arXiv subjects

Fritz Keilmann

Publications and source records attributed to Fritz Keilmann.

10 recordsLinked to original sources

arXiv2024

Transient infrared nanoscopy resolves the millisecond photoswitching dynamics of single lipid vesicles in water

Understanding the biophysical and biochemical properties of molecular nanocarriers under physiological conditions and with minimal interference is crucial for advancing nanomedicine, photopharmacology, drug delivery, nanotheranostics and synthetic biology. Yet, analytical methods struggle to combine precise chemical imaging and measurements without perturbative labeling. This challenge is exemplified for azobenzene-based photoswitchable lipids, which are intriguing reagents for controlling nanocarrier properties on fast timescales, enabling, e.g., precise light-induced drug release processes. Here, we leverage the chemical recognition and high spatio-temporal resolution of scattering-type scanning near-field optical microscopy (s-SNOM) to demonstrate non-destructive, label-free mid-infrared (MIR) imaging and spectroscopy of photoswitchable liposomes below the diffraction limit and the tracking of their dynamics down to 50 ms resolution. The vesicles are adsorbed on an ultrathin 10-nm SiN membrane, which separates the sample space from the tip space for stable and hour-long observations. By implementing a transient nanoscopy approach, we accurately resolve, for the first time, photoinduced changes in both the shape and the MIR spectral signature of individual vesicles and reveal abrupt change dynamics of the underlying photoisomerization process. Our findings highlight the methods potential for future studies on the complex dynamics of unlabeled nanoscale soft matter, as well as, in a broader context, for host-guest systems, energy materials or drugs.

physics.optics↗

arXiv2024

Revealing mode formation in quasi-bound states in the continuum metasurfaces via near-field optical microscopy

Photonic metasurfaces offer exceptional control over light at the nanoscale, facilitating applications spanning from biosensing, and nonlinear optics to photocatalysis. Many metasurfaces, especially resonant ones, rely on periodicity for the collective mode to form, which makes them subject to the influences of finite size effects, defects, and edge effects, all of which have considerable negative impact at the application level. These aspects are especially important for quasi-bound state in the continuum (BIC) metasurfaces, for which the collective mode is highly sensitive to perturbations due to high quality factors and strong near-field enhancement. Here, we quantitatively investigate the mode formation in quasi-BIC metasurfaces on the individual resonator level using scattering scanning near-field optical microscopy (s-SNOM) in combination with a new image processing technique. We find that the quasi-BIC mode is formed at a minimum size of 10 x 10-unit cells much smaller than expected from far-field measurements. Furthermore, we show that the coupling direction of the resonators, defects and edge states have pronounced influence on the quasi-BIC mode. This study serves as a link between the far-field and near-field responses of metasurfaces, offering crucial insights for optimizing spatial footprint and active area, holding promise for augmenting applications such as catalysis and biospectroscopy.

physics.optics↗

arXiv2024

Nanoscale mechanical manipulation of ultrathin SiN membranes enabling infrared near-field microscopy of liquid-immersed samples

Scattering scanning near-field optical microscopy (s-SNOM) is a powerful technique for mid-infrared spectroscopy at nanometer length scales. By investigating objects in aqueous environments through ultrathin membranes, s-SNOM has recently been extended towards label-free nanoscopy of the dynamics of living cells and nanoparticles, assessing both the optical and the mechanical interactions between the tip, the membrane and the liquid suspension underneath. Here, we report that the tapping AFM tip induces a reversible nanometric deformation of the membrane manifested as either an indentation or protrusion. This mechanism depends on the driving force of the tapping cantilever, which we exploit to minimize topographical deformations of the membrane to improve optical measurements. Furthermore, we show that the tapping phase, or phase delay between driving signal and tip oscillation, is a highly sensitive observable for quantifying the mechanics of adhering objects, exhibiting highest contrast for low tapping amplitudes where the membrane remains nearly flat. We correlate mechanical responses with simultaneously recorded spectroscopy data to reveal the thickness of nanometric water pockets between membrane and adhering objects. Besides a general applicability of depth profiling, our technique holds great promise for studying mechano-active biopolymers and living cells, biomaterials that exhibit complex behaviors when under a mechanical load.

physics.optics↗

arXiv2019

Anisotropic Strain Induced Soliton Movement Changes Stacking Order and Bandstructure of Graphene Multilayers

The crystal structure of solid-state matter greatly affects its electronic properties. For example in multilayer graphene, precise knowledge of the lateral layer arrangement is crucial, since the most stable configurations, Bernal and rhombohedral stacking, exhibit very different electronic properties. Nevertheless, both stacking orders can coexist within one flake, separated by a strain soliton that can host topologically protected states. Clearly, accessing the transport properties of the two stackings and the soliton is of high interest. However, the stacking orders can transform into one another and therefore, the seemingly trivial question how reliable electrical contact can be made to either stacking order can a priori not be answered easily. Here, we show that manufacturing metal contacts to multilayer graphene can move solitons by several $μ$m, unidirectionally enlarging Bernal domains due to arising mechanical strain. Furthermore, we also find that during dry transfer of multilayer graphene onto hexagonal Boron Nitride, such a transformation can happen. Using density functional theory modeling, we corroborate that anisotropic deformations of the multilayer graphene lattice decrease the rhombohedral stacking stability. Finally, we have devised systematics to avoid soliton movement, and how to reliably realize contacts to both stacking configurations.

cond-mat.mes-hall↗

arXiv2017

Artifact Free Transient Near-Field Nanoscopy

We report on the first implementation of ultrafast near field nanoscopy carried out with the transient pseudoheterodyne detection method (Tr-pHD). This method is well suited for efficient and artifact free pump-probe scattering-type near-field optical microscopy with nanometer scale resolution. The Tr-pHD technique is critically compared to other data acquisition methods and found to offer significant advantages. Experimental evidence for the advantages of Tr-pHD is provided in the Near-IR frequency range. Crucial factors involved in achieving proper performance of the Tr-pHD method with pulsed laser sources are analyzed and detailed in this work. We applied this novel method to time-resolved and spatially resolved studies of the photo-induced effects in the insulator-to-metal transition system vanadium dioxide with nanometer scale resolution.

cond-mat.mes-hall↗

arXiv2017

Relative efficiency of polariton emission in two-dimensional materials

We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field microscope is itself an efficient polariton launcher. Our analysis reveals that the scanning tips are superior to other types of emitters we have investigated. Furthermore, the study of polariton emission and emission efficiency may provide insights for development of polaritonic devices and for fundamental studies of collective modes in other van der Waals materials.

cond-mat.mes-hall↗

arXiv2015

Graphene-Based Platform for Infrared Near-Field Nanospectroscopy of Water and Biological Materials in an Aqueous Environment

Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene. Large-area graphene acts as an impermeable monolayer barrier that allows for nano-IR inspection of underlying molecular materials in liquid. Here, we use s-SNOM to investigate the tobacco mosaic virus (TMV) in water underneath graphene. We resolve individual virus particles and register the amide I and II bands of TMV at ca. 1520 and 1660 cm$^{-1}$, respectively, using nanoscale Fourier transform infrared spectroscopy (nano-FTIR). We verify the presence of water in the graphene liquid cell by identifying a spectral feature associated with water absorption at 1610 cm$^{-1}$.

cond-mat.mes-hall↗

arXiv2014

Ultrafast and Nanoscale Plasmonic Phenomena in Exfoliated Graphene Revealed by Infrared Pump-Probe Nanoscopy

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ~20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 femtosecond (fs) time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.

cond-mat.mes-hall↗

arXiv2012

Mid-infrared frequency comb spanning an octave based on an Er fiber laser and difference-frequency generation

We describe a coherent mid-infrared continuum source with 700 cm-1 usable bandwidth, readily tuned within 600 - 2500 cm-1 (4 - 17 \mum) and thus covering much of the infrared "fingerprint" molecular vibration region. It is based on nonlinear frequency conversion in GaSe using a compact commercial 100-fs-pulsed Er fiber laser system providing two amplified near-infrared beams, one of them broadened by a nonlinear optical fiber. The resulting collimated mid-infrared continuum beam of 1 mW quasi-cw power represents a coherent infrared frequency comb with zero carrier-envelope phase, containing about 500,000 modes that are exact multiples of the pulse repetition rate of 40 MHz. The beam's diffraction-limited performance enables long-distance spectroscopic probing as well as maximal focusability for classical and ultraresolving near-field microscopies. Applications are foreseen also in studies of transient chemical phenomena even at ultrafast pump-probe scale, and in high-resolution gas spectroscopy for e.g. breath analysis.

quant-ph↗

arXiv2011

Infrared nanoscopy of Dirac plasmons at the graphene-SiO2 interface

We report on infrared (IR) nanoscopy of 2D plasmon excitations of Dirac fermions in graphene. This is achieved by confining mid-IR radiation at the apex of a nanoscale tip: an approach yielding two orders of magnitude increase in the value of in-plane component of incident wavevector q compared to free space propagation. At these high wavevectors, the Dirac plasmon is found to dramatically enhance the near-field interaction with mid-IR surface phonons of SiO2 substrate. Our data augmented by detailed modeling establish graphene as a new medium supporting plasmonic effects that can be controlled by gate voltage.

cond-mat.mes-hall↗