Kangha Lee

Absolute primary H atom quantum yield measurements in the 193.3 and 121.6 nm photodissociation of acetylene

Absolute quantum yields for primary H atom formation (UH) were measured under collision-free conditions for the room-temperature gas-phase dissociation of acetylene (C2H2) after photoexcitation at 193.3 nm and at the H-atom Lyman-a wavelength (121.6 nm) by a pulsed laser photolysis (LP)–laser-induced fluorescence (LIF) ‘pump-and-probe’ technique. Using HCl and CH4 photolysis at 193.3 and 121.6 nm, respectively, as a reference, values of UH ð193: 3n mÞ¼0:94� 0:12 and UH ð121: 6n mÞ¼1:04� 0:16 were obtained which demonstrate that for both photolysis wavelengths the Hþ C2H product channel dominates the primary C2H2 photochemistry. 2002 Published by Elsevier Science B.V.

Air-Stable PbSe Nanocrystals Passivated by Phosphonic Acids

We developed a new chemical strategy to enhance the stability of lead selenide nanocrystals (PbSe NCs) against oxidation through the surface passivation by P-O- moieties. In the synthesis of PbSe NCs, tris(diethylamino)phosphine (TDP) selenide (Se) was used as a Se precursor, and the resulting PbSe NCs withstood long-term air exposure while showing nearly no sign of oxidation. Nuclear magnetic resonance (NMR) spectroscopy reveals that TDP derivatives passivate the surface of PbSe NC. Through a series of ligand cleavage reactions, we found that the TDP derivatives are bound on NC surface through the P-O- moiety. Based on such understanding, it turned out that direct addition of various PAs during the synthesis of PbSe NCs also results in the NCs whose absorption spectrum remains nearly intact after air exposure for weeks. The P-O- moieties render the NCs stable in the operation of field effect transistors, suggesting that our findings can enable the use of air stable PbSe NCs in wider array of optoelectronic applications.

Expanding depletion region via doping: Zn-doped Cu2O buffer layer in Cu2O photocathodes for photoelectrochemical water splitting

We report photoelectrochemical hydrogen evolution reaction using a Cu2O-based photocathode with a layer doped with Zn ions. The doping results in the shift of the onset flat-band potential of the photocathode, likely a consequence of maximized band-bending in the Cu2O/Zn : Cu2O heterojunction. Systematic electrochemical analysis reveals that expansion of depletion region is responsible for the enhanced photoelectrochemical performance, e.g., the increase of photocurrent and reduced internal resistance.

Bi2O3 as a Promoter for Cu/TiO2 Photocatalysts for the Selective Conversion of Carbon Dioxide into Methane

A significantly enhanced gas‐phase photocatalytic conversion of carbon dioxide into methane on Cu/TiO2 nanoparticles upon introducing Bi2O3 as a promoter in the vicinity of Cu was observed. The maximum rate of CH4 generation of 11.90 μmol g−1 h−1 recorded in the case of Cu‐Bi2O3/TiO2 is approximately one order of magnitude higher than that obtained with Cu/TiO2 nanoparticles. The enhanced performance was attributed to facilitated migration of CO* from Cu to the Bi2O3 surface.

Highly luminescent silica-coated CdS/CdSe/CdS nanoparticles with strong chemical robustness and excellent thermal stability

We present facile synthesis of bright CdS/CdSe/CdS@SiO2 nanoparticles with 72% of quantum yields (QYs) retaining ca 80% of the original QYs. The main innovative point is the utilization of the highly luminescent CdS/CdSe/CdS seed/spherical quantum well/shell (SQW) as silica coating seeds. The significance of inorganic semiconductor shell passivation and structure design of quantum dots (QDs) for obtaining bright QD@SiO2 is demonstrated by applying silica encapsulation via reverse microemulsion method to three kinds of QDs with different structure: CdSe core and 2 nm CdS shell (CdSe/CdS-thin); CdSe core and 6 nm CdS shell (CdSe/CdS-thick); and CdS core, CdSe intermediate shell and 5 nm CdS outer shell (CdS/CdSe/CdS-SQW). Silica encapsulation inevitably results in lower photoluminescence quantum yield (PL QY) than pristine QDs due to formation of surface defects. However, the retaining ratio of pristine QY is different in the three silica coated samples; for example, CdSe/CdS-thin/SiO2 shows the lowest retaining ratio (36%) while the retaining ratio of pristine PL QY in CdSe/CdS-thick/SiO2 and SQW/SiO2 is over 80% and SQW/SiO2 shows the highest resulting PL QY. Thick outermost CdS shell isolates the excitons from the defects at surface, making PL QY relatively insensitive to silica encapsulation. The bright SiO2-coated SQW sample shows robustness against harsh conditions, such as acid etching and thermal annealing. The high luminescence and long-term stability highlights the potential of using the SQW/SiO2 nanoparticles in bio-labeling or display applications.

Origin of photoluminescence from colloidal gallium phosphide nanocrystals synthesized via a hot-injection method

In this work, photoluminescence from colloidal GaP nanocrystals (NCs) synthesized via a hot-injection method is observed and analyzed. The emission and excitation spectra of the GaP NCs indicate that two transitions, near the direct and indirect bandgaps of bulk GaP, are responsible for the luminescence.