Marc Brecht

• Prof. Dr. rer. nat.
• Professor (Full) at Reutlingen University

Cotton, the most widely produced natural fiber, is integral to the textile industry and sustains the livelihoods of millions worldwide. However, its quality is frequently compromised by contamination, particularly from honeydew, a substance secreted by insects that leads to the formation of sticky fibers, thereby impeding textile processing. This s...

Ultraviolet (UV) hyperspectral imaging shows significant promise for the classification and quality assessment of raw cotton, a key material in the textile industry. This study evaluates the efficacy of UV hyperspectral imaging (225–408 nm) using two different light sources: xenon arc (XBO) and deuterium lamps, in comparison to NIR hyperspectral im...

The use of surface-enhanced Raman spectroscopy (SERS) in liquid solutions has always been challenging due to signal fluctuations, inconsistent data, and difficulties in obtaining reliable results, especially at very low analyte concentrations. In our study, we introduce a new method using a three-dimensional (3D) SERS substrate made of silica micro...

Malignant primary brain tumors are a group of highly aggressive and often infiltrating tumors that lack adequate therapeutic treatments to achieve long time survival. Complete tumor removal is one precondition...

The peripherical protons of the dye molecule hypericin can undergo structural interconversion (tautomerization) between different isomers separated by a low energy barrier with rates that depends sensitively on the interaction with local chemical environment defined by the nature of host material. We investigate the deuterium (D) isotope effect of...

In the manufacturing process of electrical devices, ensuring the cleanliness of technical surfaces, such as direct bonded copper substrates, is crucial. An in-line monitoring system for quality checking must provide sufficiently resolved lateral data in a short time. UV hyperspectral imaging is a promising in-line method for rapid, contactless, and...

An analytic model is used to calculate the Raman and fluorescence enhancement of a molecule in between two closely spaced gold nanospheres. Instead of using the conventional approach that only the dipolar plasmonic mode is considered, we calculate the electric field enhancement in the nanometre sized gap, by taking account of the higher order modes...

Salivary gland tumors (SGTs) are a relevant, highly diverse subgroup of head and neck tumors whose entity determination can be difficult. Confocal Raman imaging in combination with multivariate data analysis may possibly support their correct classification. For the analysis of the translational potential of Raman imaging in SGT determination, a mu...

Malignant primary brain tumors are a group of highly aggressive and often infiltrating tumors that lack adequate therapeutic treatments to achieve long time survival. Complete tumor removal is one precondition to reach this goal. A promising approach to optimize resection margins and eliminate remaining infiltrative so-called guerilla cells is phot...

Monolithic columns, unlike conventional columns, are not packed with fully porous particles. Instead, they consist of a system of macropores and mesopores. Macropores with a size of a few micrometres increase the permeability so that the back pressure is significantly lower. Mesopores with a size of a few nanometers increase the surface area and th...

This study introduces a straightforward approach to construct three-dimensional (3D) surface-enhanced Raman spec-troscopy (SERS) substrates using chemically modified silica particles as microcarriers and by attaching metal nanoparticles (NPs) onto their surfaces. Tollens' reagent and sputtering techniques are utilized to prepare the SERS substrates...

Cotton contamination by honeydew is considered one of the significant problems for quality in textiles as it causes stickiness during manufacturing. Therefore, millions of dollars in losses are attributed to honeydew contamination each year. This work presents the use of UV hyperspectral imaging (225-300 nm) to characterize honeydew contamination o...

Due to the wide variety of benign and malignant salivary gland tumors, classification and malignant behavior determination based on histomorphological criteria can be difficult and sometimes impossible. Spectroscopical procedures can acquire molecular biological information without destroying the tissue within the measurement processes. Since sever...

UV hyperspectral imaging (225 nm–410 nm) was used to identify and quantify the honeydew content of real cotton samples. Honeydew contamination causes losses of millions of dollars annually. This study presents the implementation and application of UV hyperspectral imaging as a non-destructive, high-resolution, and fast imaging modality. For this no...

Surface-enhanced Raman spectroscopy (SERS) provides a strong enhancement to an inherently weak Raman signal, which strongly depends on the material, design, and fabrication of the substrate. Here, we present a facile method of fabricating a non-uniform SERS substrate based on an annealed thin gold (Au) film that offers multiple resonances and gap s...

Glioblastoma WHO IV belongs to a group of brain tumors that are still incurable. A promising treatment approach applies photodynamic therapy (PDT) with hypericin as a photosensitizer. To generate a comprehensive understanding of the photosensitizer-tumor interactions, the first part of our study is focused on investigating the distribution and pene...

Quantifying additives in filled plastic melts pushes near-infrared (NIR) spectroscopy to its limits. The light scattering of the fillers in the NIR range overlap the additive signals, which significantly affects the signal strength of the additives. Yet in order to implement a robust prediction of the additive content, the measurement range was ext...

In this research work, the possibilities and limitations of inline spectroscopy in different wavelength ranges for the determination of additive content in highly filled polymer melts were evaluated. Usually, additives can be well quantified in the near-infrared (NIR) wavelength range. In mineral-filled melts, however, the signal in the NIR range i...

Monodisperse porous poly(glycidyl methacrylate-co–ethylene glycol dimethacrylate) particles are widely applied in different fields, as their pore properties can be influenced and functionalization of the epoxy group is versatile. However, the adjustment of parameters which control morphology and pore properties such as pore volume, pore size and sp...

Hypericin tautomerization that involves the migration of the labile protons is believed to be the primary photophysical process relevant to its light-activated antiviral activity. Despite the difficulty to isolate individual tautomers, it can be directly observed in single-molecule experiments. We show that the tautomerization of single hypericin m...

Metalworking fluids (MWFs) are widely used to cool and lubricate metal workpieces during processing to reduce heat and friction. Extending a MWF’s service life is of importance from both economical and ecological points of view. Knowledge about the effects of processing conditions on the aging behavior and reliable analytical procedures are require...

The early detection of head and neck cancer is a prolonged challenging task. It requires a precise and accurate identification of tissue alterations as well as a distinct discrimination of cancerous from healthy tissue areas. A novel approach for this purpose uses microspectroscopic techniques with special focus on hyperspectral imaging (HSI) metho...

Hyperspectral imaging and reflectance spectroscopy in the range from 200–380 nm were used to rapidly detect and characterize copper oxidation states and their layer thicknesses on direct bonded copper in a non-destructive way. Single-point UV reflectance spectroscopy, as a well-established method, was utilized to compare the quality of the hyperspe...

A lens-based Raman spectrometer is characterized by studying the optical elements in the optical path and we study the measure of aberration-diffraction effects. This is achieved by measuring the spectral resolution (SR) thus encompassing almost all optical elements of a spectrometer that are mostly responsible for such effects. An equation for SR...

A laboratory prototype for hyperspectral imaging in ultra-violet (UV) region from 225 to 400 nm was developed and used to rapidly characterize active pharmaceutical ingredients (API) in tablets. The APIs are ibuprofen (IBU), acetylsalicylic acid (ASA) and paracetamol (PAR). Two sample sets were used for a comparison purpose. Sample set one comprise...

Hypericin has large potential in modern medicine and exhibits fascinating structural dynamics, such as multiple conformations and tautomerization. However, it is difficult to study individual conformers/tautomers, as they cannot be isolated due to the similarity of their chemical and physical properties. An approach to overcome this difficulty is t...

Monodisperse polystyrene spheres are functional materials with interesting properties, such as high cohesion strength, strong adsorptivity, and surface reactivity. They have shown a high application value in biomedicine, information engineering, chromatographic fillers, supercapacitor electrode materials, and other fields. To fully understand and t...

Characterization of brain tumours requires neuropathological expertise and is generally performed by histological evaluation and molecular analysis. One emerging technique to assist pathologists in future tumour diagnostics is multimodal optical spectroscopy. In the current clinical routine, tissue preprocessing with formalin is widely established...

We present the modification of ethylene-propylene rubber (EPM) with vinyltetra-methydisiloxane (VTMDS) via reactive extrusion to create a new silicone-based material with the potential for high-performance applications in the automotive, industrial and biomedical sectors. The radical-initiated modification is achieved with a peroxide catalyst start...

Tautomerization is a fundamental chemical reaction which involves the relocation of a proton in the reactants. Studying the optical properties of tautomeric species is challenging because of ensemble averaging. Many molecules, such as porphines, porphycenes, or phenanthroperylene quinones, exhibit a reorientation of the transition dipole moment (TD...

Different types of raw cotton were investigated by a commercial ultraviolet-visible/near infrared (UV-Vis/NIR) spectrometer (210–2200 nm) as well as on a home-built setup for NIR hyperspectral imaging (NIR-HSI) in the range 1100–2200 nm. UV-Vis/NIR reflection spectroscopy reveals the dominant role proteins, hydrocarbons and hydroxyl groups play in...

Some widely used optical measurement systems require a scan in wavelength or in one spatial dimension to measure the topography in all three dimensions. Novel hyperspectral sensors based on an extended Bayer pattern have a high potential to solve this issue as they can measure three dimensions in a single shot. This paper presents a detailed examin...

Tautomerization is a fast chemical reaction where structures of the reactants differ only in the position of a proton and a double bond. Tautomerization often occurs in natural substances and is a fundamental process in organic- and biochemistry. However, studying the optical properties of tautomeric species is challenging due to ensemble averaging...

Hypericin is one of the most efficient photosensitizers used in photodynamic tumor therapy (PDT). The reported treatments of this drug reach from antidepressive, antineoplastic, antitumor and antiviral activity. We show that hypericin can be optically detected down to a single molecule at ambient conditions. Hypericin can even be observed inside of...

The critical process parameters cell density and viability during mammalian cell cultivation are assessed by UV/VIS spectroscopy in combination with multivariate data analytical methods. This direct optical detection technique uses a commercial optical probe to acquire spectra in a label-free way without signal enhancement. For the cultivation, an...

Strong optical mode coupling between two adjacent λ/2 Fabry-Pérot microresonators consisting of three parallel silver mirrors is investigated experimentally and theoretically as a function of their detuning and coupling strength. Mode coupling can be precisely controlled by tuning the mirror spacing of one resonator with respect to the other by pie...

Hypericin can be found in nature in Hypericum perforatum (St. John's Wort) and has become subject of intense biochemical research. Studies report of antidepressive, antineoplastic, antitumor and antiviral activity of hypericin. Among the variety of potential applications hypericin can be used as photosensitizer in photodynamic therapy (PDT), where...

Optical half-wave microresonators enable to control the optical mode density around a quantum system and thus to modify the temporal emission properties. If the coupling rate exceeds the damping rate, strong coupling between a microresonator and a quantum system can be achieved, leading to a coherent energy exchange and the creation of new hybrid m...

Cotton is the most important raw material for the production of fabrics in the world. Since cotton is a natural product, it shows high variance in a quality issue of raw cotton with impurities and the most relevant impurities is Honeydew. Honeydew is a sugar-rich excretion of aphids (figure 1) and whiteflies (figure 2) causing stickiness of raw co...

Embedded in a tuneable λ/2-FabryPérot micro-resonator the radiative relaxation of a dye molecule or quantum dot can reproducibly be modified allowing to determine their quantum yield, control Förster energy-transfer or localize them with nanometer precision.

Turbidity sensing is very common in the control of drinking water. Furthermore, turbidity measurements are applied in the chemical (e.g., process monitoring), pharmaceutical (e.g., drug discovery), and food industries (e.g., the filtration of wine and beer). The most common measurement technique is nephelometric turbidimetry. A nephelometer is a de...

The fluorescence of monomeric photosystem II core complexes (mPSIIcc) of the cyanobacterium Thermosynechococcus elongatus, originating from redissolved crystals, is investigated by using single-molecule spectroscopy (SMS) at 1.6 K. The emission spectra of individual mPSIIcc are dominated by sharp zero-phonon lines, showing the existence of differen...

A facile method is described to prepare micron partly hollow dumbbell silica particles in a single step. The obtained particles consist of a large dense part and a small hollow lobe. The spherical dense core as well as the hollow lobe are covered by mesoporous channels. In the case of the smaller lobe these channels are responsible for the permeabi...

Using a Fabry-Pérot-microresonator with controllable cavity lengths in the λ/2-regime, we show the controlled modification of the vibronic relaxation dynamics of a fluorescent dye molecule in the spectral and time domain. By altering the photonic mode density around the fluorophores we are able to shape the fluorescence spectrum and enhance specifi...

Here we report a simple way to enhance the resolution of a confocal scanning microscope under cryogenic conditions. Using a microscope objective (MO) with high numerical aperture (NA = 1.25) and 1-propanol as an immersion fluid with low freezing temperature we were able to reach an imaging resolution at 160 K comparable to ambient conditions. The M...

Single-molecule spectroscopy at low temperature was used to study the spectral properties, heterogeneities and spectral dynamics of the chlorophyll a (Chl a) molecules responsible for the fluorescence emission of photosystem I monomers (PS I-M) from the cyanobacterium Thermosynechococcus elongatus. The fluorescence spectra of sin- gle PS I-M are do...

The fluorescence of photosystem I (PSI) trimers in proximity to bimetallic plasmonic nanostructures have been explored by single-molecule spectroscopy (SMS) at cryogenic temperature (1.6 K). PSI serves as a model for biological multichromophore-coupled systems with high potential for biotechnological applications. Plasmonic nanostructures are fabri...

A major aim in experimental nano- and quantum optics is observing and controlling the interaction between light and matter on a microscopic scale. Coupling molecules or atoms to optical microresonators is a prominent method to alter their optical properties such as luminescence spectra or lifetimes. Until today strong coupling of optical resonators...

In this study we examined the energy transfer dynamics of a FRET coupled pair of chromophores at the single molecule level embedded in a tunable sub-wavelength Fabry-Pérot resonator with two silver mirrors and separations in the λ/2 region. By varying the spectral mode density in the resonator via the mirror separation we alter the radiative relaxa...

The spectral properties and dynamics of the fluorescence emission of photosystem II core complexes are investigated by single molecule spectroscopy at 1.6 K. The emission spectra are dominated by sharp zero-phonon lines (ZPLs). The sharp ZPLs are the result of weak to intermediate exciton-vibrational coupling and slow spectral diusion. For several...

Single-molecule spectroscopy has become a major tool to investigate molecular properties with an outstanding sensitivity. Moreover, ensemble averaging, which is inevitable in any other techniques, is circumvented by these techniques. Thus, fascinating insights into the interaction of a single molecule with its chemical nano-environment are obtained...

The structural organization of photosystem I (PSI) complexes in cyanobacteria and the origin of the PSI anten na long�wavelength chlorophylls and their role in energy migration, charge separation, and dissipation of excess absorbed energy are discussed. The PSI complex in cyanobacterial membranes is organized preferentially as a trimer with the cor...

We demonstrate controlled modification of the fluorescence and energy transfer properties of Photosystem I (PSI) - one of the most important light harvesting systems - by using a newly developed approach to produce optical subwavelength microcavities for cryogenic temperature issues. The experiments were carried out on PSI from the cyanobacterium A...

In Photosystem I (PS I) long-wavelength chlorophylls (LWC) of the core antenna are known to extend the spectral region up to 750 nm for absorbance of light that drives photochemistry. Here we present clear evidence that even far-red light with wavelengths beyond 800 nm, clearly outside the LWC absorption bands, can still induce photochemical charge...

In this study we use a combination of absorption, fluorescence and low temperature single-molecule spectroscopy to elucidate the spectral properties, heterogeneities and dynamics of the chlorophyll a (Chla) molecules responsible for the fluorescence emission of photosystem II core complexes (PS II cc) from the cyanobacterium Thermosynechococcus elo...

The accumulation of organic co-solvents in cells is a basic strategy for organisms from various species to increase stress tolerance in extreme environments. Widespread representatives of this class of co-solvents are trimethylamine-N-oxide (TMAO) and betaine; these small molecules are able to stabilize the native conformation of proteins and preve...

While single-molecule fluorescence from emitters with high quantum efficiencies such as organic dye molecules can easily be detected by modern apparatus, many less efficient emission processes such as Raman scattering and metal luminescence require dramatic enhancement to exceed the single-particle detection limit. This enhancement can be achieved...

In this study we demonstrate the impact of temperature on the luminescence emission of plasmonic nanoparticles. We examine the optical properties of single gold nanorods (GNRs) in the temperature range 1.6–295 K by confocal microscopy. Decreasing temperature leads to a reduction of the full width at half-maximum (fwhm) of the luminescence spectra,...

The construction of a microscope with fast sample transfer system for single-molecule spectroscopy and microscopy at low temperatures using 2D/3D sample-scanning is reported. The presented construction enables the insertion of a sample from the outside (room temperature) into the cooled (4.2 K) cryostat within seconds. We describe the mechanical an...

Single-molecule spectroscopy has been used to investigate the plasmonic interaction effects of nanometer-sized hexagonal arrays of Au- and Ag-triangles on the fluorescence properties of photosystem I (PSI) – a key component of the photosynthetic apparatus. The fluorescence emission of PSI is intensified upon coupling with these nanostructures. For...

The plasmonic interaction effects of various nanostructures on the fluorescence properties of photosystem I as found by single-molecule spectroscopy are summarized. The used nanostructures are spherical Au nanoparticles, silver island films as well as hexagonal arrays of nanometer-sized Au- and Ag-triangles (the Fischer patterns). The fluorescence...

Single-molecule fluorescence spectroscopy at 1.4K was used to investigate the spectral properties of red (long-wavelength) chlorophylls in trimeric Photosystem I (PSI) complexes from the cyanobacterium Arthrospira platensis. Three distinct red antenna states could be identified in the fluorescence spectra of single PSI trimers from A. platensis in...

Photosystem I of cyanobacteria contains different spectral pools of chlorophylls called red or long-wavelength chlorophylls that absorb at longer wavelengths than the primary electron donor P700. We measured the fluorescence spectra at the ensemble and the single-molecule level at low temperatures in the presence of oxidized and reduced P700. In ac...

The interaction between glycerol and photosystem I (PSI) was investigated using low temperature single-molecule spectroscopy. PSI complexes were dissolved in three different solutions: in buffer solution, in 66% glycerol/buffer solution, and in 66% glycerol/buffer solution that was afterwards diluted by buffer; the final glycerol concentration was...

Single-molecule spectroscopy at cryogenic temperatures was used to examine the impact of buffer solution, glycerol/buffer mixtures (25% and 66%), and poly(vinyl alcohol) (PVA) films on the conformation of photosystem I (PSI) from Thermosynechoccocus elongatus. PSI holds a number of chromophores embedded at different places within the protein comple...

Influencing proteins: A protein multichromophore system (photosystem I) is exposed to gold nanoparticles (NPs) and silver island films. In the presence of these nanostructures an altered fluorescence response of the chromophores is observed (see scheme), indicating a change in the protein function. A model to understand these plasmonic effects is g...

The geometric and electronic structures of the active sites in the oxidized Ni(r)-B state of the [NiFe] hydrogenases from Ralstonia eutropha H16 and Desulfovibrio vulgaris Miyazaki F were investigated in pulsed EPR and ENDOR experiments at two different microwave frequencies (X- and Q-band). Two hyperfine-couplings were clearly resolved in the froz...

Progress in the field of single-molecule techniques has yielded enormous possibilities for studying photosynthetic pigment–protein complexes. The aim of this review is to present recent developments in spectroscopy on single photosystem I (PSI) complexes. The fluorescence emission of PSI is composed of the contributions of several chlorophyll a (Ch...

Strong anticorrelation between the fluorescence emission of different emitters is observed by employing single-molecule fluorescence spectroscopy on photosystem I at cryogenic temperatures. This anticorrelation demonstrates a time-dependent interaction between pigments participating in the exciton transfer chain, implying that uniquely defined ener...

Low temperature single-molecule fluorescence emission spectroscopy on individual phytochromes from Agrobacterium tumefaciens corroborates findings from ensemble spectroscopy concerning intercomplex heterogeneity. Furthermore, time-dependent intracomplex heterogeneity has been observed.

Electron and energy transfer in proteins are key processes in bioenergetics. Their understanding on a molecular level can serve as an important guideline for the design of nanoscale assemblies. Energy transfer between pigment molecules requires a match between their transition energies for energy emission and absorption. The tuning of these pigment...

The fluorescence emission of individual photosystem I complexes from Synechocystis PCC 6803 in protonated and deuterated buffer shows zero-phonon lines as well as broad intensity distributions. The number and the line width of the zero phonon lines depend strongly on the solvent (H(2)O/D(2)O). The spectral diffusion rate of the whole fluorescence e...

Single-molecule spectroscopy at low temperatures was used to elucidate spectral properties, heterogeneities, and dynamics of the red-shifted chlorophyll a (Chl a) molecules responsible for the fluorescence from photosystem I (PSI). Emission spectra of single PSI complexes from the cyanobacterium Synechocystis PCC 6803 show zero-phonon lines (ZPLs)...

Absorption, fluorescence and single-molecule spectroscopy at low temperatures were used to elucidate spectral properties, heterogeneities and dynamics of the red-shifted chlorophyll a (Chla) molecules responsible for the fluorescence in photosystem I (PSI) from the cyanobacterium Synechoccocus sp. PCC 7002. The 77 K absorption spectrum indicates th...

Single-molecule spectroscopy at cryogenic temperatures was used to elucidate spectral properties, heterogeneities, and dynamics of the chlorophyll a (Chla) molecules responsible for the fluorescence in photosystem I (PSI) from the cyanobacteria Thermosynechococcus elongatus. Absorption and hole burning data suggest the presence of three pools absor...

Photosystem I reaction centers of the cyanobacterium Thermosynechococcus elongatus have been investigated using single-molecule spectroscopy. Single-molecule fluorescence emission spectra reveal a new fluorescence band located at 745 nm. Fluorescence polarization spectroscopy and fluorescence autocorrelation analysis show that only a few chlorophyl...

The catalytic center of the [NiFe] hydrogenase of Desulfovibrio vulgaris Miyazaki F in the oxidized states was investigated by electron paramagnetic resonance and electron-nuclear double resonance spectroscopy applied to single crystals of the enzyme. The experimental results were compared with density functional theory (DFT) calculations. For the...