\textit{Ab initio} quantum scattering calculations and a new potential energy surface for the HCl($X^1\Sigma^+$)-O$_{2}$($X^3\Sigma^-_g$) system: collision-induced line-shape parameters for O$_{2}$-perturbed R(0) 0-0 line in H$^{35}$Cl

• URL: http://arxiv.org/abs/2309.08413v1
• Date: Fri, 15 Sep 2023 14:18:01 GMT
• Title: \textit{Ab initio} quantum scattering calculations and a new potential energy surface for the HCl($X^1\Sigma^+$)-O$_{2}$($X^3\Sigma^-_g$) system: collision-induced line-shape parameters for O$_{2}$-perturbed R(0) 0-0 line in H$^{35}$Cl
• Authors: Artur Olejnik (1), Hubert J\'o\'zwiak (1), Maciej Gancewski (1), Ernesto Quintas-S\'anchez (2), Richard Dawes (2), Piotr Wcis{\l}o (1) ((1) Institute of Physics, Faculty of Physics, Astronomy and Informatics, Nicolaus Copernicus University in Toru\'n, Poland (2) Department of Chemistry, Missouri University of Science and Technology, USA)
• Abstract summary: We report the first fully quantum calculations of collisional perturbations of the shape of a pure rotational line in H$35$ perturbed by an air-relevant molecule. This result constitutes an important step towards computational population of databases with accurate textit-ab initio line-shape parameters for molecular systems of terrestrial atmospheric importance.
• Score: 0.5360099819403186
• License: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Abstract: The remote sensing of abundance and properties of HCl -- the main atmospheric reservoir of Cl atoms which directly participate in ozone depletion -- are important for monitoring the partitioning of chlorine between "ozone-depleting" and "reservoir" species. Such remote studies require knowledge of the shapes of molecular resonances of HCl, which are perturbed by collisions with the molecules of the surrounding air. In this work, we report the first fully quantum calculations of collisional perturbations of the shape of a pure rotational line in H$^{35}$Cl perturbed by an air-relevant molecule (as the first model system we choose the R(0) line in HCl perturbed by O$_2$). The calculations are performed on our new highly-accurate HCl($X^1\Sigma^+$)-O$_2$($X^3\Sigma^-_g$) potential energy surface. In addition to pressure broadening and shift, we determine also their speed dependencies and the complex Dicke parameter. This gives important input to the community discussion on the physical meaning of the complex Dicke parameter and its relevance for atmospheric spectra (previously, the complex Dicke parameter for such systems was mainly determined from phenomenological fits to experimental spectra and the physical meaning of its value in that context is questionable). We also calculate the temperature dependence of the line-shape parameters and obtain agreement with the available experimental data. We estimate the total combined uncertainties of our calculations at 2\% relative RMSE residuals in the simulated line shape at 296~K. This result constitutes an important step towards computational population of spectroscopic databases with accurate \textit{ab initio} line-shape parameters for molecular systems of terrestrial atmospheric importance.

Related papers

• Rate Coefficients for Rotational State-to-State Transitions in H$_2$O + H$_2$ Collisions as Predicted by Mixed Quantum/Classical Theory (MQCT) [0.0]
  A new database of collisional rate coefficients for transitions between the rotational states of H$$O collided with H$$ background gas is developed. The goal is to expand over the other existing databases in terms of the rotational states of water (200 states are included here) and the rotational states of hydrogen (10 states)
  arXiv  Detail & Related papers  (2024-08-23T19:19:53Z)
• Hessian QM9: A quantum chemistry database of molecular Hessians in implicit solvents [0.31457219084519]
  Hessian QM9 is the first database of equilibrium configurations and numerical Hessian matrices. We show that incorporating second derivatives of the potential energy surface into the loss function of a MLIP significantly improves the prediction of vibrational frequencies in all solvent environments.
  arXiv  Detail & Related papers  (2024-08-15T08:16:11Z)
• Impact of the ligand deformation on the $\mathcal{P}$,$\mathcal{T}$-violation effects in the YbOH molecule [77.34726150561087]
  The ytterbium monohydroxide is a promising molecule for a new physics searches. We have calculated the value of $l$-doubling for the YbOH molecule with approximation of fixed O-H bond length.
  arXiv  Detail & Related papers  (2022-08-15T08:16:19Z)
• Gaussian Process Regression for Absorption Spectra Analysis of Molecular Dimers [68.8204255655161]
  We discuss an approach based on a machine learning technique, where the parameters for the numerical calculations are chosen from Gaussian Process Regression (GPR) This approach does not only quickly converge to an optimal parameter set, but in addition provides information about the complete parameter space. We find that indeed the GPR gives reliable results which are in agreement with direct calculations of these parameters using quantum chemical methods.
  arXiv  Detail & Related papers  (2021-12-14T17:46:45Z)
• Graph neural networks for fast electron density estimation of molecules, liquids, and solids [0.0]
  We present a machine learning framework for the prediction of $rho(vecr)$. The model is tested across multiple data sets of molecules (QM9), liquid ethylene carbonate electrolyte (EC) and LixNiyMnzCo (1-y-z)O2 lithium ion battery cathodes (NMC)
  arXiv  Detail & Related papers  (2021-12-01T16:57:31Z)
• Unsupervised Spectral Unmixing For Telluric Correction Using A Neural Network Autoencoder [58.720142291102135]
  We present a neural network autoencoder approach for extracting a telluric transmission spectrum from a large set of high-precision observed solar spectra from the HARPS-N radial velocity spectrograph.
  arXiv  Detail & Related papers  (2021-11-17T12:54:48Z)
• Mechanism for particle fractionalization and universal edge physics in quantum Hall fluids [58.720142291102135]
  We advance a second-quantization framework that helps reveal an exact fusion mechanism for particle fractionalization in FQH fluids. We also uncover the fundamental structure behind the condensation of non-local operators characterizing topological order in the lowest-Landau-level (LLL)
  arXiv  Detail & Related papers  (2021-10-12T18:00:00Z)
• Rovibrational structure of the Ytterbium monohydroxide molecule and the $\mathcal{P}$,$\mathcal{T}$-violation searches [68.8204255655161]
  The energy gap between levels of opposite parity, $l$-doubling, is of a great interest. The influence of the bending and stretching modes on the sensitivities to the $mathcalP$,$mathcalT$-violation requires a thorough investigation.
  arXiv  Detail & Related papers  (2021-08-25T20:12:31Z)
• $\mathcal{P}$,$\mathcal{T}$-odd effects for RaOH molecule in the excited vibrational state [77.34726150561087]
  Triatomic molecule RaOH combines the advantages of laser-coolability and the spectrum with close opposite-parity doublets. We obtain the rovibrational wave functions of RaOH in the ground electronic state and excited vibrational state using the close-coupled equations derived from the adiabatic Hamiltonian.
  arXiv  Detail & Related papers  (2020-12-15T17:08:33Z)
• Predicting molecular dipole moments by combining atomic partial charges and atomic dipoles [3.0980025155565376]
  "MuML" models are fitted together to reproduce molecular $boldsymbolmu$ computed using high-level coupled-cluster theory. We demonstrate that the uncertainty in the predictions can be estimated reliably using a calibrated committee model.
  arXiv  Detail & Related papers  (2020-03-27T14:35:37Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.