Iontronic microscopy of a tungsten microelectrode: "seeing" ionic currents under an optical microscope.

Optical methods for monitoring electrochemical reactions at an interface are advantageous because of their table-top setup and ease of integration into reactors. Here we apply EDL-modulation microscopy to one of the main components of amperometric measurement devices: a microelectrode. We present experimental measurements of the EDL-modulation contrast from the tip of a tungsten microelectrode at various electrochemical potentials inside a ferrocene-dimethanol Fe(MeOH)2 solution. Using the combination of the dark-field scattering microscope and the lock-in detection technique, we measure the phase and amplitude of local ion-concentration oscillations in response to an AC potential as the electrode potential is scanned through the redox-activity window of the dissolved species. We present the amplitude and phase map of this response, as such this method can be used to study the spatial and temporal variations of the ion-flux due to an electrochemical reaction close to metallic and semiconducting objects of general geometry. We discuss the advantages and possible extensions of using this microscopy method for wide-field imaging of ionic currents.

Regulating the aggregation of colloidal particles in an electro-osmotic micropump.

Unrestricted particle transport through microfluidic channels is of paramount importance to a wide range of applications, including lab-on-a-chip devices. In this article, we study via video microscopy the electro-osmotic aggregation of colloidal particles at the opening of a micrometer-sized silica channel in the presence of a salt gradient. Particle aggregation eventually leads to clogging of the channel, which may be undone by a time-adjusted reversal of the applied electric potential. We numerically model our system via the Stokes-Poisson-Nernst-Planck equations in a geometry that approximates the real sample. This allows us to identify the transport processes induced by the electric field and salt gradient and to provide evidence that a balance thereof leads to aggregation. We further demonstrate experimentally that a net flow of colloids through the channel may be achieved by applying a square-waveform electric potential with an appropriately tuned duty cycle. Our results serve to guide the design of microfluidic and nanofluidic pumps that allow for controlled particle transport and provide new insights for anti-fouling in ultra-filtration.

Interfacing Superconducting Qubits and Single Optical Photons Using Molecules in Waveguides.

We propose an efficient light-matter interface at optical frequencies between a single photon and a superconducting qubit. The desired interface is based on a hybrid architecture composed of an organic molecule embedded inside an optical waveguide and electrically coupled to a superconducting qubit placed near the outside surface of the waveguide. We show that high fidelity, photon-mediated, entanglement between distant superconducting qubits can be achieved with incident pulses at the single photon level. Such a low light level is highly desirable for achieving a coherent optical interface with superconducting qubit, since it minimizes decoherence arising from the absorption of light.

Nanocapillary electrokinetic tracking for monitoring charge fluctuations on a single nanoparticle.

We introduce nanoCapillary Electrokinetic Tracking (nanoCET), an optofluidic platform for continuously measuring the electrophoretic mobility of a single colloidal nanoparticle or macromolecule in vitro with millisecond time resolution and high charge sensitivity. This platform is based on using a nanocapillary optical fiber in which liquids may flow inside a channel embedded inside the light-guiding core and nanoparticles are tracked using elastic light scattering. Using this platform we have experimentally measured the electrophoretic mobility of 60 nm gold nanoparticles in an aqueous environment. Further, using numerical simulations, we demonstrate the underlying electrokinetic dynamics inside the nanocapillary and the necessary steps for extending this method to probing single biomolecules, which can be achieved with existing technologies. This achievement will immensely facilitate the daunting challenge of monitoring biochemical or catalytic reactions on a single entity over a wide range of timescales. The unique measurement capabilities of this platform pave the way for a wide range of discoveries in colloid science, analytical biochemistry, and medical diagnostics.

Intersystem crossing rates of single perylene molecules in ortho-dichlorobenzene.

Triplet states can be interesting for optical switching of molecular fluorescence as well as quantum experiments relying on the manipulation of spin states. However, the ground state of molecules is usually a singlet state. It is therefore interesting to study the intersystem crossing (ISC) rates between singlet and triplet states. We have measured the autocorrelation function of the fluorescence from single perylene molecules in an ortho-dichlorobenzene host matrix at cryogenic temperatures (1.3 K). We observed two time scales in the autocorrelation function corresponding to intersystem crossing to two indistinguishable triplet states (TX and TY) and a third triplet state (TZ). By studying the power dependence of the correlation times and contrasts in the autocorrelation functions of single molecules, we determine the ISC rates of perylene for the first time.

Design and synthesis of aromatic molecules for probing electric fields at the nanoscale.

We propose using halogenated organic dyes as nanoprobes for electric fields and show their greatly enhanced Stark coefficients using density functional theory (DFT) calculations. We analyse halogenated variants of three molecules that have been of interest for cryogenic single molecule spectroscopy: perylene, terrylene, and dibenzoterrylene, with the zero-phonon optical transitions at blue, red, and near-infrared. Out of all the combinations of halides and binding sites that are calculated, we have found that fluorination of the optimum binding site induces a dipole difference between the ground and excited states larger than 0.5 D for all three molecules with the highest value of 0.69 D for fluoroperylene. We also report on the synthesis of 3-fluoroterrylene and the bulk spectroscopy of this compound in liquid and solid organic environments.

Coherent interaction of light and single molecules in a dielectric nanoguide.

Many of the currently pursued experiments in quantum optics would greatly benefit from a strong interaction between light and matter. Here, we present a simple new scheme for the efficient coupling of single molecules and photons. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor (ß) of 18% for the dye molecules doped in the organic crystal. A combination of extinction, fluorescence excitation, and resonance fluorescence spectroscopy with microscopy provides high-resolution spatiospectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum-optical phenomena, including polaritonic interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.

Origami nanogap electrodes for reversible nanoparticle trapping.

We present a facile desktop fabrication method for origami-based nanogap indium tin oxide (ITO) electrokinetic particle traps, providing a simplified approach compared to traditional lithographic techniques and effective trapping of nanoparticles. Our approach involves bending ITO thin films on optically transparent polyethylene terephthalate (PET), creating an array of parallel nanogaps. By strategically introducing weak points through cut-sharp edges, we successfully controlled the spread of nanocracks. A single crack spanning the constriction width and splitting the conductive layers forms a nanogap that can effectively trap small nanoparticles after applying an alternating electric potential across the nanogap. We analyze the conditions for reversible trapping and optimal performance of the nanogap ITO electrodes with optical microscopy and electrokinetic impedance spectroscopy. Our findings highlight the potential of this facile fabrication method for the use of ITO at active electro-actuated traps in microfluidic systems.

Open hardware in microscopy.

The field of microscopy has been empowering humankind for many centuries by enabling the observation of objects that are otherwise too small to detect for the naked human eye. Microscopy techniques can be loosely divided into three main branches, namely photon-based optical microscopy, electron microscopy, and scanning probe microscopy with optical microscopy being the most prominent one. On the high-end level, optical microscopy nowadays enables nanometer resolution covering many scientific disciplines ranging from material sciences over the natural sciences and life sciences to the food sciences. On the lower-end level, simplified hardware and openly available description and blueprints have helped to make powerful microscopes widely available to interested scientists and researchers. For this special issue, we invited contributions from the community to share their latest ideas, designs, and research results on open-source hardware in microscopy. With this collection of articles, we hope to inspire the community to further increase the accessibility, interoperability, and reproducibility of microscopy. We further touch on the standardization of methodologies and devices including the use of computerized control of data acquisition and data analysis to achieve high quality and efficiency in research and development.

Dark-field light scattering microscope with focus stabilization.

We present detailed design and operation instructions for a single-objective inverted microscope. Our design is suitable for two dark-field modes of operation: 1- total internal reflection scattering, and 2- cross-polarization backscattering. The user can switch between the two modes by exchanging one mode-steering element, which is also adapted to the Thorlabs cage system. To establish a stable background speckle for differential microscopy the imaging plane is stabilized with active feedback. We validate the stabilization efficacy by performing long-term scattering measurement on single nanoparticles. This setup can be extended for simultaneous scattering, fluorescence, and confocal imaging modes.

Sensing force and charge at the nanoscale with a single-molecule tether.

Measuring the electrophoretic mobility of molecules is a powerful experimental approach for investigating biomolecular processes. A frequent challenge in the context of single-particle measurements is throughput, limiting the obtainable statistics. Here, we present a molecular force sensor and charge detector based on parallelised imaging and tracking of tethered double-stranded DNA functionalised with charged nanoparticles interacting with an externally applied electric field. Tracking the position of the tethered particle with simultaneous nanometre precision and microsecond temporal resolution allows us to detect and quantify the electrophoretic force down to the sub-piconewton scale. Furthermore, we demonstrate that this approach is suitable for detecting changes to the particle charge state, as induced by the addition of charged biomolecules or changes to pH. Our approach provides an alternative route to studying structural and charge dynamics at the single molecule level.