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Wolfgang Langbein

Publications and source records attributed to Wolfgang Langbein.

At least 19 recordsLinked to original sources

Ultra-high-speed line-scan Raman imaging

Raman spectroscopic imaging has emerged as a potent tool due to its non-invasive nature and capability for chemical composition analysis. Line-scan Raman spectroscopy accelerates imaging speed by two orders of magnitude compared to point detection Raman methods. However, further enhancements in imaging speed were constrained by the readout speed of typically used charge-coupled device (CCD) spectroscopic detectors. We developed an ultra-fast line-scan Raman imaging technique based on recently available complementary metal-oxide-semiconductor (CMOS) detectors with low cost and read noise, and fast readout during exposure combined with a global shutter. Employing a high-efficiency transmissiongrating imaging spectrometer, we demonstrate imaging speeds up to two orders of magnitude faster than traditional line scan Raman imaging techniques and up to four orders of magnitude faster than point scan Raman methods, achieving Raman imaging up to 80 kHz spectral rate. We demonstrate that this technology is applicable to a variety of samples, including microplastics, biological cells, and tablets, creating images in an extremely short time frame, showcasing exceptional detection capabilities and the ability to reveal detailed information.

physics.optics↗

Sub-nanometer 3D morphometric precision of polarisation-resolved wide-field optical extinction microscopy determines the roundness of individual gold nanospheres

Quantitative polarisation-resolved optical extinction microscopy of individual plasmonic nanoparticles has recently been introduced as a powerful tool to characterise the nanoparticle's morphology with a precision comparable to electron microscopy, while using a simple optical microscope [Nanoscale 12, 16215 (2020)]. Here we provide a step change by adding measurements for radial polarisation in the condenser back focal plane, probing plasmonic resonances polarised in axial direction. The combined linear and radial polarisation measurements provide a significantly enhanced precision of the retrieved 3D morphology, as we show on defect-free ultra-uniform gold nanospheres of 30 nm nominal diameter characterised by transmission electron microscopy. The measured cross-sections are modelled for an ellipsoidal particle, determining the three semi-axes and rotation angles by fitting the measurements. The material permittivity and surface damping providing the best fit are found. The particle aspect ratio is determined with a precision better than 5%, and the size with an impressive precision of 0.1 nm. Notably, corrections to the Rayleigh-Gans ellipsoid model due to retardation are significant even though the particle diameters are more than an order of magnitude smaller than the wavelength in the medium. Taking them into account improves the shape accuracy.

physics.optics↗

The origin and influence of non-cavity modes in a micropillar Bragg microcavity

Controlling the photonic environment of emitters is essential to the design of classical and quantum light sources. We study the case of a dipole-like emitter in a cylindrical pillar etched into a planar Bragg microcavity, which is a common design of quantum-dot single photon source. In addition to the well-known cavity modes created by the high-reflectivity of the Bragg mirrors at small in-plane wavevectors, we show the presence of broad spectral features that play a key role in controlling photon collection efficiency and Purcell enhancement. These non-cavity modes are insensitive to the periodic index modulation of the Bragg reflectors, but arise from the cylindrical pillar geometry, as we show by comparison with simulations of uniform pillars, which reproduce the non-cavity modes. This approach provides a tool for understanding and modelling these often-disregarded decay channels as a function of source height, cavity dimensions and surface layers.

physics.optics↗

Exciton coherence propagation measured with non-local four-wave mixing micro-spectroscopy

Coherence transfer is a multi-disciplinary topic of interest, including chemistry, biology and physics. In quantum technologies, achieving non-local coherent coupling between solid-state qubits is of the utmost importance. Here, we demonstrate that excitons - i.e. electron-hole pairs bound by the Coulomb force within a quantum well - can act as a medium for mesoscopic optical coherence transfer in semiconductors. To this end, we use a femtosecond laser pulse to resonantly generate excitons within the light cone. These excitons can then either recombine radiatively or scatter out of the light cone, gaining an in-plane momentum in the process. In samples without disorder, such as the CdTe quantum wells used here, the resulting fast excitons can diffuse over mesoscopic distances before recombining radiatively. Using coherent nonlinear micro-spectroscopy, we carry out exciton time-of-flight measurements. Specifically, we monitor the spatio-temporal propagation of launched exciton wave packets, selectively observing their coherence or density on a scale of up to 10$\,μ$m. Our proof-of-principle experiment demonstrates that free excitons inherit a phase modulation from the optical pulsed excitation and can generate coherent links within excitonic circuits, offerring a higher level of miniaturisation and compactness than photonic or polaritonic architectures.

physics.optics↗

Understanding the mechanisms of supported lipid membrane reshaping into tubular networks using quantitative DIC microscopy

Biological membranes are known to form various structural motifs, from lipid bilayers to tubular filaments and networks facilitating e.g. adhesion and cell-cell communication. To understand the biophysical processes underpinning lipid-lipid interactions in these systems, synthetic membrane models are crucial. Here, we demonstrate the formation of tubular networks from supported lipid membranes of controlled lipid composition on glass. We quantify tube radii using quantitative differential interference contrast (qDIC) and propose a biophysical mechanism for the formation of these structures, regulated by surface tension and lipid exchange with connected supported membranes. Two lipid types are investigated, namely DOPC and DC15PC, exhibiting a liquid disordered and a solid ordered phase at room temperature, respectively. Tube formation is studied versus temperature, revealing bilamellar layers retracting and folding into tubes upon DC15PC lipids transitioning from liquid to solid phase, which is explained by lipid transfer from bilamellar to unilamellar layers. This study introduces a novel model system for bilayer tubes, allowing to elucidate the biophysics of lipid-lipid interactions governing lipid membrane reshaping into tubular structures, important for our understanding of biological membrane filaments.

cond-mat.soft↗

Designing low-loss cavities across the band-gap of photonic crystal slabs

Photonic crystal cavities (PCCs) are defects in host photonic crystals (PCs) which create bound states in the PC band gap. These bound states are resonant states of the electromagnetic field with a complex resonance frequency and can have very small mode volumes. PCCs are attractive for a variety of applications, from cavity quantum electrodynamics to biosensing. A PC slab geometry is advantageous given its superior manufacturability compared to three-dimensional crystals, and the accessibility of the surface allows sensing and coupling. However, the emission into the half spaces above and below the slab limits the bound state lifetime. Controlling this emission is thus crucial for applications, most of which benefiting from a long lifetime. A range of methods to find defect geometries suppressing the emission to increase the lifetime have been demonstrated in the past. However, they do not cater for a designed resonant frequency covering a wide addressable range, as needed for multiplexed devices. Here, we demonstrate a design method controlling both resonance frequency and emission, by minimising a cost function including both losses and target frequency. We show applications on PCCs in GaAs PC slabs immersed in water, relevant for biosensing. The reduced refractive index contrast in these structures compared to previously studied PCCs embedded in vacuum renders the emission suppression more challenging. We optimize the quality factor of a standard L3 cavity from 1000 to 10^4-10^5, with an addressable resonance frequency range covering 12% relative bandwidth, spanning more than half of the band gap. We furthermore report optimised structures of H1 cavities, and provide the optimisation code for widespread use.

physics.optics↗

Genetically encoding stimulated Raman-scattering probes for cell imaging using infrared fluorescent proteins

Stimulated Raman scattering (SRS) microscopy offers great potential to surpass fluorescent-based approaches, owing to the sharp linewidth of Raman vibrations amenable to super-multiplex cell imaging, but currently lacks one crucial component: genetically encodable tags equivalent to fluorescent proteins. Here, we show that infrared fluorescent proteins (IRFPs) can be used as genetically encoded SRS probes and benefit from the electronic pre-resonant SRS enhancement effect with near-infrared exciting pulses, comparable to synthetic dyes reported in the literature. SRS imaging of the nucleus in mammalian cells is demonstrated where a histone protein is fused to an IRFP. This work opens the route towards Raman-based cell imaging using genetically encoded probes, motivating efforts in solving the challenges of photostability and creating a vibrational palette.

physics.chem-ph↗

Förster transfer between quantum dots in a shared phonon environment: An exact approach, revealing the role of pure dephasing

Förster resonance energy transfer has an important role in nature and technology, rendering its exact theoretical understanding significant. To this end, a system of two electronically decoupled quantum dots (QDs) is considered, interacting via dipole-dipole interaction and a common phonon bath. While the former leads to an oscillatory excitation transfer between the dots, the latter provide the dissipation resulting in directional Förster transfer. We present an exact microscopic treatment of the phonon-assisted transitions between hybridized exciton levels of the coupled QD system, going beyond the simple perturbative approaches commonly used in the literature. From our asymptotically exact results we extract population decay times $T_1$, dephasing times $T_2$, and resulting pure dephasing times $T_2^*$ of the states. We compare this treatment with an analytical model based on Fermi's golden rule, combining the most accurate elements of existing analytical treatments. The exact results show a significant deviation from this model in some parameter regimes, mainly due to the role of multi-phonon processes, which become important for comparable electron-phonon and dipolar coupling, realised at short distances between the QDs and at elevated temperatures.

cond-mat.mes-hall↗

Extending completeness of the eigenmodes of an open system beyond its boundary, for Green's function and scattering-matrix calculations

The asymptotic completeness of a set of the eigenmodes of an open system with increasing number of modes enables an accurate calculation of the system response in terms of these modes. Using the exact eigenmodes, such completeness is limited to the interior of the system. Here we show that when the eigenmodes of a target system are obtained by the resonant-state expansion, using the modes of a basis system embedding the target system, the completeness extends beyond the boundary of the target system. We illustrate this by using the Mittag-Leffler series of the Green's function expressed in terms of the eigenmodes, which converges to the correct solution anywhere within the basis system, including the space outside the target system. Importantly, this property allows one to treat pertubations outside the target system and to calculate the scattering cross-section using the boundary conditions for the basis system. Choosing a basis system of spherical geometry, these boundary conditions have simple analytical expressions, allowing for an efficient calculation of the response of the target system, as we demonstrate for a resonator in a form of a finite dielectric cylinder.

physics.optics↗

Thousand foci coherent anti-Stokes Raman scattering microscopy

We demonstrate coherent anti-Stokes Raman scattering (CARS) microscopy with 1089 foci, enabled by a high repetition rate amplified oscillator and optical parametric amplifier. We employ a camera as multichannel detector to acquire and separate the signals from the foci, rather than using the camera image itself. This allows to retain the insensitivity of the imaging to sample scattering afforded by the non-linear excitation point-spread function, which is the hallmark of point-scanning techniques. We show frame rates of 0.3Hz for a megapixel CARS image, limited by the camera used. The laser source and corresponding CARS signal allows for at least 1000 times higher speed, and using faster cameras would allow acquiring at that speed, opening a perspective to megapixel CARS imaging with more than 100Hz frame rate.

physics.optics↗

Direct visualization of domain wall pinning in sub-100nm 3D magnetic nanowires with cross-sectional curvature

The study of 3D magnetic nanostructures has uncovered a range of rich phenomena including the stabilization and control of topological spin textures using nanoscale curvature, dynamic effects allowing controlled spin-wave emission, and novel ground states enabled by collective 3D frustrated interactions. From a technological perspective, 3D nanostructures offer routes to ultrahigh density data storage, massive interconnectivity within neuromorphic devices, as well as applications within health technologies, such as mechanical induction of stem cell differentiation. However, the fabrication of 3D nanomagnetic systems with feature sizes down to 10 nm poses a significant challenge. In this work we present a means of fabricating sub-100 nm 3D ferromagnetic nanowires, with both cross-sectional and longitudinal curvature, using two-photon lithography at a wavelength of 405 nm, combined with conventional deposition. Physical characterization illustrates that nanostructures with lateral features as low as 70 nm can be rapidly and reproducibly fabricated. A range of novel domain walls, with anti-vortex textures, coupled transverse textures, and hybrid vortex/anti-vortex textures are found to be enabled by the cross-sectional curvature of the system, as demonstrated by finite-element micromagnetic simulations. Magnetic force microscopy experiments in an externally applied magnetic field are used to image the injection and pinning of domain walls in the 3D magnetic nanowire. At specific field values, domain walls are observed to hop from trap to trap, providing a direct means to probe the local energy landscape. A simple model is presented demonstrating that thickness gradients and local roughness dictate the variation of pinning probability across the wire.

cond-mat.mes-hall↗

Probing Purcell enhancement and photon collection efficiency of InAs quantum dots at nodes of the cavity electric field

The interaction of excitonic transitions with confined photonic modes enables tests of quantum physics and design of efficient optoelectronic devices. Here we study how key metrics such as Purcell factor, beta-factor and collection efficiency are determined by the non-cavity modes which exist in real devices, taking the well-studied micropillar cavity as an example. Samples with dots at different positions in the cavity field allow us to quantify the effect of the non-cavity modes and show that the zero-phonon line and the phonon-assisted emission into the cavity mode HE11 is suppressed by positioning dots at the field node.

cond-mat.mes-hall↗

Giant microwave-optical Kerr nonlinearity via Rydberg excitons in cuprous oxide

Microwave-optical conversion is key to future networks of quantum devices, such as those based on superconducting technology. Conversion at the single quantum level requires strong nonlinearity, high bandwidth, and compatibility with a millikelvin environment. A large nonlinearity is observed in Rydberg atoms, but combining atomic gases with dilution refrigerators is technically challenging. Here we demonstrate that a strong microwave-optical nonlinearity in a cryogenic, solid-state system by exploiting Rydberg states of excitons in \cuprite. We measure a microwave-optical cross-Kerr coefficient of $B_0 = 0.022 \pm 0.008 $ m V$^{-2}$ at 4~K, which is several orders of magnitude larger than other solid-state systems. Our results highlight the potential of Rydberg excitons for nonlinear optics, and form the basis for a microwave-optical frequency converter based on Cu$_2$O.

cond-mat.mes-hall↗

Differential Dynamic Microscopy can be applied to Differential Interference Contrast images despite shadowing effects

During In Vitro Fertilisation (IVF), combining time-lapse contrast microscopy with suitable image processing techniques could facilitate non-invasive classification of oocyte health, driving oocyte selection to maximise success rates. One image processing technique, Differential Dynamic Microscopy (DDM), has been used in a variety of microscopy settings including bright field, dark field and fluorescence. However, in some applications, effects stemming from the choice of microscopy may invalidate underlying assumptions of DDM. Here, we study the DDM analysis of differential interference contrast (DIC) microscopy movies. DIC exhibits a characteristic shadowing effect that gives the illusion of a 3D appearance, which we show causes deformation of the output DDM matrix. We present a mathematical description of this deformation, and conclude that, when studying isotropic motion, no account of the DIC shadow needs to be considered during DDM analysis. We validate our conclusions with simulated particle data, and with DIC images of colloidal dispersions. Although this conclusion does not generally extend to anisotropic motion, we demonstrate that for directed advection and diffusion behaviour, parameter fitting invariance still holds. These results validate the current practice of applying DDM to DIC, and are a foundation for further exploration of DDM in other phase-contrast image datasets.

cond-mat.stat-mech↗

Correlative extinction and single fluorophore bleaching microscopy for ligand quantification on gold nanoparticles

Nanoparticles (NPs) are promising therapeutic delivery agents, yet it is increasingly apparent that the number and manner of presentation of cell binding ligands on the NP can affect the eventual fate of the therapeutic. Whenever NPs are conjugated with biomolecules, a heterogenous population of decorated NPs will be produced and the details of the subpopulations of particle-ligand structures needs to be characterised for a reliable interpretation of NP-based data. We report an optical microscopy method to quantitatively evaluate the conjugation on a single particle basis in samples consisting of gold NPs (GNPs) decorated with human holo-transferrin fluorescently labelled with Alexa647 (Tf). We employed widefield fluorescence and extinction microscopy on NP-ligand constructs sparesly deposited onto a glass surface, alongside a correlative analysis which spatially co-localises diffraction-limited sources of fluorescence with the optical extinction by individual GNPs. A photobleaching step analysis of the fluorescence emission was employed to estimate the number of fluorophores contributing to the detected emission rate. The method quantifies the number of fluorescent biomolecules attached per GNP, the numbers of unconjugated GNPs and unbound Tf present within the mixed population, and the size and intraparticle clustering propensity of conjugated GNPs. We found a high variability in the number of Tf ligands per GNP within the GNP population, when analysed at the single-particle level, unraveling a non-trivial statistical distribution not accessible in ensemble averaged approaches

physics.optics↗

Correlative light electron microscopy using small gold nanoparticles as single probes

Correlative light electron microscopy (CLEM) requires the availability of robust probes which are visible both in light and electron microscopy. Here we demonstrate a CLEM approach using small gold nanoparticles as a single probe. Individual gold nanoparticles bound to the epidermal growth factor protein were located with nanometric precision background-free in human cancer cells by light microscopy using resonant four-wave-mixing (FWM), and were correlatively mapped with high accuracy to the corresponding transmission electron microscopy images. We used nanoparticles of 10 nm and 5 nm radius, and show a correlation accuracy below 60 nm over an area larger than 10 um size, without the need for additional fiducial markers. Correlation accuracy was improved to below 40 nm by reducing systematic errors, while the localisation precision is below 10 nm. Polarisation-resolved FWM correlates with nanoparticle shapes, promising for multiplexing by shape recognition in future applications. Owing to the photostability of gold nanoparticles and the applicability of FWM microscopy to living cells, FWM-CLEM opens up a powerful alternative to fluorescence-based methods.

physics.optics↗

Quantitatively linking morphology and optical response of individual silver nanohedra

The optical response of metal nanoparticles is governed by plasmonic resonances, which are dictated by the particle morphology. A thorough understanding of the link between morphology and optical response requires quantitatively measuring optical and structural properties of the same particle. Here we present such a study, correlating electron tomography and optical micro-spectroscopy. The optical measurements determine the scattering and absorption cross-section spectra in absolute units, and electron tomography determines the 3D morphology. Numerical simulations of the spectra for the individual particle geometry, and the specific optical setup used, allow for a quantitative comparison including the cross-section magnitude. Silver nanoparticles produced by photochemically driven colloidal synthesis, including decahedra, tetrahedra and bi-tetrahedra are investigated. A mismatch of measured and simulated spectra is found when assuming pure silver particles, which is resolved by the presence of a few atomic layers of tarnish on the surface, not evident in electron tomography. The presented method tightens the link between particle morphology and optical response, supporting the predictive design of plasmonic nanomaterials.

physics.optics↗

First-order perturbation theory of eigenmodes for systems with interfaces

We present an exact first-order perturbation theory for the eigenmodes in systems with interfaces causing material discontinuities. We show that when interfaces deform, higher-order terms of the perturbation series can contribute to the eigenmode frequencies in first order in the deformation depth. This means that the usual diagonal approximation is not necessarily equal to the firstorder approximation, rendering the well known single-mode result insufficient. Extracting the true first-order correction from all higher-order terms enables us to recover the diagonal formalism in a modified form. A general formula for the single-mode first-order correction to electromagnetic eigenmodes is derived, capable of treating dispersive, magnetic, and chiral materials with arbitrary shapes.

physics.optics↗