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Gao-Lei Hou

Publications and source records attributed to Gao-Lei Hou.

5 recordsLinked to original sources

Infrared Spectroscopy of Cyanonaphthalenes under Interstellar Relevant Conditions and Their Potential Connection with Astronomical Aromatic Infrared Bands

Context. Aromatic infrared bands (AIBs) are widely observed in diverse astrophysical environments and are generally attributed to vibrational emission from polycyclic aromatic hydrocarbons (PAHs). The recent interstellar detection of 1-cyanonaphthalene (1-CNN) and 2-cyanonaphthalene (2-CNN) has motivated detailed infrared spectroscopic studies of cyano-substituted PAHs. Aims. We aim to characterize the infrared spectra and vibrational modes of neutral 1-CNN and 2-CNN under cold and gas-phase conditions and to assess their possible spectroscopic relevance to the astronomical AIBs. Methods. The gas-phase infrared spectra of neutral 1-CNN and 2-CNN were measured in a cold molecular beam using ion-dip spectroscopy. The observed bands were assigned with the aid of harmonic and anharmonic calculations at the B3LYP/N07D level. Infrared emission spectra were subsequently simulated from the experimental spectra within a single-photon approximation framework. Results. We report the infrared spectra of neutral 1-CNN and 2-CNN measured under cold and gas-phase conditions relevant to the interstellar medium. Their vibrational features were assigned in detail, including fundamental vibrations as well as overtone and combination bands. The simulated emission spectra exhibit features in several wavelength regions associated with prominent AIBs, including the aromatic CH stretching region near 3.3 micron, the CC stretching region near 6.2 micron, the mixed CH in-plane bending and CC stretching region at 8.6-8.9 microns, and the CH out-of-plane bending region between 10 and 15 microns. Conclusions. The present spectra provide laboratory reference data for small cyano-substituted PAHs and offer useful clues for interpreting selected AIB regions. These results suggest that cyanonaphthalene molecules are promising contributors to the aromatic infrared bands.

astro-ph.GA↗

Pentagon, Hexagon, or Bridge? Identifying the Location of a Single Vanadium Cation on Buckminsterfullerene Surface

Buckminsterfullerene C60 has received extensive research interest ever since its discovery. In addition to its interesting intrinsic properties of exceptional stability and electron-accepting ability, the broad chemical tunability by decoration or substitution on the C60-fullerene surface makes it a fascinating molecule. However, to date there is uncertainty about the binding location of such decorations on the C60 surface, even for a single adsorbed metal atom. In this work, we report the gas-phase synthesis of the C60V+ complex and its in-situ characterization by mass spectrometry and in-frared spectroscopy with the help of quantum chemical calculations and molecular dynamics simulations. We identify the most probable binding position of a vanadium cation on C60 above a pentagon center in eta5-fashion, demonstrate a high thermal stability for this complex, and explore the bonding nature between C60 and the vanadium cation, reveal-ing that large orbital and electrostatic interactions lie at the origin of the stability of the eta5-C60V+ complex.

physics.chem-ph↗

Towards a reliable prediction of the infrared spectra of cosmic fullerenes and their derivatives in the JWST era

Fullerenes, including C60, C70, and C60+, are widespread in space through their characteristic infrared vibrational features (C60+ also reveals its presence in the interstellar medium through its electronic transitions) and offer great insights into the carbon chemistry and stellar evolution. The potential existence of fullerene-related species in space has long been speculated and recently put forward by a set of laboratory experiments of C60+, C60H+, C60O+, C60OH+, C70H+, and [C60-Metal]+ complexes. The advent of the James Webb Space Telescope (JWST) provides a unique opportunity to search for these fullerene-related species in space. To facilitate JWST search, analysis, and interpretation, an accurate knowledge of their vibrational properties is essential. Here, we compile a VibFullerene database and conduct a systematic theoretical study on those species. We derive a set of range-specific scaling factors for vibrational frequencies, to account for the deficiency of density functional theory calculations in predicting the accurate frequencies. Scaling factors with low root-mean-square and median errors for the frequencies are obtained, and their performance is evaluated, from which the best-performing methods are recommended for calculating the infrared spectra of fullerene derivatives which balance the accuracy and computational cost. Finally, the recommended vibrational frequencies and intensities of fullerene derivatives are presented for future JWST detection.

astro-ph.GA↗

Photochemical origin of SiC$_2$ in the circumstellar envelope of carbon-rich AGB stars revealed by ALMA

Whether SiC$_2$ is a parent species, that is formed in the photosphere or as a by-product of high-temperature dust formation, or a daughter species, formed in a chemistry driven by the photodestruction of parent species in the outer envelope, has been debated for a long time. Here, we analyze the ALMA observations of four SiC$_2$ transitions in the CSEs of three C-rich AGB stars (AI Vol, II Lup, and RAFGL 4211), and found that SiC$_2$ exhibits an annular, shell-like distribution in these targets, suggesting that SiC$_2$ can be a daughter species in the CSEs of carbon-rich AGB stars. The results can provide important references for future chemical models.

astro-ph.SR↗

Buckyball-metal complexes as promising carriers of astronomical unidentified infrared emission bands

Infrared emission bands with wavelengths between 3-20 μm are observed in a variety of astrophysical environments [1,2]. They were discovered in the 1970s and are generally attributed to organic compounds [3,4]. However, over 40 years of research efforts still leave the source of these emission bands largely unidentified [5-7]. Here, we report the first laboratory infrared (6-25 μm) spectra of gas-phase fullerene-metal complexes, [C60-Metal]+ (Metal = Fe and V), and show with density functional theory calculations that complexes of C60 with cosmically abundant metals, including Li, Na, K, Mg, Ca, Al, V, and Fe, all have similar infrared spectral patterns. Comparison with observational infrared spectra from several fullerene-rich planetary nebulae demonstrates a strong positive linear cross-correlation. The infrared features of [C60-Metal]+ coincide with four bands attributed earlier to neutral C60 bands, and in addition also with several to date unexplained bands. Abundance and collision theory estimates furthermore indicate that [C60-Metal]+ could plausibly form and survive in astrophysical environments. Hence, [C60-Metal]+ are proposed as promising carriers, in supplement to C60, of astronomical infrared emission bands, potentially representing the largest molecular species in space other than the bare fullerenes C60, C60+, and C70. This work opens a new chapter for studying cosmic fullerene species and carbon chemistry in the Universe.

astro-ph.GA↗