Nanoscale quantum emitters are key elements in quantum optics and sensing. However, efficient optical excitation and detection of such emitters involves large solid angles because their interaction ...with freely propagating light is omnidirectional. Here, we present unidirectional emission of a single emitter by coupling to a nanofabricated Yagi-Uda antenna. A quantum dot is placed in the near field of the antenna so that it drives the resonant feed element of the antenna. The resulting quantum-dot luminescence is strongly polarized and highly directed into a narrow forward angular cone. The directionality of the quantum dot can be controlled by tuning the antenna dimensions. Our results show the potential of optical antennas to communicate energy to, from, and between nano-emitters.
Label-free biosensing based on metallic nanoparticles supporting localized surface plasmon resonances (LSPR) has recently received growing interest (Anker, J. N., et al. Nat. Mater. 2008, 7, ...442–453). Besides its competitive sensitivity (Yonzon, C. R., et al. J. Am. Chem. Soc. 2004, 126, 12669–12676; Svendendahl, M., et al. Nano Lett. 2009, 9, 4428–4433) when compared to the surface plasmon resonance (SPR) approach based on extended metal films, LSPR biosensing features a high-end miniaturization potential and a significant reduction of the interrogation device bulkiness, positioning itself as a promising candidate for point-of-care diagnostic and field applications. Here, we present the first, paralleled LSPR lab-on-a-chip realization that goes well beyond the state-of-the-art, by uniting the latest advances in plasmonics, nanofabrication, microfluidics, and surface chemistry. Our system offers parallel, real-time inspection of 32 sensing sites distributed across 8 independent microfluidic channels with very high reproducibility/repeatability. This enables us to test various sensing strategies for the detection of biomolecules. In particular we demonstrate the fast detection of relevant cancer biomarkers (human alpha-feto-protein and prostate specific antigen) down to concentrations of 500 pg/mL in a complex matrix consisting of 50% human serum.
In this study, we report on ultrasensitive protein detection with lithographically prepared plasmonic nanostructures. We have engineered optical nanosensors by the combined approach of negative ...resist, electron beam lithography, and reactive ion etching to form highly reproducible arrays of gold dimers in which the near-field coupling in their subwavelength gap enables for scaling the sensing volume down to the single-protein scale. In good agreement with recent theoretical predictions, the dimer geometry offers enhanced sensitivity compared to isolated particles for the detection of both small organic molecules and proteins. Beyond, by exploiting size exclusion, we are capable of monitoring the number of proteins able to bind across the gap region through the precise engineering of the structures coupled to the selective binding of a surface-assembled monolayer and covalent attachment of the protein.
Background/objectives:
Repetitive transcranial magnetic stimulation (rTMS) has been established as an effective therapeutic intervention for the treatment of depression. Preliminary data suggest that ...the efficacy of rTMS is reduced in patients taking benzodiazepines (BZD). Here, we use real-world data from a large sample to investigate the influence of lorazepam on the effectiveness of rTMS.
Methods
From a retrospective cohort of clinically depressed patients that were treated with rTMS, we compared 176 patients not taking any BZD with 73 patients taking lorazepam with respect to changes in the Hamilton Depression Rating Scale (HRDS).
Results
Both groups improved during rTMS according to HRDS scores, but the amelioration of symptoms was significantly less pronounced in patients taking lorazepam (18% vs. 38% responders in the non-lorazepam group). We could not see any association of intake regimen of lorazepam with response in rTMS.
Conclusion
Our observational study suggests that intake of lorazepam impedes the response to rTMS. The impact of lorazepam and other BZD on rTMS should receive more attention and be further investigated in prospective, hypothesis-based treatment studies to determine causal relationships between medication treatments and outcome. This could lead to specific recommendations for pharmacological treatment for depressed patients undergoing rTMS.
The kinetics of UV radiation-induced fast collapse and recovery in thermally cycled and rehydrated light- and thermo- double-responsive copolymer films of poly(oligo(ethylene glycol) methyl ether ...methacrylate-co-6-(4-phenylazophenoxy)hexyl acrylate), abbreviated as P(OEGMA300-co-PAHA), are probed by in situ neutron reflectivity (NR). The copolymer film is exposed to a thermal treatment starting at a temperature of 60 °C, which is well above its transition temperature (TT = 53 °C) before the temperature is rapidly decreased from 60 to 23 °C. Based on the applied protocol, the initially collapsed P(OEGMA300-co-PAHA) film is rehydrated due to the switching of polymer chains from a more hydrophobic to a more hydrophilic state when the temperature falls below its TT. The whole rehydration process can be divided into 3 stages: D2O absorption, chain rearrangement, and film reswelling. After rehydration, the thermally cycled P(OEGMA300-co-PAHA) film is switched by UV irradiation via setting the UV radiation on and off. Considering the UV-induced collapse and recovery, both processes are slower than those observed in freshly hydrated films without any thermal stimulus history. Therefore, the experienced thermal history of the film should be considered in the design of sensors and detectors based on double-responsive copolymer films.
The swelling and co-nonsolvency behaviors in pure H2O and in a mixed H2O/CH3OH vapor atmosphere of two different polar, water-soluble polymers in thin film geometry are studied in situ. Films of a ...zwitterionic poly(sulfobetaine), namely, poly3-((2-(methacryloyloxy)ethyl)dimethylammonio) propane-1-sulfonate (PSPE), and a polar nonionic polymer, namely, poly(N-isopropylmethacrylamide) (PNIPMAM), are investigated in real time by spectral reflectance (SR) measurements and Fourier transform infrared (FTIR) spectroscopy. Whereas PSPE is insoluble in methanol, PNIPMAM is soluble but exhibits co-nonsolvency behavior in water/methanol mixtures. First, the swelling of PSPE and PNIPMAM thin films in H2O vapor is followed. Subsequently, CH3OH is added to the vapor atmosphere, and its contracting effect on the water-swollen films is monitored, revealing a co-nonsolvency-type behavior for PNIPMAM and PSPE. SR measurements indicate that PSPE and PNIPMAM behave significantly different during the H2O swelling and subsequent exposure to CH3OH, not only with respect to the amounts of absorbed water and CH3OH, but also to the cosolvent-induced contraction mechanisms. While PSPE thin films exhibit an abrupt one-step contraction, the contraction of PNIPMAM thin films occurs in two steps. FTIR studies corroborate these findings on a molecular scale and reveal the role of the specific functional groups, both during the swelling and the cosolvent-induced switching of the solvation state.
The swelling and phase transition behavior upon increasing temperature of a doubly thermoresponsive diblock copolymer thin film in steps above the characteristic cloud points (CPs) of the blocks is ...studied. An upper critical solution temperature (UCST)-type zwitterionic poly(sulfobetaine), poly(N,N-dimethyl-N-(3-methacrylamidopropyl)-ammoniopropane sulfonate) (PSPP, CPUCST = 31.5 °C), is combined with a lower critical solution temperature (LCST)-type nonionic poly(N-isopropyl-/methacrylamide) (PNIPMAM, CPLCST = 49.5 °C) block. Using time-of-flight neutron reflectivity (ToF-NR), we observe the swelling in D2O vapor at a constant temperature of 20 °C, followed by two subsequent temperature jumps, from 20 to 40 °C (above CPUCST) and from 40 to 60 °C (above CPLCST). The observed response of the diblock copolymer films deviates from the aqueous solution behavior, which is mainly attributed to the increased polymer concentration. Temperature-induced changes in the thin-film nanostructure are investigated with ToF grazing-incidence small-angle neutron scattering (GISANS). Alterations in the chain conformation and hydrogen bonding are probed by Fourier transform infrared (FTIR) spectroscopy. The ionic SO3 – groups (in the PSPP block) and the nonionic hydrophilic amide groups (in both blocks) are found to affect the mechanisms of D2O uptake and release significantly.
Perovskite solar cells (PSCs) have been developed as a promising photovoltaic technology because of their excellent photovoltaic performance. However, interfacial recombination and charge carrier ...transport losses at the surface greatly limit the performance and stability of PSCs. In this work, the fabrication of high-quality PSCs based on methylammonium lead iodide with excellent ambient stability is reported. An anionic surfactant, sodium dodecylbenzene sulfonate (SDBS), is introduced to simultaneously passivate the defect states and stabilize the cubic phase of the perovskite film. The SDBS located at grain boundaries and the surface of the active layer can effectively passivate under-coordinated lead ions and protect the perovskite components from water-induced degradation. As a result, a champion power conversion efficiency (PCE) of 19.42% is achieved with an open-circuit voltage (V OC) of 1.12 V, a short-circuit current (J SC) of 23.23 mA cm–2, and a fill factor (FF) of 74% in combination with superior moisture stability. The SDBS-passivated devices retain 80% of their initial average PCE after 2112 h of storage under ambient conditions.
The ligand exchange process is a key step in fabrications of quantum dot (QD) optoelectronic devices. In this work, on the basis of grazing incidence X-ray scattering techniques, we find that the ...ligand exchange process with halide ions changes the PbS QD superlattice from face-centered-cubic to body-centered-cubic stacking, while the QD crystal lattice orientation also changes from preferentially “edge-up” to “corner-up”. Thus, the QDs’ shape is supposed to be the main factor for the alignment of QDs in close packed solids. Moreover, we tailor the alignment of the close packed solids by thermal treatments and further investigate their inner charge carrier dynamics by pump–probe transient absorption experiments. An overall better structure alignment optimizes the charge carrier hopping rate, as confirmed by the time dependence of the photon bleaching peak shift. The QD solid treated at 100 °C shows the best inner structure alignment with the best charge carrier hopping rate.
Plasmonic antennas are key elements to control the luminescence of quantum emitters. However, the antenna's influence is often hidden by quenching losses. Here, the luminescence of a quantum dot ...coupled to a gold dimer antenna is investigated. Detailed analysis of the multiply excited states quantifies the antenna's influence on the excitation intensity and the luminescence quantum yield separately.
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