Lane formation in gravitationally driven colloid mixtures consisting of up to three different particle sizes.

Brownian dynamics simulations are utilized to study segregation phenomena far from thermodynamic equilibrium. In the present study, we expand upon the analysis of binary colloid mixtures and introduce a third particle species to further our understanding of colloidal systems. Gravitationally driven, spherical colloids immersed in an implicit solvent are confined in two-dimensional linear microchannels. The interaction between the colloids is modeled by the Weeks-Chandler-Andersen potential, and the confinement of the colloids is realized by hard walls based on the solution of the Smoluchowski equation in half space. In binary and ternary colloidal systems, a difference in the driving force is achieved by differing colloid sizes but fixed mass density. We observe for both the binary and ternary systems that a driving force difference induces a nonequilibrium phase transition to lanes. For ternary systems, we study the tendency of lane formation to depend on the diameter of the medium-sized colloids. Here we find a sweet spot for lane formation in ternary systems. Furthermore, we study the interaction of two differently sized colloids at the channel walls. Recently we observed that driven large colloids push smaller colloids to the walls. This results in small particle lanes at the walls at early simulation times. In this work we additionally find that thin lanes are unstable and dissolve over very long time frames. Furthermore, we observe a connection between lane formation and the nonuniform distribution of particles along the channel length. This nonuniform distribution occurs either alongside lane formation or in shared lanes (i.e., lanes consisting of two colloid types).

Lane formation of colloidal particles driven in parallel by gravity.

We investigate the lane formation in nonequilibrium systems of colloidal particles moving in parallel that are driven by the force of gravity. For this setup, an experimental implementation of a channel on a slope can be conceptualized. We employ the Brownian dynamics algorithm and confine the repulsive particles with hard walls based on the solution of the Smoluchowski equation in the half space. A difference of the driving force acting on the colloids could be achieved by using two spherical particle types with differing diameters but equal mass density. First, we investigate how a difference in the channel slope affects the lane formation of the systems, after which we analyze the lanes that formed. We find that the large particles push the small particles to the walls, resulting in exclusively small particle lanes at the walls. This contrasts the equilibrium state, where depletion forces push the larger particles to the walls. Additionally, we have a closer look at the mechanisms by which the lanes form. Finally, we find system parameter values that foster lane formation to lay the foundation for an experimental realization of our proposed setup. To round this off, we give an exemplary calculation of the slope angle needed to get the experimental system into a state of lane order. With the examination of lane order in systems that are driven in parallel, we hope to deepen our understanding of nonequilibrium order phenomena.

Negative resistance for colloids driven over two barriers in a microchannel.

When considering the flow of currents through obstacles, one core expectation is that the total resistance of sequential single resistors is additive. While this rule is most commonly applied to electronic circuits, it also applies to other transport phenomena such as the flow of colloids or nanoparticles through channels containing multiple obstacles, as long as these obstacles are sufficiently far apart. Here we explore the breakdown of this additivity for fluids of repulsive colloids driven over two energetic barriers in a microchannel, using real-space microscopy experiments, particle-resolved simulations, and dynamical density functional theory. If the barrier separation is comparable to the particle correlation length, the resistance is highly non-additive, such that the resistance added by the second barrier can be significantly higher or lower than that of the first. Surprisingly, in some cases the second barrier can even add a negative resistance, such that two identical barriers are easier to cross than a single one. We explain this counterintuitive observation in terms of the structuring of particles trapped between the barriers.

Giant polarization anisotropic optical response from anodic aluminum oxide templates embedded with plasmonic metamaterials.

Plasmonic metamaterials enable extraordinary manipulation of key constitutive properties of light at a subwavelength scale and thus have attracted significant interest. Here, we report a simple and convenient nanofabrication method for a novel meta-device by glancing deposition of gold into anodic aluminum oxide templates on glass substrates. A methodology with the assistance of ellipsometric measurements to examine the anisotropy and optical activity properties is presented. A tunable polarization conversion in both transmission and reflection is demonstrated. Specifically, giant broadband circular dichroism for reflection at visible wavelengths is experimentally realized by oblique incidence, due to the extrinsic chirality resulting from the mutual orientation of the metamaterials and the incident beam. This work paves the way for practical applications for large-area, low-cost polarization modulators, polarization imaging, displays, and bio-sensing.

Fast quantitative optical detection of heat dissipation by surface plasmon polaritons.

Heat management at the nanoscale is an issue of increasing importance. In optoelectronic devices the transport and decay of plasmons contribute to the dissipation of heat. By comparison of experimental data and simulations we demonstrate that it is possible to gain quantitative information about excitation, propagation and decay of surface plasmon polaritons (SPPs) in a thin gold stripe supported by a silicon membrane. The temperature-dependent optical transmissivity of the membrane is used to determine the temperature distribution around the metal stripe with high spatial and temporal resolution. This method is complementary to techniques where the propagation of SPPs is monitored optically, and provides additional information which is not readily accessible by other means. In particular, we demonstrate that the thermal conductivity of the membrane can also be derived from our analysis. The results presented here show the high potential of this tool for heat management studies in nanoscale devices.

Tuning the transmission of surface plasmon polaritons across nano and micro gaps in gold stripes.

We applied a far-field technique to measure the surface plasmon propagation over a wide range of gap sizes in thin gold stripes. This is realized with a grating technique which allows the excitation and out coupling of surface plasmon polaritons (SPPs). With this method the intensity can be monitored before and after the gap. The observations show that the SPPs can transmit over gaps with a width of 1µm with a probability of about 40% for Au stripe-waveguides (7 µm width) at a wavelength of 780 nm. The transmission decays exponentially above a gap size of 1 µm. The results also demonstrate that the transmission has non-monotonic behavior for gap sizes smaller than 1 µm that we attribute to excitation of Fabry-Perot modes and resonant localized plasmons within the gap. The experimental results are supported by numerical simulations using a Finite-Difference Time-Domain (FDTD) approach.

Thermo-voltage measurements of atomic contacts at low temperature.

We report the development of a novel method to determine the thermopower of atomic-sized gold contacts at low temperature. For these measurements a mechanically controllable break junction (MCBJ) system is used and a laser source generates a temperature difference of a few kelvins across the junction to create a thermo-voltage. Since the temperature difference enters directly into the Seebeck coefficient S = -ΔV/ΔT, the determination of the temperature plays an important role. We present a method for the determination of the temperature difference using a combination of a finite element simulation, which reveals the temperature distribution of the sample, and the measurement of the resistance change due to laser heating of sensor leads on both sides next to the junction. Our results for the measured thermopower are in agreement with recent reports in the literature.

Controlling the magnetic structure of Co/Pd thin films by direct laser interference patterning.

Nanosecond pulsed two-beam laser interference is used to generate two-dimensional temperature patterns on a magnetic thin film sample. We show that the original domain structure of a [Co/Pd] multilayer thin film changes drastically upon exceeding the Curie temperature by thermal demagnetization. At even higher temperatures the multilayer system is irreversibly changed. In this area no out-of-plane magnetization can be found before and after a subsequent ac-demagnetization. These findings are supported by numerical simulations using the Landau-Lifshitz-Bloch formalism which shows the importance of defect sites and anisotropy changes to model the experiments. Thus, a one-dimensional temperature pattern can be transferred into a magnetic stripe pattern. In this way one can produce magnetic nanowire arrays with lateral dimensions of the order of 100 nm. Typical patterned areas are in the range of several square millimeters. Hence, the parallel direct laser interference patterning method of magnetic thin films is an attractive alternative to the conventional serial electron beam writing of magnetic nanostructures.

Nonlinear optical imaging of single plasmonic nanoparticles with 30 nm resolution.

We show that background free nonlinear optical imaging of Au nanostructures with a resolution down to 30 nm can be achieved. To attain such performance, an ultrafast laser source (110 fs pulse duration) has been integrated into a parabolic mirror assisted scanning near-field optical microscope. Combining nonlinear hyperspectral imaging and the simultaneously obtained topography, the setup allows one to directly correlate/assign locations with nonlinear signals originating from either second harmonic generation or two-photon excitation processes. The contrast mechanisms of the far-field background free nonlinear optical image are discussed based on the different tip-sample coupling schemes and the selective excitation of the plasmonic modes.

Lateral and temporal dependence of the transport through an atomic gold contact under light irradiation: signature of propagating surface plasmon polaritons.

Metallic point contacts (MPCs) with dimensions comparable to the Fermi wavelength of conduction electrons act as electronic waveguides and might operate as plasmon transmitters. Here we present a correlated study of optical and conductance response of MPCs under irradiation with laser light. For elucidating the role of surface plasmon polaritons (SPPs), we integrate line gratings into the leads that increase the SPP excitation efficiency. By analyzing spatial, polarization, and time dependence, we identify two SPP contributions that we attribute to transmitted and decaying SPPs, respectively. The results demonstrate the role of SPPs for optically controlling the transport in metallic nanostructures and are important for designing opto-nanoelectronic devices.

Mapping of plasmonic resonances in nanotriangles.

Plasmonic resonances in metallic nano-triangles have been investigated by irradiating these structures with short laser pulses and imaging the resulting ablation and melting patterns. The triangular gold structures were prepared on Si substrates and had a thickness of 40 nm and a side length of ca. 500 nm. Irradiation was carried out with single femtosecond and picosecond laser pulses at a wavelength of 800 nm, which excited higher order plasmon modes in these triangles. The ablation distribution as well as the local melting of small parts of the nanostructures reflect the regions of large near-field enhancement. The observed patterns are reproduced in great detail by FDTD simulations with a 3-dimensional model, provided that the calculations are not based on idealized, but on realistic structures. In this realistic model, details like the exact shape of the triangle edges and the dielectric environment of the structures are taken into account. The experimental numbers found for the field enhancement are typically somewhat smaller than the calculated ones. The results demonstrate the caveats for FDTD simulations and the potential and the limitations of "near field photography" by local ablation and melting for the mapping of complex plasmon fields and their applications.

Femtosecond-resolved ablation dynamics of Si in the near field of a small dielectric particle.

In this work we analyze the ablation dynamics of crystalline Si in the intense near field generated by a small dielectric particle located at the material surface when being irradiated with an infrared femtosecond laser pulse (800 nm, 120 fs). The presence of the particle (7.9 µm diameter) leads to a strong local enhancement (ca. 40 times) of the incoming intensity of the pulse. The transient optical response of the material has been analyzed by means of fs-resolved optical microscopy in reflection configuration over a time span from 0.1 ps to about 1 ns. Characteristic phenomena like electron plasma formation, ultrafast melting and ablation, along with their characteristic time scales are observed in the region surrounding the particle. The use of a time resolved imaging technique allows us recording simultaneously the material response at ordinary and large peak power densities enabling a direct comparison between both scenarios. The time resolved images of near field exposed regions are consistent with a remarkable temporal shift of the ablation onset which occurs in the sub-picosend regime, from about 500 to 800 fs after excitation.

Near-field effects and energy transfer in hybrid metal-oxide nanostructures.

One of the big challenges of the 21st century is the utilization of nanotechnology for energy technology. Nanoscale structures may provide novel functionality, which has been demonstrated most convincingly by successful applications such as dye-sensitized solar cells introduced by M. Grätzel. Applications in energy technology are based on the transfer and conversion of energy. Following the example of photosynthesis, this requires a combination of light harvesting, transfer of energy to a reaction center, and conversion to other forms of energy by charge separation and transfer. This may be achieved by utilizing hybrid nanostructures, which combine metallic and nonmetallic components. Metallic nanostructures can interact strongly with light. Plasmonic excitations of such structures can cause local enhancement of the electrical field, which has been utilized in spectroscopy for many years. On the other hand, the excited states in metallic structures decay over very short lifetimes. Longer lifetimes of excited states occur in nonmetallic nanostructures, which makes them attractive for further energy transfer before recombination or relaxation sets in. Therefore, the combination of metallic nanostructures with nonmetallic materials is of great interest. We report investigations of hybrid nanostructured model systems that consist of a combination of metallic nanoantennas (fabricated by nanosphere lithography, NSL) and oxide nanoparticles. The oxide particles were doped with rare-earth (RE) ions, which show a large shift between absorption and emission wavelengths, allowing us to investigate the energy-transfer processes in detail. The main focus is on TiO2 nanoparticles doped with Eu(3+), since the material is interesting for applications such as the generation of hydrogen by photocatalytic splitting of water molecules. We use high-resolution techniques such as confocal fluorescence microscopy for the investigation of energy-transfer processes. The experiments are supported by simulations of the electromagnetic field enhancement in the vicinity of well-defined nanoantennas. The results show that the presence of the nanoparticle layer can modify the field enhancement significantly. In addition, we find that the fluorescent intensities observed in the experiments are affected by agglomeration of the nanoparticles. In order to further elucidate the possible influence of agglomeration and quenching effects in the vicinity of the nanoantennas, we have used a commercial organic pigment containing Eu, which exhibits an extremely narrow particle size distribution and no significant agglomeration. We demonstrate that quenching of the Eu fluorescence can be suppressed by covering the nanoantennas with a 10 nm thick SiO x layer.

Control over Janus micromotors by the strength of a magnetic field.

For transportation of molecules or biological cells using artificial motors, the control over their motion, i.e. direction and speed of transfer, is important. Here, we demonstrate that modification of the velocity and orientation of a magnetic Janus particle can be efficiently controlled by tuning the strength of an applied homogeneous magnetic field. Interestingly, by keeping the same orientation of the magnetic field but changing its magnitude not only the velocity of capped particles can be altered but even their direction of motion can be reversed. We put forth a simple qualitative model, which allows us to explain this intriguing observation.

Assessing the plasmonics of gold nano-triangles with higher order laser modes.

Regular arrays of metallic nano-triangles - so called Fischer patterns - are fabricated by nano-sphere lithography. We studied such gold nano-triangle arrays on silicon or glass substrates. A series of different samples was investigated with a parabolic mirror based confocal microscope where the sample is scanned through the laser focus. By employing higher order laser modes (azimuthally and radially polarised laser beams), we can excite the Fischer patterns using either a pure in-plane (x,y) electric field or a strongly z-directional (optical axis of the optical microscope) electric field. We collected and evaluated the emitted luminescence and thereby investigated the respectively excited plasmonic modes. These varied considerably: firstly with the light polarisation in the focus, secondly with the aspect ratio of the triangles and thirdly with the employed substrate. Moreover, we obtained strongly enhanced Raman spectra of an adenine (sub-)monolayer on gold Fischer patterns on glass. We thus showed that gold Fischer patterns are promising surface-enhanced Raman scattering (SERS) substrates.

Revealing thermal effects in the electronic transport through irradiated atomic metal point contacts.

We report on the electronic transport through nanoscopic metallic contacts under the influence of external light fields. Various processes can be of relevance here, whose underlying mechanisms can be studied by comparing different kinds of atomic contacts. For this purpose two kinds of contacts, which were established by electrochemical deposition, forming a gate-controlled quantum switch (GCQS), have been studied. We demonstrate that in these kinds of contacts thermal effects resulting from local heating due to the incident light, namely thermovoltage and the temperature dependences of the electrical resistivity and the electrochemical (Helmholtz) double layer are the most prominent effects.

Stochastic transport of particles across single barriers.

Transport phenomena of interacting particles are of high interest for many applications in biology and mesoscopic systems. Here we present measurements on colloidal particles, which are confined in narrow channels on a substrate and interact with a barrier, which impedes the motion along the channel. The substrate of the particle is tilted in order for the particles to be driven towards the barrier and, if the energy gained by the tilt is large enough, surpass the barrier by thermal activation. We therefore study the influence of this barrier as well as the influence of particle interaction on the particle transport through such systems. All experiments are supported with Brownian dynamics simulations in order to complement the experiments with tests of a large range of parameter space which cannot be accessed in experiments.

Quantitative imaging of the optical near field.

When exposing small particles on a substrate to a light plane wave, the scattered optical near field is spatially modulated and highly complex. We show, for the particular case of dielectric microspheres, that it is possible to image these optical near-field distributions in a quantitative way. By placing a single microsphere on a thin film of the photosensitive phase change material Ge(2)Sb(5)Te(5) and exposing it to a single short laser pulse, the spatial intensity modulation of the near field is imprinted into the film as a pattern of different material phases. The resulting patterns are investigated by using optical as well as high-resolution scanning electron microscopy. Quantitative information on the local optical near field at each location is obtained by calibrating the material response to pulsed laser irradiation. We discuss the influence of polarization and angle of incidence of the laser beam as well as particle size on the field distribution. The experimental results are in good quantitative agreement with a model based on a rigorous solution of Maxwell's equations. Our results have potential application to near-field optical lithography and experimental determination of near fields in complex nanostructures.

Quantitative measurement of the near-field enhancement of nanostructures by two-photon polymerization.

The quantitative determination of the strength of the near-field enhancement in and around nanostructures is essential for optimizing and using these structures for applications. We combine the gaussian intensity distribution of a laser profile and two-photon-polymerization of SU-8 to a suitable tool for the quantitative experimental measurement of the near-field enhancement of a nanostructure. Our results give a feedback to the results obtained by finite-difference time-domain (FDTD) simulations. The structures under investigation are gold nanotriangles on a glass substrate with 85 nm side length and a thickness of 40 nm. We compare the threshold fluence for polymerization for areas of the gaussian intensity profile with and without the near-field enhancement of the nanostructures. The experimentally obtained value of the near-field intensity enhancement is 600 ± 140, independent of the laser power, irradiation time, and spot size. The FDTD simulation shows a pointlike maximum of 2600 at the tip. In a more extended area with an approximate size close to the smallest polymerized structure of 25 nm in diameter, we find a value between 800 and 600. Using our novel approach, we determine the threshold fluence for polymerization of the commercially available photopolymerizable resin SU-8 by a femtosecond laser working at a wavelength of 795 nm and a repetition rate of 82 MHz to be 0.25 J/cm(2) almost independent of the irradiation time and the laser power used. This finding is important for future applications of the method because it enables one to use varying laser systems.