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Atmospheric Pressure Laser Ionization Mass Spectrometry with Tunable UV Wavelength Utilizing an Optical Parametric Oscillator.
Anal Chem
December 2024
Joint Mass Spectrometry Centre/Chair of Analytical Chemistry, University of Rostock, 18059 Rostock, Germany.
To our knowledge, this study presents the first implementation of wavelength-resolved resonance-enhanced multiphoton ionization (REMPI) spectroscopy under atmospheric pressure ionization conditions using a high-resolution mass spectrometric system. Atmospheric pressure laser ionization MS spectroscopic measurements were conducted on over 70 different polycyclic aromatic hydrocarbons (PAHs) and hetero-PAHs (N, S, and O) in standard solutions, as well as three complex PAH-containing samples. The results demonstrate the successful transfer of REMPI spectroscopy from vacuum to atmospheric pressure conditions, maintaining spectral integrity without significant band broadening.
View Article and Find Full Text PDFSpectroscopy and Excited-State Dynamics of Methyl Ferulate in Molecular Beams.
J Phys Chem A
December 2024
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, Amsterdam 1098 XH, the Netherlands.
The spectroscopic and dynamic properties of methyl ferulate─a naturally occurring ultraviolet-protecting filter─and microsolvated methyl ferulate have been studied under molecular beam conditions using resonance-enhanced multiphoton ionization spectroscopy in combination with quantum chemical calculations. We demonstrate and rationalize how the phenyl substitution pattern affects the state ordering of the lower excited singlet state manifold and what the underlying reason is for the conformation-dependent Franck-Condon (FC) activity in the UV-excitation spectra. Studies on microsolvated methyl ferulate reveal potential coordination sites and the influence of such coordination on the spectroscopic properties.
View Article and Find Full Text PDFDeciphering Isotopic Fine Structures of Silylated Compounds in Gas Chromatography-Vacuum Photoionization Orbitrap Mass Spectrometry of Bio-Oils.
J Am Soc Mass Spectrom
December 2024
Joint Mass Spectrometry Centre (JMSC)/Chair of Analytical Chemistry, University of Rostock, 18059 Rostock, Germany.
We introduce vacuum resonance-enhanced multiphoton ionization (REMPI) with high-resolution Orbitrap Fourier transform mass spectrometry (FTMS) for analyzing silylated polar compounds. UV laser radiation at 248 nm sensitively and selectively targets aromatic constituents, while high-resolution mass spectrometry (HRMS) enables high-performance mass spectrometric detection. This workflow enhances the detection confidence of polar constituents by identifying unique isotopologue patterns, including at the isotopic fine structure (IFS) level, in analytical standards and complex bio-oils.
View Article and Find Full Text PDFPhotodesorption of CO ices: Rotational and translational energy distributions.
J Chem Phys
November 2024
CNRS, De la Molécule aux Nano-Objets: Réactivité, Interactions et Spectroscopies, MONARIS, Sorbonne Université, 75005 Paris, France.
This study investigates the translational and rovibrational energy of vacuum-ultraviolet (VUV) photodesorbed CO molecules from a CO polycrystalline ice (15 K) at ∼8 eV. The electronic excitation was produced by a pulsed VUV laser, and the photodesorption of CO molecules in their ground and first vibrational states was observed using resonance enhanced multiphoton ionization. Time-of-flight and rotationally resolved spectra were measured, and the kinetic and internal energy distribution were obtained.
View Article and Find Full Text PDFOvertone Excitation of Nitrogen Molecules via Stimulated Raman Pumping.
J Phys Chem Lett
November 2024
Department of Chemistry and Center for Advanced Light Source, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China.
Nitrogen bond activation is a pivotal process in chemistry, with bond excitation being fundamental to understanding the underlying mechanisms, making the preparation of molecules in specific quantum states crucial. Here we report the first overtone excitation of the N molecule from XΣ( = 0, = 0, 1, and 2) to XΣ( = 2, = 0, 1, 2, and 3) using the stimulated Raman pumping (SRP) method in a pulsed molecular beam. N was detected using 2+1 resonance-enhanced multiphoton ionization through the a″Σ state.
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