Universität Stuttgart
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Item Open Access Long-term stability of capped and buffered palladium-nickel thin films and nanostructures for plasmonic hydrogen sensing applications(2013) Strohfeldt, Nikolai; Tittl, Andreas; Giessen, HaraldOne of the main challenges in optical hydrogen sensing is the stability of the sensor material. We found and studied an optimized material combination for fast and reliable optical palladium-based hydrogen sensing devices. It consists of a palladium-nickel alloy that is buffered by calcium fluoride and capped with a very thin layer of platinum. Our system shows response times below 10 s and almost no short-term aging effects. Furthermore, we successfully incorporated this optimized material system into plasmonic nanostructures, laying the foundation for a stable and sensitive hydrogen detector.Item Open Access Surface- and tip-enhanced resonant Raman scattering from CdSe nanocrystals(2015) Sheremet, Evgeniya; Milekhin, Alexander G.; Rodriguez, Raul D.; Weiss, Thomas; Nesterov, Maxim; Rodyakina, Ekaterina E.; Gordan, Ovidiu D.; Sveshnikova, Larisa L.; Duda, Tatyana A.; Gridchin, Victor A.; Dzhagan, Volodymyr M.; Hietschold, Michael; Zahn, Dietrich R. T.Surface- and tip-enhanced resonant Raman scattering (resonant SERS and TERS) by optical phonons in a monolayer of CdSe quantum dots (QDs) is demonstrated. The SERS enhancement was achieved by employing plasmonically active substrates consisting of gold arrays with varying nanocluster diameters prepared by electron-beam lithography. The magnitude of the SERS enhancement depends on the localized surface plasmon resonance (LSPR) energy, which is determined by the structural parameters. The LSPR positions as a function of nanocluster diameter were experimentally determined from spectroscopic micro-ellipsometry, and compared to numerical simulations showing good qualitative agreement. The monolayer of CdSe QDs was deposited by the Langmuir–Blodgett-based technique on the SERS substrates. By tuning the excitation energy close to the band gap of the CdSe QDs and to the LSPR energy, resonant SERS by longitudinal optical (LO) phonons of CdSe QDs was realized. A SERS enhancement factor of 2 × 10 3 was achieved. This allowed the detection of higher order LO modes of CdSe QDs, evidencing the high crystalline quality of QDs. The dependence of LO phonon mode intensity on the size of Au nanoclusters reveals a resonant character, suggesting that the electromagnetic mechanism of the SERS enhancement is dominant. Finally, the resonant TERS spectrum from CdSe QDs was obtained using electrochemically etched gold tips providing an enhancement on the order of 10 4 . This is an important step towards the detection of the phonon spectrum from a single QD.Item Open Access Short-range surface plasmonics: localized electron emission dynamics from a 60-nm spot on an atomically flat single-crystalline gold surface(2017) Frank, Bettina; Kahl, Philip; Podbiel, Daniel; Spektor, Grisha; Orenstein, Meir; Fu, Liwei; Weiss, Thomas; Horn-von Hoegen, Michael; Davis, Timothy J.; Meyer zu Heringdorf, Frank-Joachim; Giessen, HaraldItem Open Access Nearly diffraction limited FTIR mapping using an ultrastable broadband femtosecond laser tunable from 1.33 to 8 µm(2017) Mörz, Florian; Semenyshyn, Rostyslav; Steinle, Tobias; Neubrech, Frank; Zschieschang, Ute; Klauk, Hagen; Steinmann, Andy; Giessen, HaraldMicro-Fourier-transform infrared (FTIR) spectroscopy is a widespread technique that enables broadband measurements of infrared active molecular vibrations at high sensitivity. SiC globars are often applied as light sources in tabletop systems, typically covering a spectral range from about 1 to 20 µm (10 000 - 500 cm−1) in FTIR spectrometers. However, measuring sample areas below 40x40 µm2 requires very long integration times due to their inherently low brilliance. This hampers the detection of ultrasmall samples, such as minute amounts of molecules or single nanoparticles. In this publication we extend the current limits of FTIR spectroscopy in terms of measurable sample areas, detection limit and speed by utilizing a broadband, tabletop laser system with MHz repetition rate and femtosecond pulse duration that covers the spectral region between 1250 - 7520 cm−1 (1.33 - 8 µm). We demonstrate mapping of a 150x150 µm2 sample of 100 nm thick molecule layers at 1430 cm−1 (7 µm) with 10x10 µm2 spatial resolution and a scan speed of 3.5 µm/sec. Compared to a similar globar measurement an order of magnitude lower noise is achieved, due to an excellent long-term wavelength and power stability, as well as an orders of magnitude higher brilliance.Item Open Access Tailoring enhanced optical chirality : design principles for chiral plasmonic nanostructures(2012) Schäferling, Martin; Dregely, Daniel; Hentschel, Mario; Giessen, HaraldElectromagnetic fields with strong optical chirality can be formed in the near-field of chiral plasmonic nanostructures. We calculate and visualize the degree of chirality to identify regions with relatively high values. This leads to design principles for a simple utilization of chiral fields. We investigate planar geometries which offer a convenient way to access the designated fields as well as three-dimensional nanostructures which show a very high local optical chirality.Item Open Access Highly ordered LB films of DHAP : a donor acceptor substituted polyene(1993) Schmelzer, Michael; Roth, Siegmar; Niesert, Claus-Peter; Effenberger, Franz; Li, Rui ChengThe donor acceptor substituted polyene 5-(4-dihexadecylaminophenyl)-2-methyl-2,4-pentadienal (DHAP) is - due to its amphiphilic nature - a promising candidate for the Langmuir-Blodgett (LB) technique. The molecule was studied as a monolayer on a pure water surface under argon atmosphere. Monolayers and multilayers were transfered onto solid support. The films showed a high degree of order in the monolayer as well as in thick multilayers. LB films were investigated with polarisation dependent UV/VIS absorption spectroscopy. The film spectra showed additional absorption peaks which were not present in the spectra of the molecules in solution. The relative peak intensities were highly dependent on the orientation of the electric field vector with respect to the substrate normal. To get a detailed picture of the arrangement of the films on the molecular level, we studied the polarisation dependence of the FTIR spectra in different experimental set-ups. The spectra showed a perpendicular orientation of the conjugated system with respect to the substrate, whereas the backbone of the saturated hydrocarbon chains showed a medium tilt angle of 20.0° with respect to the substrate normal. X-ray small angle diffraction measurements were applied to investigate the thickness of the LB layers. From the position of the Bragg peaks, a thickness of 5.45 nm per bilayer can be calculated, in agreement with a bilayer model showing different molecular alignment of the molecules transferred during upstroke and downstroke.Item Open Access Linear refractive index and absorption measurements of nonlinear optical liquids in the visible and near-infrared spectral region(2012) Kedenburg, Stefan; Vieweg, Marius; Gissibl, Timo; Giessen, HaraldLiquid-filled photonic crystal fibers and optofluidic devices require infiltration with a variety of liquids whose linear optical properties are still not well known over a broad spectral range, particularly in the near infrared. Hence, dispersion and absorption properties in the visible and near-infrared wavelength region have been determined for distilled water, heavy water, chloroform, carbon tetrachloride, toluene, ethanol, carbon disulfide, and nitrobenzene at a temperature of 20 °C. For the refractive index measurement a standard Abbe refractometer in combination with a white light laser and a technique to calculate correction terms to compensate for the dispersion of the glass prism has been used. New refractive index data and derived dispersion formulas between a wavelength of 500 nm and 1600 nm are presented in good agreement with sparsely existing reference data in this wavelength range. The absorption coefficient has been deduced from the difference of the losses of several identically prepared liquid filled glass cells or tubes of different lengths. We present absorption data in the wavelength region between 500 nm and 1750 nm.Item Open Access Photo-excited dynamics in the excitonic insulator Ta2NiSe5(2018) Werdehausen, Daniel; Takayama, Tomohiro; Albrecht, Gelon; Lu, Yangfan; Takagi, Hidenori; Kaiser, StefanThe excitonic insulator is an intriguing correlated electron phase formed of condensed excitons. A promising candidate is the small band gap semiconductor Ta2NiSe5. Here we investigate the quasiparticle and coherent phonon dynamics in Ta2NiSe5 in a time resolved pump probe experiment. Using the models originally developed by Kabanov et al for superconductors (Kabanov et al 1999 Phys. Rev. B 59 1497), we show that the material’s intrinsic gap can be described as almost temperature independent for temperatures up to about 250 K to 275 K. This behavior supports the existence of the excitonic insulator state in Ta2NiSe5. The onset of an additional temperature dependent component to the gap above these temperatures suggests that the material is located in the BEC-BCS crossover regime. Furthermore, we show that this state is very stable against strong photoexcitation, which reveals that the free charge carriers are unable to effectively screen the attractive Coulomb interaction between electrons and holes, likely due to the quasi 1D structure of Ta2NiSe5.Item Open Access Broadly tunable femtosecond near- and mid-IR source by direct pumping of an OPA with a 41.7 MHz Yb:KGW oscillator(2013) Krauth, Joachim; Steinmann, Andy; Hegenbarth, Robin; Conforti, Matteo; Giessen, HaraldWe generate over half a watt of tunable near-IR (1380-1830 nm) and several hundred milliwatts in the mid-IR (2.4-4.2 µm) as well as milliwatt level mid-IR (4.85-9.33 µm) femtosecond radiation by pumping an optical parametric amplifier directly with a 7.4 W Yb:KGW oscillator at 41.7 MHz repetition rate. We use 5 mm PPLN and 2 mm GaSe as downconversion crystals and seed this process by a supercontinuum from a tapered fiber. The system is extremely simple and very stable and could replace more complex OPOs as tunable light sources.Item Open Access Watt-level optical parametric amplifier at 42 MHz tunable from 1.35 to 4.5 μm coherently seeded with solitons(2014) Steinle, Tobias; Steinmann, Andy; Hegenbarth, Robin; Giessen, HaraldWe report on an optical parametric amplifier at high repetition rate of 41.7 MHz seeded by an optical soliton from a tapered fiber. Gap-free signal tuning from 1.35 µm to 1.95 µm with corresponding idler wavelengths from 2.2 µm to 4.5 µm is demonstrated. The system provides up to 1.8 W average power at 1.4 µm, more than 1.1 W up to 1.7 µm, and more than 400 mW up to 4.0 µm with a signal pulse duration of 200 to 300 fs. It is directly pumped by a solid-state oscillator providing up to 7.4 W at 1.04 µm wavelength with 425 fs pulse duration. Soliton-seeding is shown to lead to excellent pulse-to-pulse stability, but it introduces a timing-jitter on the millisecond timescale. Using a two-stage concept the timing-jitter is efficiently suppressed due to the passive synchronization of both conversion stages.