Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect.

Single atom (SA), noble metal catalysts are of interest due to high projected catalytic activity while minimizing cost. Common issues facing many synthesis methodologies include complicated processes, low yields of SA product, and production of mixtures of SA and nanoparticles (NPs). Herein we report a simple, room-temperature synthesis of single Pt-atom decorated, anatase Fe-doped TiO particles that leverages the Fe dopant as an engineered defect site to photodeposit and stabilize atomically dispersed Pt.

Phase-Sensitive Sum-Frequency Generation Measurements Using a Femtosecond Nonlinear Interferometer.

Phase-sensitive sum-frequency spectroscopy is a unique tool to interrogate the vibrational structure of interfaces. A precise understanding of the interfacial structure often relies on accurately determining the phase of χ, which has recently been demonstrated using a nonlinear interferometer in conjunction with a frequency-scanning picosecond laser system. Here, we implement nonlinear interferometry using a femtosecond laser system for broadband sum-frequency generation.

Gold as a standard phase reference in complex sum frequency generation measurements.

Complex, soft interfaces abound in the environment, biological systems, and technological applications. Probing these interfaces, particularly those buried between two condensed phases presents many challenges. The only current method capable of probing such interfaces with molecular specificity is the vibrational spectroscopy, sum frequency generation (SFG).

Nonlinear interferometer: Design, implementation, and phase-sensitive sum frequency measurement.

Sum frequency generation (SFG) spectroscopy is a unique tool for probing the vibrational structure of numerous interfaces. Since SFG is a nonlinear spectroscopy, it has long been recognized that measuring only the intensity-the absolute square of the surface response-limits the potential of SFG for examining interfacial interactions and dynamics. The potential is unlocked by measuring the phase-sensitive or imaginary response.

Single-crystal ice surfaces unveil connection between macroscopic and molecular structure.

Physics and chemistry of ice surfaces are not only of fundamental interest but also have important impacts on biological and environmental processes. As ice surfaces-particularly the two prism faces-come under greater scrutiny, it is increasingly important to connect the macroscopic faces with the molecular-level structure. The microscopic structure of the ubiquitous ice crystal is well-known.

Measuring Complex Sum Frequency Spectra with a Nonlinear Interferometer.

Currently, the only techniques capable of delivering molecular-level data on buried or soft interfaces are the nonlinear spectroscopic methods: sum frequency generation (SFG) and second harmonic generation (SHG). Deducing molecular information from spectra requires measuring the complex components-the amplitude and the phase-of the surface response. A new interferometer has been developed to determine these components with orders-of-magnitude improvement in uncertainty compared with current methods.

Producing desired ice faces.

The ability to prepare single-crystal faces has become central to developing and testing models for chemistry at interfaces, spectacularly demonstrated by heterogeneous catalysis and nanoscience. This ability has been hampered for hexagonal ice, Ih--a fundamental hydrogen-bonded surface--due to two characteristics of ice: ice does not readily cleave along a crystal lattice plane and properties of ice grown on a substrate can differ significantly from those of neat ice. This work describes laboratory-based methods both to determine the Ih crystal lattice orientation relative to a surface and to use that orientation to prepare any desired face.

A compact Raman converter for UV-VIS spectrometers.

A small form factor, easily constructed converter that adapts fiber coupled UV/VIS CCD detector-based spectrometers into a right angle scattering Raman spectrometer is described. Its design philosophy and design are discussed. An example measurement, the depolarization ratio of carbon tetrachloride, a classic Raman test compound, is presented.

Best face forward: crystal-face competition at the ice-water interface.

The ice-water interface plays an important role in determining the outcome of both biological and environmental processes. Under ambient pressure, the most stable form of ice is hexagonal ice (Ih). Experimentally probing the surface free energy between each of the major faces of Ih ice and the liquid is both experimentally and theoretically challenging.

Hydrogen bonding in the prism face of ice I(h) via sum frequency vibrational spectroscopy.

The prism face of single crystal ice I(h) has been studied using sum frequency vibrational spectroscopy focusing on identification of resonances in the hydrogen-bonded region. Several modes have been observed at about 3400 cm(-1); each mode is both polarization and orientation dependent. The polarization capabilities of sum frequency generation (SFG) are used in conjunction with the crystal orientation to characterize three vibrational modes.