The hydroxyl radical (OH) is one of the most interesting molecules in molecular dynamics. In particular, inelastic collisions of free radicals such as OH are profoundly important in environments ranging from combustion to astrochemistry. However, measuring the velocities of OH molecules in specific internal quantum states has proven to be very difficult. A method that can provide this important information is velocity-map imaging. Although this technique is very widely applicable in principle, it does require a sensitive and selective laser-ionization scheme. Here we show that, under the right conditions, velocity-map imaging can be applied to the study of the inelastic scattering of OH using crossed-molecular-beam methods. We measure fully quantum-state-specified product angular distributions for OH collisions with helium and argon. The agreement between exact close-coupling quantum scattering calculations on ab initio potential energy surfaces and experimental data is generally very satisfactory, except for scattering in the most forward directions.
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http://dx.doi.org/10.1038/nchem.1480 | DOI Listing |
J Phys Chem A
January 2025
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University, Shanghai 200438, China.
Understanding the interactions between transition metal atoms and molecules is important for the study of various related chemical and physical processes. In this study, we have investigated collisions between iron (Fe), iridium (Ir), and platinum (Pt) and the small molecules CH, O, and CO using a crossed-beam and time-sliced ion velocity map imaging technique. Elastic collisions were observed in all cases, except for collisions of Pt with O and CO.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, Faculty of Science, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan.
We present velocity-map imaging (VMI) of photoelectrons detached from anions using an optical parametric amplifier operating at a repetition rate as high as 100 kHz. The light source generates femtosecond (fs) laser pulses tunable from near-infrared to ultraviolet (310-2600 nm), which interact synchronously with mass-selected anion bunches. We demonstrate this technique by measuring two-dimensional projections of photoelectrons ejected from silver trimer anions, Ag3-, across a photon energy range from 2.
View Article and Find Full Text PDFRev Sci Instrum
January 2025
Université Paris-Saclay, CNRS, Institut des Sciences Moléculaires d'Orsay, 91405 Orsay, France.
We present the design of a VMI spectrometer optimized for attosecond spectroscopy in the 0-40 eV energy range. It is based on a compact three-electrode configuration where the lens shape, size, and material have been optimized using numerical simulations to improve the spectral resolution by a factor of ∼5 relative to the initial design [Eppink and Parker, Rev. Sci.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Department of Chemistry, University of Missouri, Columbia, MO 65211, USA.
We present state-to-state differential cross sections for rotationally inelastic collisions of vibrationally excited NO XΠ ( = 9) with Ar using a near-counterpropagating molecular beam geometry. These were obtained using the stimulated emission pumping technique coupled with velocity map imaging. Collision energies well over ∼1 eV were achieved and rotational excitations up to ∼Δ = 60 recorded for the first time for inelastic collisions.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Chemistry, KAIST, Daejeon 34141, Republic of Korea.
A photodetachment and photoelectron spectroscopic study by employing a cryogenically cooled ion trap combined with a velocity-map imaging setup has been carried out to unravel the vibrational structures and autodetachment dynamics of the dipole-bound states (DBSs) of -, -, and -methylphenolate anions (-, -, and -CHPhO). The electron binding energy of the DBS increases monotonically with the increase of the neutral dipole moment to give respective values of 66 ± 15, 123 ± 18, or 154 ± 14 cm for the -, -, or -isomer. The different electron-donating effects of the methyl moieties in the three geometrically different isomers seem to be reflected in the experiment.
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