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- ItemPlasmon induced deprotonation of 2-mercaptopyridine(Cambridge : Royal Society of Chemistry, 2020) Singh P.; Deckert-Gaudig T.; Zhang Z.; Deckert V.Surface plasmons can provide a novel route to induce and simultaneously monitor selective bond formation and breakage. Here pH-induced protonation, followed by plasmon-induced deprotonation of 2-mercaptopyridine was investigated using surface- and tip-enhanced Raman scattering (SERS and TERS). A large difference in the deprotonation rate between SERS and TERS will be demonstrated and discussed with respect to hot-spot distribution. © 2020 The Royal Society of Chemistry.
- ItemMorpho-molecular ex vivo detection and grading of non-muscle-invasive bladder cancer using forward imaging probe based multimodal optical coherence tomography and Raman spectroscopy(Cambridge : Royal Society of Chemistry, 2020) Placzek F.; Cordero Bautista E.; Kretschmer S.; Wurster L.M.; Knorr F.; González-Cerdas G.; Erkkilä M.T.; Stein P.; Ataman Ç.; Hermann G.G.; Mogensen K.; Hasselager T.; Andersen P.E.; Zappe H.; Popp J.; Drexler W.; Leitgeb R.A.; Schie I.W.Non-muscle-invasive bladder cancer affects millions of people worldwide, resulting in significant discomfort to the patient and potential death. Today, cystoscopy is the gold standard for bladder cancer assessment, using white light endoscopy to detect tumor suspected lesion areas, followed by resection of these areas and subsequent histopathological evaluation. Not only does the pathological examination take days, but due to the invasive nature, the performed biopsy can result in significant harm to the patient. Nowadays, optical modalities, such as optical coherence tomography (OCT) and Raman spectroscopy (RS), have proven to detect cancer in real time and can provide more detailed clinical information of a lesion, e.g. its penetration depth (stage) and the differentiation of the cells (grade). In this paper, we present an ex vivo study performed with a combined piezoelectric tube-based OCT-probe and fiber optic RS-probe imaging system that allows large field-of-view imaging of bladder biopsies, using both modalities and co-registered visualization, detection and grading of cancerous bladder lesions. In the present study, 119 examined biopsies were characterized, showing that fiber-optic based OCT provides a sensitivity of 78% and a specificity of 69% for the detection of non-muscle-invasive bladder cancer, while RS, on the other hand, provides a sensitivity of 81% and a specificity of 61% for the grading of low- and high-grade tissues. Moreover, the study shows that a piezoelectric tube-based OCT probe can have significant endurance, suitable for future long-lasting in vivo applications. These results also indicate that combined OCT and RS fiber probe-based characterization offers an exciting possibility for label-free and morpho-chemical optical biopsies for bladder cancer diagnostics. © 2020 The Royal Society of Chemistry.
- ItemOptical and chemical control of the wettability of nanoporous photoswitchable films(Cambridge : Royal Society of Chemistry, 2022) Zhang, Zejun; Chen, Donghui; Mutruc, Dragos; Hecht, Stefan; Heinke, LarsWettability is a central surface property of functional thin films. Here, we present a nanoporous film made of an azobenzene-containing metal-organic framework material where the wettability is controlled by photoswitching of the fluorinated azobenzene moieties and by reversible incorporation of guest molecules with different polarities in the pores. Using both, the optical and the chemical stimuli, the water contact angle was modified over a wide range, from 23° to 97°.
- ItemShape-adaptive single-molecule magnetism and hysteresis up to 14 K in oxide clusterfullerenes Dy2O@C72 and Dy2O@C74 with fused pentagon pairs and flexible Dy-(μ2-O)-Dy angle(Cambridge : Royal Society of Chemistry, 2020) Velkos, G.; Yang, W.; Yao, Y.-R.; Sudarkova, S.M.; Liu, X.; Büchner, B.; Avdoshenko, S.M.; Chen, N.; Popov, A.A.Dysprosium oxide clusterfullerenes Dy2O@Cs(10528)-C72 and Dy2O@C2(13333)-C74 are synthesized and characterized by single-crystal X-ray diffraction. Carbon cages of both molecules feature two adjacent pentagon pairs. These pentalene units determine positions of endohedral Dy ions hence the shape of the Dy2O cluster, which is bent in Dy2O@C72 but linear in Dy2O@C74. Both compounds show slow relaxation of magnetization and magnetic hysteresis. Nearly complete cancelation of ferromagnetic dipolar and antiferromagnetic exchange Dy⋯Dy interactions leads to unusual magnetic properties. Dy2O@C74 exhibits zero-field quantum tunneling of magnetization and magnetic hysteresis up to 14 K, the highest temperature among Dy-clusterfullerenes.
- ItemA wafer-scale two-dimensional platinum monosulfide ultrathin film via metal sulfurization for high performance photoelectronics(Cambridge : Royal Society of Chemistry, 2022) Pang, Jinbo; Wang, Yanhao; Yang, Xiaoxin; Zhang, Lei; Li, Yufen; Zhang, Yu; Yang, Jiali; Yang, Feng; Wang, Xiao; Cuniberti, Gianaurelio; Liu, Hong; Rümmeli, Mark H.2D nonlayered materials have attracted enormous research interests due to their novel physical and chemical properties with confined dimensions. Platinum monosulfide as one of the most common platinum-group minerals has been less studied due to either the low purity in the natural product or the extremely high-pressure conditions for synthesis. Recently, platinum monosulfide (PtS) 2D membranes have emerged as rising-star materials for fundamental Raman and X-ray photoelectron spectral analysis as well as device exploration. However, a large-area homogeneous synthesis route has not yet been proposed and released. In this communication, we report a facile metal sulfurization strategy for the synthesis of a 4-inch wafer-scale PtS film. Enhanced characterization tools have been employed for thorough analysis of the crystal structure, chemical environment, vibrational modes, and atomic configuration. Furthermore, through theoretical calculations the phase diagram of the Pt–S compound has been plotted for showing the successful formation of PtS in our synthesis conditions. Eventually, a high-quality PtS film has been reflected in device demonstration by a photodetector. Our approach may shed light on the mass production of PtS films with precise control of their thickness and homogeneity as well as van der Waals heterostructures and related electronic devices.
- ItemLi+/H+ exchange of Li7La3Zr2O12 single and polycrystals investigated by quantitative LIBS depth profiling(Cambridge : Royal Society of Chemistry, 2022) Smetaczek, Stefan; Limbeck, Andreas; Zeller, Veronika; Ring, Joseph; Ganschow, Steffen; Rettenwander, Daniel; Fleig, JürgenLi7La3Zr2O12 (LLZO) garnets are highly attractive to be used as solid electrolyte in solid-state Li batteries. However, LLZO suffers from chemical interaction with air and humidity, causing Li+/H+ exchange with detrimental implication on its performance, processing and scalability. To better understand the kinetics of the detrimental Li+/H+ exchange and its dependence on microstructural features, accelerated Li+/H+ exchange experiments were performed on single crystalline and polycrystalline LLZO, exposed for 80 minutes to 80 °C hot water. The resulting chemical changes were quantified by analytical methods, i.e. inductively coupled plasma optical emission spectroscopy (ICP-OES) and laser induced breakdown spectroscopy (LIBS). From the time dependence of the Li+ enrichment in the water, measured by ICP-OES, a bulk interdiffusion coefficient of Li+/H+ could be determined (7 × 10−17 m2 s−1 at 80 °C). Depth dependent concentrations were obtained from the LIBS data for both ions after establishing a calibration method enabling not only Li+ but also H+ quantification in the solid electrolyte. Short interdiffusion lengths in the 1 μm range are found for the single crystalline Ga:LLZO, in accordance with the measured bulk diffusion coefficient. In polycrystalline Ta:LLZO, however, very long diffusion tails in the 20 μm range and ion exchange fractions up to about 70% are observed. Those are attributed to fast ion interdiffusion along grain boundaries. The severe compositional changes also strongly affect the electrical properties measured by impedance spectroscopy. This study highlights that microstructural effects may be decisive for the Li+/H+ ion exchange kinetics of LLZO.
- ItemFlexible and transparent electrodes imprinted from metal nanostructures: morphology and opto-electronic performance(Cambridge : Royal Society of Chemistry, 2022) Engel, Lukas F.; González-García, Lola; Kraus, TobiasWe directed the self-assembly of nanoscale colloids via direct nanoimprint lithography to create flexible transparent electrodes (FTEs) with metal line widths below 3 μm in a roll-to-roll-compatible process. Gold nanowires and nanospheres with oleylamine shells were imprinted with soft silicone stamps, arranged into grids of parallel lines, and converted into metal lines in a plasma process. We studied the hierarchical structure and opto-electronic performance of the resulting grids as a function of particle geometry and concentration. The performance in terms of optical transmittance was dominated by the line width. Analysis of cross-sections indicated that plasma sintering only partially removed the insulating ligands and formed lines with thin conductive shells and a non-conductive core. We provide evidence that the self-assembly of high-aspect nanowires can compensate for defects of the stamp and substrate irregularities during imprinting, while spheres cannot. The wire-based electrodes thus outperformed the sphere-based electrodes at ratios of optical transmittance to sheet resistance of up to ≈ 0.9% Ωsq−1, while spheres only reached ≈ 0.55% Ωsq−1
- ItemPorous spherical gold nanoparticles via a laser induced process(Cambridge : Royal Society of Chemistry, 2022) Schmidl, Gabriele; Raugust, Marc; Jia, Guobin; Dellith, Andrea; Dellith, Jan; Schmidl, Frank; Plentz, JonathanNanoparticles consisting of a mixture of several metals and also porous nanoparticles due to their special structure exhibit properties that find applications in spectroscopic detection or catalysis. Different approaches of top down or bottom up technologies exist for the fabrication of such particles. We present a novel combined approach for the fabrication of spherical porous gold nanoparticles on low-cost glass substrates under ambient conditions using a UV-laser induced particle preparation process with subsequent wet chemical selective etching. In this preparation route, nanometer-sized branched structures are formed in spherical particles. The laser process, which is applied to a silver/gold bilayer system with different individual layer thicknesses, generates spherical mixed particles in a nanosecond range and influences the properties of the fabricated nanoparticles, such as the size and the mixture and thus the spectral response. The subsequent etching process is performed by selective wet chemical removal of silver from the nanoparticles with diluted nitric acid. The gold to silver ratio was investigated by energy-dispersive X-ray spectroscopy. The porosity depends on laser parameters and film thickness as well as on etching parameters such as time. After etching, the surface area of the remaining Au nanoparticles increases which makes these particles interesting for catalysis and also as carrier particles for substances. Such substances can be positioned at defined locations or be released in appropriate environments. Absorbance spectra are also analyzed to show how the altered fractured shape of the particles changes localized plasmon resonances of the resultingt particles.
- ItemControlling optical trapping of metal–dielectric hybrid nanoparticles under ultrafast pulsed excitation: a theoretical investigation(Cambridge : Royal Society of Chemistry, 2021) Devi, Anita; Nair, Shruthi S.; Yadav, Sumit; De, Arijit K.Crucial to effective optical trapping is the ability to precisely control the nature of force/potential to be attractive or repulsive. The nature of particles being trapped is as important as the role of laser parameters in determining the stability of the optical trap. In this context, hybrid particles comprising of both dielectric and metallic materials offer a wide range of new possibilities due to their tunable optical properties. On the other hand, femtosecond pulsed excitation is shown to provide additional advantages in tuning of trap stiffness through harnessing optical and thermal nonlinearity. Here we demonstrate that (metal/dielectric hybrid) core/shell type and hollow-core type nanoparticles experience more force than conventional core-type nanoparticles under both continuous-wave and, in particular, ultrafast pulsed excitation. Thus, for the first time, we show how tuning both materials properties as well as the nature of excitation can impart unprecedented control over nanoscale optical trapping and manipulation leading to a wide range of applications.
- ItemReversible magnetism switching of iron oxide nanoparticle dispersions by controlled agglomeration(Cambridge : Royal Society of Chemistry, 2021) Müssig, Stephan; Kuttich, Björn; Fidler, Florian; Haddad, Daniel; Wintzheimer, Susanne; Kraus, Tobias; Mandel, KarlThe controlled agglomeration of superparamagnetic iron oxide nanoparticles (SPIONs) was used to rapidly switch their magnetic properties. Small-angle X-ray scattering (SAXS) and dynamic light scattering showed that tailored iron oxide nanoparticles with phase-changing organic ligand shells agglomerate at temperatures between 5 °C and 20 °C. We observed the concurrent change in magnetic properties using magnetic particle spectroscopy (MPS) with a temporal resolution on the order of seconds and found reversible switching of magnetic properties of SPIONs by changing their agglomeration state. The non-linear correlation between magnetization amplitude from MPS and agglomeration degree from SAXS data indicated that the agglomerates' size distribution affected magnetic properties.
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