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Dynamic Ligand Surface Chemistry of Excited PbS Quantum Dots
摘要： The ligand shell around colloidal quantum dots mediates the electron and energy transfer processes that underpin their use in optoelectronic and photocatalytic applications. Here, we show that the surface chemistry of carboxylate anchoring groups of oleate ligands passivating PbS quantum dots undergoes significant changes when the quantum dots are excited to their excitonic states. We directly probe the changes of surface chemistry using time-resolved mid-infrared spectroscopy that records the evolution of the vibrational frequencies of carboxylate groups following excitation of the electronic states. The data reveal a reduction of the Pb?O coordination of carboxylate anchoring groups to lead atoms at the quantum dot surfaces. The dynamic surface chemistry of the ligands may increase their surface mobility in the excited state and enhance the ability of molecular species to penetrate the ligand shell to undergo energy and charge transfer processes that depend sensitively on distance.
关键词： surface chemistry,PbS quantum dots,ligand shell,colloidal quantum dots,time-resolved mid-infrared spectroscopy
更新于2025-09-19 17:13:59
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Modeling Equilibrium Binding at Quantum Dot Surfaces Using Cyclic Voltammetry
摘要： Cyclic voltammetry is demonstrated as a useful method to measure equilibrium binding between quantum dots and redox active small molecules. Specifically, the interaction of a library of ferrocene derivatives with CdSe interfaces is examined. For the strongly interacting systems, ferrocene carboxylic acid (FcCOOH) and ferrocene hexane thiol (Fc-hexSH), the binding equilibria can be quantitatively deduced from modeling the cyclic voltammetry data. This modeling allows extraction of the diffusion coefficients, equilibrium constants associated with both the reduced and oxidized species, and forward and reverse rates associated with binding for both the reduced and oxidized species. Taken together these data give direct insight into the binding of small molecules to quantum-dot surfaces as a function of oxidation state, critical information for the design of quantum dots as photoredox catalysts and charge transfer mediators.
关键词： quantum dots,surface chemistry,equilibrium binding,nanoparticles,cyclic voltammetry
更新于2025-09-19 17:13:59
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Sonication-Enhanced Alignment Relay Technique for the Orientation of Single-Walled Carbon Nanotubes
摘要： The high demand for thin, lightweight yet fast and e?cient devices is a driving force behind the miniaturization trend in the electronics industry. Speci?cally, the advancement of semiconducting single-walled carbon nanotubes (SWNTs) can continue to revolutionize transistors, although there are still many challenges ahead. We have previously reported an alignment relay technique (ART) that is capable of simultaneously controlling the alignment, length, and diameter of surface deposited SWNTs. However, the current technique yields inconsistencies in orientation, lengths of tubes, and their density. Here, we present a reviewed ART protocol that includes sonication for improved selectivity. We show that the SWNTs average alignment increased from 40% to 77% within a 10° range in orientation with sonication times as low as 5 min. Sonication generated larger diameter nanotubes on the surface, with a preference for semiconducting chiral tubes in the range of 1.44?1.61 nm in diameter. Consequently, simple alterations to the standard alignment relay technique can prove to be prosperous in improving selectivity and orientational control of single-walled carbon nanotubes. This work has direct impact for the simultaneous control of nanotube alignment and nanotube chiralities.
关键词： alignment relay technique,iptycenes,alignment,sonication,single-walled carbon nanotubes,surface chemistry,liquid crystals
更新于2025-09-16 10:30:52
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Exploration of Interfacial Porphine Coupling Schemes and Hybrid Systems by Bond-Resolved Scanning Probe Microscopy
摘要： The templated synthesis of porphyrin-based oligomers and heterosystems is of considerable interest for materials with tunable electronic gaps, photovoltaics, or sensing device elements. In this work, temperature-induced dehydrogenative coupling between unsubstituted free-base porphine units and their attachment to graphene nanoribbons on a well-defined Ag(111) support are scrutinized by bond-resolved scanning probe microscopy techniques. The detailed inspection of covalently fused porphine dimers obtained by in vacuo on-surface synthesis clearly reveals atomistic details of coupling motifs, whereby also putative reaction intermediates are identified. Moreover, the covalent attachment of porphines at preferred locations of atomically precise armchair-type graphene nanoribbons is demonstrated.
关键词： porphyrins,graphene nanoribbons,scanning probe microscopy,surface chemistry,C–C coupling
更新于2025-09-10 09:29:36
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Exploration of Interfacial Porphine Coupling Schemes and Hybrid Systems by Bond-Resolved Scanning Probe Microscopy
摘要： The templated synthesis of porphyrin-based oligomers and heterosystems is of considerable interest for materials with tunable electronic gaps, photovoltaics, or sensing device elements. In this work, temperature-induced dehydrogenative coupling between unsubstituted free-base porphine units and their attachment to graphene nanoribbons on a well-defined Ag(111) support are scrutinized by bond-resolved scanning probe microscopy techniques. The detailed inspection of covalently fused porphine dimers obtained by in vacuo on-surface synthesis clearly reveals atomistic details of coupling motifs, whereby also putative reaction intermediates are identified. Moreover, the covalent attachment of porphines at preferred locations of atomically precise armchair-type graphene nanoribbons is demonstrated.
关键词： porphyrins,graphene nanoribbons,scanning probe microscopy,surface chemistry,C–C coupling
更新于2025-09-10 09:29:36
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Effect of the reaction medium on the characteristics of silanized titanium dioxide particles: Differences obtained in the Zeta potential data and infrared spectra
摘要： In this document we present the differences in the Zeta potential and in the Infrared spectra data obtained from the characterization of silanized titanium dioxide particles, using two different solvents as reaction media: ethanol and toluene. Also, we provide micrographs of transmission electron microscopy in order to show morphological differences between the analyzed samples.
关键词： Zeta Potential Figure,Fourier Transformed Infrared Figure,Colloid and Surface Chemistry,Chemical Engineering,Transmission Electron Microscope images
更新于2025-09-10 09:29:36
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Photoactivatable Reaction for Covalent Nanoscale Patterning of Multiple Proteins
摘要： This article describes a photochemical approach for independently patterning multiple proteins to an inert substrate, particularly for studies of cell adhesion. A photoactivatable chloropyrimidine ligand was employed for covalent immobilization of SnapTag fusion proteins on self-assembled monolayers of alkanethiolates on gold. A two-step procedure was used: first, patterned UV illumination of the surface activated protein capture ligands, and second, incubation with a SnapTag fusion protein bound to the surface in illuminated regions. Two different fluorescent proteins were patterned in registry with features of 400 nm in size over a 1 mm2 area. An example is given wherein an anti-carcinoembryonic antigen (anti-CEA) scFv antibody was patterned to direct the selective attachment of a human cancer cell line that express the CEA antigen. This method enables the preparation of surfaces with control over the density and activity of independently patterned proteins.
关键词： immobilization,photochemistry,monolayers,surface chemistry,proteins
更新于2025-09-10 09:29:36
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Evolutions on surface chemistry, microstructure, morphology and electrical characteristics of SnO2/p-Si heterojuction under various annealing parameters
摘要： The influences of annealing temperature and ambient on surface chemistry, microstructure, morphology and electrical characteristics of Tin Oxide (SnO2)/Si heterojuctions are systematically identified. Metallic and oxygen deficient SnO2-x bonds have been consistently treated to stoichiometric SnO2 with annealing temperatures up to 600 0C in nitrogen environment. It has been observed that further increase in the annealing temperature causes the formation of the silicate layer. Presence of hydrogen in forming gas environment causes formation of the oxygen deficient SnO2-x, while the presence of the oxygen contributes to the formation of the stoichiometric SnO2 layer in oxygen annealing ambient. Parasitic phases significantly affect the crystalline structure of the films. Surface roughness of the samples decreases up to 1.02 nm which is strongly correlated with stress and strain on the film. On the other hand, oxidations of the dangling bonds and/or hydrogen diffusion cause variations in the total dipole moments which significantly change the capacitance. Depending on the annealing parameters, effective charge densities and interface trap densities decrease to 1011 cm-2, while the ideality factor and barrier potential are improved to 1.43 and 0.59 eV, respectively. Owing to the crystallization of the SnO2 layer, leakage current increase at low temperature annealing. However, passivation of the dangling bonds becomes more effective than phase crystallization at higher temperatures on the leakage characteristics. The current study shows that any changes in the surface chemistry directly affect the device performance.
关键词： Tin Oxide,XPS,Oxide Films.,Heterojuction,Surface Chemistry,Annealing
更新于2025-09-10 09:29:36
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Polarization-Direction Dependence of Thermodynamic Stability of Ferroelectric BiAlO <sub/>3</sub> (0001) Polar Surfaces
摘要： Polar surfaces of ferroelectric oxides are of great importance for both fundamental and practical interest. In this report, we present a theoretical study to determine the thermodynamic stability and electronic properties of ferroelectric BiAlO3(0001) surfaces. According to the calculated surface phase diagram, we predict that the equilibrium stoichiometries are distinct for the oppositely polarized BiAlO3 surfaces under the same chemical conditions. In addition to nonstoichiometry of the surface chemical compositions, we find that anomalous filling of the surface states can also result in surface metallization in order to compensate the remarkable surface polarity. Besides providing atomic-scale understanding of the BiAlO3(0001) surfaces, we also put forward the practical implications in novel magnetoelectric devices and advanced surface chemistry.
关键词： Magnetoelectric devices,Surface chemistry,Thermodynamic stability,Surface metallization,BiAlO3(0001) surfaces,Electronic properties,Ferroelectric oxides
更新于2025-09-09 09:28:46
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Surface Chemistry and Long-Term Stability of Amorphous Zn-Sn-O Thin Films
摘要： Amorphous (a-) oxides form an important category of transparent conducting/semiconducting thin films used as electrodes and channel layers in thin film transistors. The compositional flexibility of amorphous states, through doping, makes it possible to fine tune the electrical properties of films from conducting to semiconducting. However, surface chemistry and stability of these films are rarely addressed. Surface studies of amorphous materials, in general, are scarce due to disorder. Here, long-term surface stability of a-Zn-Sn-O films is investigated using grazing incidence X-ray absorption spectroscopy techniques. We present a detailed description of film surface structures and their evolution over time. It is found that the surface structure is, locally, a close analogue of the crystalline counterpart and that surface chemistry is governed by vacancies, strain, composition, and film density. It will be shown that the long-term stability of a film is questionable when the film has a high Zn content and a low density.
关键词： Zn-Sn-O thin films,Long-term stability,Grazing incidence X-ray absorption spectroscopy,Surface chemistry,Amorphous oxides
更新于2025-09-09 09:28:46