arXiv subjects

Alexandre Faure

Publications and source records attributed to Alexandre Faure.

At least 19 recordsLinked to original sources

arXiv2026

Chemistry and ro-vibrational excitation of CH$^+$ in the planetary nebula NGC 7027

Small carbon hydride cations, such as the methylidyne ion (CH$^+$), play an important role in the chemistry of the interstellar medium (ISM). They participate in gas-phase reaction networks leading to the formation of hydrocarbon species that act as precursors to more complex organic molecules. CH$^+$ is a highly reactive ion that is rapidly destroyed by H, H$_2$, and free electrons, making its excitation challenging to model. Its level populations depend not only on radiative and inelastic processes but also on chemical formation and destruction rates, a mechanism known as chemical pumping. We investigate this effect using a new set of ab initio state-resolved ro-vibrational (reactive and inelastic) collision data to model the observed CH$^+$ emission. Multiple rotational and ro-vibrational transitions of CH$^+$ detected toward the planetary nebula NGC 7027 are analyzed. The chemical structure of CH$^+$ is modeled with the CLOUDY code using updated reaction rates, providing the temperature and density structure across the nebula. A non-local thermodynamic equilibrium (NLTE) analysis is performed using CLOUDY and the single-zone RADEX code with a comprehensive set of spectroscopic and collisional data. In addition, chemical formation and destruction processes are implemented in RADEX and explored via Markov Chain Monte Carlo sampling. The CLOUDY model reproduces the observed CH$^+$ line fluxes within a factor of 1.3 on average. It indicates that rotational and ro-vibrational lines arise from physically distinct regions, primarily differing in temperature. RADEX models show that chemical pumping significantly enhances populations above ($\upsilon = 0, J = 1$), strongly increasing ro-vibrational emission, especially in the $\upsilon =2 \to 1$ band. Single-zone models remain limited, highlighting the need for full 1D modeling including all excitation processes.

astro-ph.GA↗

arXiv2025

VIRAL: Vision-grounded Integration for Reward design And Learning

The alignment between humans and machines is a critical challenge in artificial intelligence today. Reinforcement learning, which aims to maximize a reward function, is particularly vulnerable to the risks associated with poorly designed reward functions. Recent advancements has shown that Large Language Models (LLMs) for reward generation can outperform human performance in this context. We introduce VIRAL, a pipeline for generating and refining reward functions through the use of multi-modal LLMs. VIRAL autonomously creates and interactively improves reward functions based on a given environment and a goal prompt or annotated image. The refinement process can incorporate human feedback or be guided by a description generated by a video LLM, which explains the agent's policy in video form. We evaluated VIRAL in five Gymnasium environments, demonstrating that it accelerates the learning of new behaviors while ensuring improved alignment with user intent. The source-code and demo video are available at: https://github.com/VIRAL-UCBL1/VIRAL and https://youtu.be/Hqo82CxVT38.

cs.AI↗

arXiv2025

Experimental observation of quantum interferences in CO-H$_2$ rotational energy transfer at room temperature

Using time-resolved infrared-vacuum-ultraviolet double-resonance spectroscopy, experimental room temperature measurements of state-to-state rate coefficients for rotational energy transfer within the X $^1\Sigma^+(v=2)$ vibrational state of CO due to H$_2$ collisions have been compared to accurate 4-D close-coupling quantum calculations. Theoretically predicted quantum interferences in the CO-H$_2$ collisional system are experimentally observed at room temperature, and excellent agreement between theory and experiment is observed. These results provide a valuable benchmark for validating the anisotropic part of the potential energy surface, thereby supporting the theoretical modeling of CO emission in warm astrophysical environments such as photodissociation regions.

quant-ph↗

arXiv2025

Chemistry and ro-vibrational excitation of HeH$^+$ in the Planetary Nebula NGC 7027

HeH$^+$ belongs to the class of "reactive" ions that can be destroyed so quickly that chemical formation and destruction rates may compete with inelastic rates and should be considered when solving the statistical equilibrium equations. This so-called chemical "pumping" or "excitation" effect is investigated here for the first time in HeH$^+$. The chemical evolution of HeH$^+$ in NGC 7027 is modeled with the CLOUDY photoionization code using updated reaction rate coefficients. The non-LTE analysis of the three observed HeH$^+$ emission lines is then performed with the CLOUDY and RADEX codes using an extensive set of spectroscopic and inelastic collisional data suitable for the specific high-temperature environment of NGC 7027. In a second approach, chemical formation and destruction rates of HeH$^+$ are implemented in RADEX. This code is combined with MCMC sampling (performed on the RADEX-parameters space) to extract the best-fit HeH$^+$ column density and physical conditions from the observed line fluxes. The CLOUDY and RADEX non-LTE results are found to be in good agreement, and the $\upsilon=1-0 \ P(2)/P(1)$ line ratio is better than 20%. Agreement to better than a factor of 2.3 is obtained when including the reaction between He($2^3S$) and H as an additional source of HeH$^+$. The RADEX/MCMC model with chemical pumping is found to reproduce both the observed line fluxes and the line ratio to 20%. Our results suggest that additional HeH$^+$ lines must be detected in NGC 7027 to better constrain the physical conditions via non-LTE models. Uncertainties in collisional (reactive and inelastic) data of HeH$^+$ have been largely reduced in this work. The three observed lines are not sensitive to chemical pumping while excited "short-lived" levels are significantly overpopulated with respect to a non-LTE model neglecting chemical excitation.

astro-ph.GA↗

arXiv2025

PDRs4All XI. Detection of infrared CH$^+$ and CH$_3^+$ rovibrational emission in the Orion Bar and disk d203-506: evidence of chemical pumping

The methylidyne cation (CH$^+$) and the methyl cation (CH$_3^+$) are building blocks of organic molecules, yet their coupled formation and excitation mechanisms remain mainly unprobed. The James Webb Space Telescope (JWST), with its high spatial resolution and good spectral resolution, provides unique access to the detection of these molecules. Our goal is to use the first detection of CH$^+$ and CH$_3^+$ rovibrational emission in the Orion Bar and in the protoplanetary disk d203-506, irradiated by the Trapezium cluster, to probe their formation and excitation mechanisms and constrain the physico-chemical conditions. We use spectro-imaging acquired using both the NIRSpec and MIRI-MRS instruments to study the CH$^+$ and CH$_3^+$ spatial distribution at very small scales, and compare it to excited H$_2$ emission. CH$^+$ and CH$_3^+$ emissions originate from the same region as highly excited H$_2$. Our comparison between the Bar and d203-506 reveals that both CH$^+$ and CH$_3^+$ excitation and/or formation are highly dependent on gas density. The excitation temperature of the observed CH$^+$ and CH$_3^+$ rovibrational lines is around $T$ ~ 1500 K in the Bar and $T$ ~ 800 K in d203-506. Moreover, the column densities derived from the rovibrational emission are less than 0.1 % of the total known (CH$^+$) and expected (CH$_3^+$) column densities. These results show that CH$^+$ and CH$_3^+$ level populations strongly deviate from ETL. CH$^+$ rovibrational emission can be explained by chemical formation pumping with excited H$_2$ via C$^+$ + H$_2^*$ = CH$^+$ + H. These results support a gas phase formation pathway of CH$^+$ and CH$_3^+$ via successive hydrogen abstraction reactions. However, we do not find any evidence of CH$_2^+$ emission in the JWST spectrum. Finally, observed CH$^+$ intensities coupled with chemical formation pumping model provide a diagnostic tool to trace the local density.

astro-ph.GA↗

arXiv2024

Rotational excitation cross sections for chloronium based on a new 5D interaction potential with molecular hydrogen

Chloronium (H$_2$Cl$^+$) is an important intermediate of Cl-chemistry in space. The accurate knowledge of its collisional properties allows a better interpretation of the corresponding observations in interstellar clouds and therefore a better estimation of its abundance in these environments. While the ro-vibrational spectroscopy of H$_2$Cl$^+$ is well known, the studies of its collisional excitation are rather limited and these are available for the interaction with helium atoms only. We provide a new 5-dimensional rigid-rotor potential energy surface for the interaction of H$_2$Cl$^+$ with H$_2$, calculated from explicitly correlated coupled cluster ab initio theory, which was fitted then with a set of analytical functions, allowing to perform scattering calculations using accurate quantum theories. We analyze the collision-energy-dependence of the rotational state-to-state cross sections and the temperature dependence of the corresponding thermal rate coefficients, with a particular attention on the collisional propensity rules. When comparing our results for collisions with H$_2$ with those obtained with He as a colliding partner, we found very significant differences with non-linear scaling trends, which proves again that He is not a suitable proxy for collisions between hydride molecules and molecular hydrogen, the most abundant gas particle in the interstellar medium.

physics.chem-ph↗

arXiv2024

Revisiting rotationally excited CH at radio wavelengths: A case study towards W51

Ever since they were first detected in the interstellar medium, the radio wavelength (3.3 GHz) hyperfine-structure splitting transitions in the rotational ground state of CH have been observed to show anomalous excitation. Astonishingly, this behaviour has been uniformly observed towards a variety of different sources probing a wide range of physical conditions. While the observed level inversion can be explained globally by a pumping scheme involving collisions, a description of the extent of 'over-excitation' observed in individual sources requires the inclusion of radiative processes, involving transitions at higher rotational levels. Therefore, a complete description of the excitation mechanism in the CH ground state, observed towards individual sources entails observational constraints from the rotationally excited levels of CH and in particular that of its first rotationally excited state. Given the limited detections of these lines, the objective of this work is to characterise the physical and excitation properties of the rotationally excited lines of CH near 700 MHz, and investigate their influence on the pumping mechanisms of the ground-state lines of CH. This work presents the first interferometric search for the rotationally excited lines of CH near 700 MHz carried out using the uGMRT array and jointly models the physical and excitation conditions traced by lines from both the ground and first rotationally excited states of CH.

astro-ph.GA↗

arXiv2024

Fate and detectability of rare gas hydride ions in nova ejecta: A case study with nova templates

HeH$^+$ was the first heteronuclear molecule to form in the metal-free Universe after the Big Bang. The molecule gained significant attention following its first circumstellar detection in the young and dense planetary nebula NGC 7027. We target some hydride ions associated with the noble gases (HeH$^+$, ArH$^+$, and NeH$^+$) to investigate their formation in harsh environments like the nova outburst region. We use a photoionization modeling (based on previously published best-fit physical parameters) of the moderately fast ONe type nova, QU Vulpeculae 1984, and the CO type novae, RS Ophiuchi and V1716 Scorpii. Our steady-state modeling reveals a convincing amount of HeH$^+$, especially in the dense clump of RS Ophiuchi and V1716 Scorpii. The calculated upper limit on the surface brightness of HeH$^+$ transitions suggests that the James Webb Space Telescope (JWST) could detect some of them, particularly in sources like RS Ophiuchi and V1716 Scorpii, which have similar physical and chemical conditions and evolution. It must be clearly noted that the sources studied are used as templates, and not as targets for observations. The detection of these lines could be useful for determining the physical conditions in similar types of systems and for validating our predictions based on new electron-impact ro-vibrational collisional data at temperatures of up to 20,000 K.

astro-ph.GA↗

arXiv2024

Maser Activity of Organic Molecules toward Sgr B2(N)

At centimeter wavelengths, single-dish observations have suggested that the Sagittarius (Sgr) B2 molecular cloud at the Galactic Center hosts weak maser emission from several organic molecules, including CH$_2$NH, HNCNH, and HCOOCH$_3$. However, the lack of spatial distribution information of these new maser species has prevented us from assessing the excitation conditions of the maser emission as well as their pumping mechanisms. Here, we present a mapping study toward Sgr B2 North (N) to locate the region where the complex maser emission originates. We report the first detection of the Class I methanol (CH$_3$OH) maser at 84 GHz and the first interferometric map of the methanimine (CH$_2$NH) maser at 5.29 GHz toward this region. In addition, we present a tool for modeling and fitting the unsaturated molecular maser signals with non-LTE radiative transfer models and Bayesian analysis using the Markov-Chain Monte Carlo approach. These enable us to quantitatively assess the observed spectral profiles. The results suggest a two-chain-clump model for explaining the intense CH$_3$OH Class I maser emission toward a region with low continuum background radiation. By comparing the spatial origin and extent of maser emission from several molecular species, we find that the 5.29 GHz CH$_2$NH maser has a close spatial relationship with the 84 GHz CH$_3$OH Class I masers. This relationship serves as observational evidence to suggest a similar collisional pumping mechanism for these maser transitions.

astro-ph.GA↗

arXiv2024

H2CO and CS in diffuse clouds: Excitation and abundance

To provide constraints on the chemical processes responsible for the observed columns of organic species, we used NOEMA to observe the sight line toward NRAO150 in the 2mm spectral window. We targeted the low excitation lines of o-H2CO 2(1,1)-1(1,0) and p-H2CO 2(0,2)-1(0,1) as well as the nearby transitions of CS(3-2) and c-C3H2. We combined these data with previous observations to determine the excitation conditions, column densities, and abundances relative to H2 in the different velocity components. We performed non-LTE radiative transfer calculations including collision cross sections with ortho and para H2 and with electrons. New collision cross sections with electrons were computed for ortho and para formaldehyde. The c-C3H2 line profiles are very similar to those of HCO+ and CCH, while the CS absorption features are narrower and mostly concentrated in two main velocity components at V = -17 and -10 km/s. H2CO absorption lines present an intermediate pattern with absorption in all velocity components but larger opacities in the two main velocity components. The ortho-to-para ratios of H2CO and c-C3H2 are consistent with the statistical value of 3. While the excitation temperature of all c-C3H2 velocity components is consistent with the CMB, the two strong components detected in CS show a clear excess over the CMB indicating that CS resides at higher densities than other species along this particular sightline, n(H2) ~ 2500 cm-3 while n(H2) < 500 cm-3 for the other velocity components. We detected faint absorption from o-H213CO and C34S allowing us to derive isotopic ratios: o-H2CO/o-H213CO = 61 and C32S/C34S = 24. The excitation of the 4.8GHz line of formaldehyde is sensitive to the electron fraction and its excitation temperature is predicted to be lower than the CMB at low and moderate electron fractions, x(e)< 6E-5, and to rise above the CMB at high electron fractions, > 1e-4.

astro-ph.GA↗

arXiv2023

Identification of Ammonium Salts on Comet 67P/C-G Surface from Infrared VIRTIS/Rosetta Data Based on Laboratory Experiments. Implications and Perspectives

The nucleus of comet 67P/Churyumov-Gerasimenko exhibits a broad spectral reflectance feature around 3.2 $\mu$m, which is omnipresent in all spectra of the surface, and whose attribution has remained elusive since its discovery. Based on laboratory experiments, we have shown that most of this absorption feature is due to ammonium (NH4+) salts mixed with the dark surface material. The depth of the band is compatible with semi-volatile ammonium salts being a major reservoir of nitrogen in the comet, which could dominate over refractory organic matter and volatile species. These salts may thus represent the long-sought reservoir of nitrogen in comets, possibly bringing their nitrogen-to-carbon ratio in agreement with the solar value. Moreover, the reflectance spectra of several asteroids are compatible with the presence of NH4+ salts at their surfaces. The presence of such salts, and other NH4+-bearing compounds on asteroids, comets, and possibly in proto-stellar environments, suggests that NH4+ may be a tracer of the incorporation and transformation of nitrogen in ices, minerals and organics, at different phases of the formation of the Solar System.

astro-ph.EP↗

arXiv2023

Bending relaxation of H$_2$O by collision with para- and ortho-H$_2$

We extend our recent theoretical work on the bending relaxation of H$_2$O in collisions with H$_2$ by including the three water modes of vibration coupled with rotation, as well as the rotation of H$_2$. Our full quantum close-coupling method (excluding the H$_2$ vibration) is combined with a high-accuracy nine-dimensional potential energy surface. The collisions of para-H$_2$O and ortho-H$_2$O with the two spin modifications of H$_2$ are considered and compared for several initial states of H$_2$O. The convergence of the results as a function of the size of the rotational basis set of the two colliders is discussed. In particular, near-resonant energy transfer between H$_2$O and H$_2$ is found to control the vibrational relaxation process, with a dominant contribution of transitions with delta j2 = +2, +4. Finally, the calculated value of the H$_2$O bending relaxation rate coefficient at 295 K is found to be in excellent agreement with its experimental estimate.

physics.chem-ph↗

arXiv2022

An accurate set of H$_3$O$^+ -$ H$_2$ collisional rate coefficients for non-LTE modelling of warm interstellar clouds

Hydronium (H$_3$O$^+$) was first detected in 1986 in interstellar molecular clouds. It was reported in many galactic diffuse and dense regions, as well as in extragalactic sources. H$_3$O$^+$ plays a major role both in interstellar oxygen and water chemistry. However, despite the large number of H$_3$O$^+$ observations, its collisional excitation was investigated only partially. In the present work we study the state-to-state rotational de-excitation of $ortho$- and $para$-H$_3$O$^+$ in collisions both with $ortho$- and $para$-H$_2$. The cross sections are calculated within the close-coupling formalism using a highly accurate potential energy surface developed for this system. The rate coefficients are computed up to $300$ K kinetic temperature. Transitions between the lowest 21 rotation-inversion states were studied for $para$-H$_3$O$^+$, and the lowest 11 states for $ortho$-H$_3$O$^+$, i.e. all levels with rotational energies below 430 K ($\sim 300$ cm$^{-1}$) are considered (up to $j\leq5$). In order to estimate the impact of the new rate coefficients on the astrophysical models for H$_3$O$^+$, radiative transfer calculations were also carried out. We have examined how the new collisional data affect the line intensities with respect to older data previously used for the interpretation of observations. By analysing all detected transitions we find that our new, accurate rate coefficients have a significant impact (typically within a factor of 2) on radiation temperatures, allowing more accurate estimation of column densities and relative abundances of hydronium, especially in warm molecular clouds, paving the path towards better interpretation of interstellar water and oxygen chemistry.

astro-ph.GA↗

arXiv2021

Rotational excitation of H$_3$O$^+$ cations by para-H$_2$: improved collisional data at low temperatures

The hydronium cation plays a crucial role in interstellar oxygen and water chemistry. While its spectroscopy was extensively investigated earlier, the collisional excitation of H$_3$O$^+$ is not well studied yet. In this work we present state-to-state collisional data for rotational de-excitation of both ortho- and para-H$_3$O$^+$ due to para-H$_2$ impact. The cross sections are calculated within the close-coupling formalism using our recent, highly accurate rigid-rotor potential energy surface for this collision system. The corresponding thermal rate coefficients are calculated up to 100 K. For para-H$_3$O$^+$ the lowest 20 rotation-inversion states were considered in the calculations, while for ortho-H$_3$O$^+$ the lowest 11 states are involved (up to $j\leq5$), so all levels with rotational energy below 420 K (292 cm$^{-1}$) are studied. In order to analyse the impact of the new collisional rates on the excitation of H$_3$O$^+$ in astrophysical environments radiative transfer calculations are also provided. The most relevant emission lines from an astrophysical point of view are studied, taking into account the transitions at 307, 365, 389 and 396 GHz. We show that our new collisional data have a non-negligible impact (from a few percents up to about a factor of 3) on the brightness and excitation temperatures of H$_3$O$^+$, justifying the revision of the physical conditions in the appropriate astrophysical observations. The calculated rate coefficients allow one to recalculate the column density of hydronium in interstellar clouds, which can lead to a better understanding of interstellar water and oxygen chemistry.

physics.chem-ph↗

arXiv2021

Observations and analysis of CH$^+$ vibrational emissions from the young, carbon-rich planetary nebula NGC 7027: a textbook example of chemical pumping

We discuss the detection of 14 rovibrational lines of CH$^+$, obtained with the iSHELL spectrograph on NASA's Infrared Telescope Facility (IRTF) on Maunakea. Our observations in the 3.49 - 4.13 $\mu$m spectral region, obtained with a 0.375" slit width that provided a spectral resolving power $\lambda/\Delta \lambda \sim 80,000$, have resulted in the unequivocal detection of the $R(0) - R(3)$ and $P(1)-P(10)$ transitions within the $v=1-0$ band of CH$^+$. The $R$-branch transitions are anomalously weak relative to the $P$-branch transitions, a behavior that is explained accurately by rovibronic calculations of the transition dipole moment reported in a companion paper (Changala et al. 2021). Nine infrared transitions of H$_2$ were also detected in these observations, comprising the $S(8)$, $S(9)$, $S(13)$ and $S(15)$ pure rotational lines; the $v=1-0$ $O(4) - O(7)$ lines, and the $v=2-1$ $O(5)$ line. We present a photodissociation region model, constrained by the CH$^+$ and H$_2$ line fluxes that we measured, that includes a detailed treatment of the excitation of CH$^+$ by inelastic collisions, optical pumping, and chemical ("formation") pumping. The latter process is found to dominate the excitation of the observed rovibrational lines of CH$^+$, and the model is remarkably successful in explaining both the absolute and relative strengths of the CH$^+$ and H$_2$ lines.

astro-ph.GA↗

arXiv2019

Deuterated methanol toward NGC 7538-IRS1

We investigate the deuteration of methanol towards the high-mass star forming region NGC 7538-IRS1. We have carried out a multi-transition study of CH$_3$OH, $^{13}$CH$_3$OH and of the deuterated fllavors, CH$_2$DOH and CH$_3$OD, between 1.0--1.4 mm with the IRAM-30~m antenna. In total, 34 $^{13}$CH$_3$OH, 13 CH$_2$DOH lines and 20 CH$_3$OD lines spanning a wide range of upper-state energies (E$_{up}$) were detected. From the detected transitions, we estimate that the measured D/H does not exceed 1$\%$, with a measured CH$_2$DOH/CH$_3$OH and CH$_3$OD/CH$_3$OH of about (32$\pm$8)$\times$10$^{-4}$ and (10$\pm$4)$\times$10$^{-4}$, respectively. This finding is consistent with the hypothesis of a short-time scale formation during the pre-stellar phase. We find a relative abundance ratio CH$_2$DOH/CH$_3$OD of 3.2 $\pm$ 1.5. This result is consistent with a statistical deuteration. We cannot exclude H/D exchanges between water and methanol if water deuteration is of the order 0.1$\%$, as suggested by recent Herschel observations.

astro-ph.GA↗

arXiv2019

Efficient methanol production on the dark side of a prestellar core

We present ALMA maps of the starless molecular cloud core Ophiuchus/H-MM1 in the lines of deuterated ammonia (ortho-NH2D), methanol (CH3OH), and sulphur monoxide (SO). The dense core is seen in NH2D emission, whereas the CH3OH and SO distributions form a halo surrounding the core. Because methanol is formed on grain surfaces, its emission highlights regions where desorption from grains is particularly efficient. Methanol and sulphur monoxide are most abundant in a narrow zone that follows the eastern side of the core. This side is sheltered from the stronger external radiation field coming from the west. We show that photodissociation on the illuminated side can give rise to an asymmetric methanol distribution, but that the stark contrast observed in H-MM1 is hard to explain without assuming enhanced desorption on the shaded side. The region of the brightest emission has a wavy structure that rolls up at one end. This is the signature of Kelvin-Helmholtz instability occurring in sheared flows. We suggest that in this zone, methanol and sulphur are released as a result of grain-grain collisions induced by shear vorticity.

astro-ph.GA↗

arXiv2018

Collisional Excitation and Weak Maser Action of Interstellar Methanimine

The inelastic cross sections and rate coefficients for the rotational excitation of methanimine (CH$_2$NH) by cold H$_2$ have been determined quantum mechanically based on a new highly correlated five-dimensional potential energy surface. This surface was fitted to more than 60 000 ab initio points with a root mean square error of $\sim$ 1-2 cm$^{-1}$ in the region of the potential well whose depth is -374.0 cm$^{-1}$. The rotationally inelastic rate coefficients have been combined with spectroscopic data to generate the non-equilibrium spectrum of CH$_2$NH towards the interstellar molecular cloud Sgr~B2(N). The transition $1_{10}\to 1_{11}$ at 5.29 GHz is found to be inverted and the predicted weak maser emission spectrum is in excellent agreement with new observations performed with the 100-meter Green Bank Telescope.

astro-ph.GA↗