A crossed molecular beam apparatus with multi-channel Rydberg tagging time-of-flight detection.

We report a new crossed molecular beam apparatus with the H atom Rydberg tagging detection technique. The multi-channel detection scheme with 15 microchannel plate (MCP) detectors enables simultaneously accumulating time-of-flight spectra over a wide range of scattering angles (112°). The efficiency of data acquisition has been enhanced by an order of magnitude. The angular distribution of H atoms from photodissociation of CH4 at 121.6 nm was used for calibrating the detection efficiency of different MCP detectors. The differential cross section of the reaction F + H2 → HF + H at the collision of 6.9 meV was measured, demonstrating the feasibility and accuracy of this multi-channel detection method. This apparatus could be a powerful tool for investigating the dynamics of reactions at very low collision energy.

Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths.

The difficulty in achieving high spectral resolution and accurate line shape in sum-frequency generation vibrational spectroscopy (SFG-VS) has restricted its use in applications requiring precise detection and quantitative analysis. Recently, the development of high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS) with sub-wavenumber resolution generated by synchronizing two independent amplifier lasers have opened new opportunities for probing an intrinsic SFG response. Here, we present a new flexible approach to achieve HR-BB-SFG-VS. In this system, two regeneration amplifiers shared the same oscillator laser as the seed, and a time-asymmetric visible pulse with a nearly Lorentzian line shape filtered by an etalon was used to overlap with a femtosecond broadband infrared pulse. This Lorentzian line shape of the visible pulse can greatly simplify the spectral fitting and analysis. We also demonstrated that the single-sided long visible pulse provided both high spectral resolution (1.4 cm-1) and effective suppression of the non-resonant background by detuning the time delay between visible and infrared pulses in SFG-VS measurements. With this new SFG setup, a pair of spectral splittings by 3.1 ± 0.7 and 3 ± 0.2 cm-1 for the symmetric and antisymmetric stretching of the CH3 group was resolved at the CH3CN/TiO2(110) surface, which are tentatively attributed to two different orientational methyl groups. These technological advancements can help broaden the applications of HR-BB-SFG-VS and provide solid ground for a better understanding of complex molecular structures and dynamics at interfaces.