Sum frequency

Recently, in situ studies of catalytic surface chemical reactions at high pressures have been undertaken [46, 47]. These studies employed sum frequency generation (SFG) and STM in order to probe the surfaces as the reactions are occurring under conditions similar to those employed for industrial catalysis (SFG is a laser-based teclmique that is described in section A 1.7.5.5 and section BT22). These studies have shown that the highly stable adsorbate sites that are probed under vacuum conditions are not necessarily tlie same sites that are active in high-pressure catalysis. Instead, less stable sites that are only occupied at high pressures are often responsible for catalysis. Because the active... 

Shen Y R 1998 Sum frequency generation for vibrational spectroscopy applications to water interfaces and films of water and ice Solid State Commun. 108 399... 

Gragson D E and Richmond G I 1998 Investigations of the structure and hydrogen bonding of water molecules at liquid surfaces by vibrational sum frequency spectroscopy J. Phys. Chem. 102 3847... 

These effects correspond, respectively, to the processes of sum-frequency generation (SFG), SFIG and optical rectification. 

Figure Bl.5.15 SFG spectrum for the water/air interface at 40 °C using the ssp polarization combination (s-, s- and p-polarized sum-frequency signal, visible input and infrared input beams, respectively). The peaks correspond to OH stretching modes. (After [ ].)...

Shen Y R 1989 Surface-properties probed by second-harmonic and sum-frequency generation Nature 337 519-25... 

Bain C D 1995 Sum-frequency vibrational spectroscopy of the solid-liquid interface J. Chem. See. Faraday Trans. 91 1281-96... 

Petukhov A V 1995 Sum-frequency generation on isotropic surfaces general phenomenology and microscopic theory for ]ellium surfaces Phys. Rev. B 52 16 901 -11... 

Zhu X D, Suhr H and Shen Y R 1987 Surface vibrational spectroscopy by infrared-visible sum frequency generation Phys. Rev. B 35 3047-59... 

Lin S H and Villaeys A A 1994 Theoretical description of steady-state sum-frequency generation in molecular absorbates Phys. Rev. A 50 5134-44... 

Richter L T, Petralli-Mallow T P and Stephenson J C 1998 Vibrationally resolved sum-frequency generation with broad-bandwidth infrared pulses Opt Lett. 23 1594-6... 

McGuire J A, Beck W, Wei X and Shen Y R 1999 Fourier-transform sum-frequency surface vibrational... 

The amplified signal is passed to a double-balanced mixer configured as a phase-sensitive detector where the two inputs are the NMR signal (cOq) and the frequency of the synthesizer (03. gf) with the output proportional to cos(coq - co gj.)t + 0) + cos((coq + + 9). The sum frequency is much larger than the total bandwidth of the... 

Figure Bl.22.8. Sum-frequency generation (SFG) spectra in the C N stretching region from the air/aqueous acetonitrile interfaces of two solutions with different concentrations. The solid curve is the IR transmission spectrum of neat bulk CH CN, provided here for reference. The polar acetonitrile molecules adopt a specific orientation in the air/water interface with a tilt angle that changes with changing concentration, from 40° from the surface nonnal in dilute solutions (molar fractions less than 0.07) to 70° at higher concentrations. This change is manifested here by the shift in the C N stretching frequency seen by SFG [ ]. SFG is one of the very few teclnhques capable of probing liquid/gas, liquid/liquid, and even liquid/solid interfaces.

The sum-frequency case of co = co -t CO2 is called up-conversion, tire difference-frequency co = co - CO2 down-conversion, reflecting tire increase or decrease of tire generated optical frequency co from tire input frequencies co and 052-... 

Unlike linear optical effects such as absorption, reflection, and scattering, second order non-linear optical effects are inherently specific for surfaces and interfaces. These effects, namely second harmonic generation (SHG) and sum frequency generation (SFG), are dipole-forbidden in the bulk of centrosymmetric media. In the investigation of isotropic phases such as liquids, gases, and amorphous solids, in particular, signals arise exclusively from the surface or interface region, where the symmetry is disrupted. Non-linear optics are applicable in-situ without the need for a vacuum, and the time response is rapid. 

SFG [4.309, 4.310] uses visible and infrared lasers for generation of their sum frequency. Tuning the infrared laser in a certain spectral range enables monitoring of molecular vibrations of adsorbed molecules with surface selectivity. SFG includes the capabilities of SHG and can, in addition, be used to identify molecules and their structure on the surface by analyzing the vibration modes. It has been used to observe surfactants at liquid surfaces and interfaces and the ordering of interfacial... 

Keywords lasers, laser guide star, adaptice optics, sum-frequency lasers, fiber lasers, Ra-... 

Sum-frequency mixing of two solid-state YAG lasers in a nonlinear crystal (see Ch. 20) to generate 589 nm in CW, CW mode-locked and macromicro pulse formats. The Nd YAG lasers can be pumped by flashlamps, but higher efficiency is obtained using diode lasers. 

Sum-frequency mixing of two diode pumped fiber lasers (938 and 1583 nm) in a nonlinear crystal. CW format has been demonstrated at low power levels higher powers and pulsed formats are under development. 

Figure 16. Sum-frequency mixing two Nd YAG lasers at 1064 and 1319 nm in a nonlinear crystal produces 589 nm light.

Figure 17. Schematic diagram of the AFRL CW sum-frequency laser.

Gemini North Observatory/CTI Mode-locked SFG Laser. CTT is developing the first commercial solid-state Na LGS system. It will be installed on the center section of the 8-m Gemini North telescope, with the output beam relayed to a projector behind the secondary mirror. The projected beam is required to be 10-20 W power, with M2 < 1.5. The architecture is based on sum-frequency mixing two mode-locked solid-state Nd YAG lasers. The mode-locked format provides significantly higher peak intensity than CW, enabling more efficient SFG conversion. The laser is also free of the thermal and intensity transients that are inherent in the macro pulse format. The chosen... 

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