propulsion is derived, and comparisons between the colloidal system and the corresponding effect at the molecular scale are made.

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Video - Nanospropellers DOI [BibTex]

Video - Nanospropellers DOI [BibTex]


Indirect absorption spectroscopy using quantum cascade lasers: mid-infrared refractometry and photothermal spectroscopy
Indirect absorption spectroscopy using quantum cascade lasers: mid-infrared refractometry and photothermal spectroscopy

Pfeifer, M., Ruf, A., Fischer, P.

OPTICS EXPRESS, 21(22):25643-25654, 2013 (article)

Abstract
We record vibrational spectra with two indirect schemes that depend on the real part of the index of refraction: mid-infrared refractometry and photothermal spectroscopy. In the former, a quantum cascade laser (QCL) spot is imaged to determine the angles of total internal reflection, which yields the absorption line via a beam profile analysis. In the photothermal measurements, a tunable QCL excites vibrational resonances of a molecular monolayer, which heats the surrounding medium and changes its refractive index. This is observed with a probe laser in the visible. Sub-monolayer sensitivities are demonstrated. (C) 2013 Optical Society of America

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DOI [BibTex]


Plasmonic nanohelix metamaterials with tailorable giant circular dichroism
Plasmonic nanohelix metamaterials with tailorable giant circular dichroism

Gibbs, J. G., Mark, A. G., Eslami, S., Fischer, P.

APPLIED PHYSICS LETTERS, 103(21), 2013, Featured cover article. (article)

Abstract
Plasmonic nanohelix arrays are shown to interact with electromagnetic fields in ways not typically seen with ordinary matter. Chiral metamaterials (CMMs) with feature sizes small with respect to the wavelength of visible light are a promising route to experimentally achieve such phenomena as negative refraction without the need for simultaneously negative e and mu. Here we not only show that giant circular dichroism in the visible is achievable with hexagonally arranged plasmonic nanohelix arrays, but that we can precisely tune the optical activity via morphology and lattice spacing. The discrete dipole approximation is implemented to support experimental data. (C) 2013 AIP Publishing LLC.

Featured cover article.

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DOI [BibTex]

DOI [BibTex]

2010


Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field
Molecular QED of coherent and incoherent sum-frequency and second-harmonic generation in chiral liquids in the presence of a static electric field

Fischer, P., Salam, A.

MOLECULAR PHYSICS, 108(14):1857-1868, 2010 (article)

Abstract
Coherent second-order nonlinear optical processes are symmetry forbidden in centrosymmetric environments in the electric-dipole approximation. In liquids that contain chiral molecules, however, and which therefore lack mirror image symmetry, coherent sum-frequency generation is possible, whereas second-harmonic generation remains forbidden. Here we apply the theory of molecular quantum electrodynamics to the calculation of the matrix element, transition rate, and integrated signal intensity for sum-frequency and second-harmonic generation taking place in a chiral liquid in the presence and absence of a static electric field, to examine which coherent and incoherent processes exist in the electric-dipole approximation in liquids. Third- and fourth-order time-dependent perturbation theory is employed in combination with single-sided Feynman diagrams to evaluate two contributions arising from static field-free and field-induced processes. It is found that, in addition to the coherent term, an incoherent process exists for sum-frequency generation in liquids. Surprisingly, in the case of dc-field-induced second-harmonic generation, the incoherent contribution is found to always vanish for isotropic chiral liquids even though hyper-Rayleigh second-harmonic generation and electric-field-induced second-harmonic generation are both independently symmetry allowed in any liquid.

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DOI [BibTex]

2009


Full phase and amplitude control in computer-generated holography
Full phase and amplitude control in computer-generated holography

Fratz, M., Fischer, P., Giel, D. M.

OPTICS LETTERS, 34(23):3659-3661, 2009 (article)

Abstract
We report what we believe to be the first realization of a computer-generated complex-valued hologram recorded in a single film of photoactive polymer. Complex-valued holograms give rise to a diffracted optical field with control over its amplitude and phase. The holograms are generated by a one-step direct laser writing process in which a spatial light modulator (SLM) is imaged onto a polymer film. Temporal modulation of the SLM during exposure controls both the strength of the induced birefringence and the orientation of the fast axis. We demonstrate that complex holograms can be used to impart arbitrary amplitude and phase profiles onto a beam and thereby open new possibilities in the control of optical beams. (C) 2009 Optical Society of America

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[BibTex]

2009


[BibTex]


Digital polarization holograms with defined magnitude and orientation of each pixel's birefringence
Digital polarization holograms with defined magnitude and orientation of each pixel’s birefringence

Fratz, M., Giel, D. M., Fischer, P.

OPTICS LETTERS, 34(8):1270-1272, 2009 (article)

Abstract
A new form of digital polarization holography is demonstrated that permits both the amplitude and the phase of a diffracted beam to be independently controlled. This permits two independent intensity images to be stored in the same hologram. To fabricate the holograms, a birefringence with defined retardance and orientation of the fast axis is recorded into a photopolymer film. The holograms are selectively read out by choosing the polarization state of the read beam. Polarization holograms of this kind increase the data density in holographic data storage and allow higher quality diffractive optical elements to be written. (C) 2009 Optical Society of America

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[BibTex]


Controlled Propulsion of Artificial Magnetic Nanostructured Propellers
Controlled Propulsion of Artificial Magnetic Nanostructured Propellers

Ghosh, A., Fischer, P.

NANO LETTERS, 9(6):2243-2245, 2009, Featured highlight ‘Nanotechnology: The helix that delivers’ Nature 459, 13 (2009). (article)

Abstract
For biomedical applications, such as targeted drug delivery and microsurgery, it is essential to develop a system of swimmers that can be propelled wirelessly in fluidic environments with good control. Here, we report the construction and operation of chiral colloidal propellers that can be navigated in water with micrometer-level precision using homogeneous magnetic fields. The propellers are made via nanostructured surfaces and can be produced in large numbers. The nanopropellers can carry chemicals, push loads, and act as local probes in rheological measurements.

Featured highlight ‘Nanotechnology: The helix that delivers’ Nature 459, 13 (2009).

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Video - Nanospropellers DOI [BibTex]

Video - Nanospropellers DOI [BibTex]


Absolute Asymmetric Reduction Based on the Relative Orientation of Achiral Reactants
Absolute Asymmetric Reduction Based on the Relative Orientation of Achiral Reactants

Kuhn, A., Fischer, P.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 48(37):6857-6860, 2009 (article)

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DOI [BibTex]

DOI [BibTex]