Infrared bands of neutral gas-phase carbon clusters in a broad spectral range

Ferrari, Piero; Lemmens, Alexander K.; Redlich, Britta

doi:10.1039/d3cp05756a

Phys. Chem. Chem. Phys.

2024

DOI: 10.1039/d3cp05756a

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Infrared bands of neutral gas-phase carbon clusters in a broad spectral range

Piero Ferrari,

Alexander K. Lemmens,

Britta Redlich

Abstract: The identification of species in the interstellar medium requires precise and molecule-specific spectroscopic information in the laboratory framework, in broad spectral ranges and under conditions relevant to interstellar environments. In...

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2024

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Cited by 4 publications

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Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

Jia,

Wang,

Tian

et al. 2024

J. Phys. Chem. A

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Recently, novel algorithms and enhanced computational capabilities have created unprecedented opportunities to precisely determine the geometric structures of clusters through theoretical calculations. In this study, we extensively investigated and characterized the geometric arrangements of the carbon clusters C n (n = 2–60), employing the efficient ABCluster algorithm in conjunction with the gradient-corrected PBE and higher-accuracy B3LYP hybrid functional in density functional theory (DFT). New structures and a discernible structural growth pattern have been discovered. We observed a distinct preference in carbon clusters that transform from the linear chains (n = 2–9) to closed single-ring and planar structures (n = 10–27) and finally evolve to carbon cages (n = 28–60). A shortcut to construct the cage clusters was unveiled by inserting or rotating specific atoms within a distinct structural unit. The research results obtained from combining ABCluster with DFT calculations offer valuable new insights into the growth mechanisms and evolutionary trajectories of carbon clusters, providing a crucial theoretical framework for the development of innovative carbon-based materials and their potential applications.

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Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

Jia,

Wang,

Tian

et al. 2024

J. Phys. Chem. A

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show abstract

A Low-Order Permutationally Invariant Polynomial Approach to Learning Potential Energy Surfaces Using the Bond-Order Charge-Density Matrix: Application to C_n Clusters for n = 3–10, 20

Gutierrez-Cardenas,

Gibbas,

Whitaker

et al. 2024

J. Phys. Chem. A

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A representation for learning potential energy surfaces (PESs) in terms of permutationally invariant polynomials (PIPs) using the Hartree−Fock expression for electronic energy is proposed. Our approach is based on the oneelectron core Hamiltonian weighted by the configuration-dependent elements of the bond-order charge density matrix (CDM). While the previously reported model used an s-function Gaussian basis for the CDM, the present formulation is expanded with p-functions, which are crucial for describing chemical bonding. Detailed results are demonstrated on linear and cyclic C n clusters (n = 3−10) trained on extensive B3LYP/aug-cc-pVTZ data. The described method facilitates PES learning by reducing the root mean squared error (RMSE) by a factor of 5 relative to the s-function formulation and by a factor of 20 relative to the conventional PIP approach. This is equivalent to using CDM and an sp basis with a PIP of order M to achieve the same RMSE as with the conventional method with a PIP of order M + 2. Implications for large-scale problems are discussed using the case of the PES of the C 20 fullerene in full permutational symmetry.

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Laboratory infrared spectra and fragmentation chemistry of sulfur allotropes

Ferrari,

Berden,

Redlich

et al. 2024

Nat Commun

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Sulfur is one of six life-essential elements, but its path from interstellar clouds to planets and their atmospheres is not well known. Astronomical observations in dense clouds have so far been able to trace only 1 percent of cosmic sulfur, in the form of gas phase molecules and volatile ices, with the missing sulfur expected to be locked in a currently unidentified form. The high sulfur abundances inferred in icy and rocky solar system bodies indicate that an efficient pathway must exist from volatile atomic sulfur in the diffuse interstellar medium to some form of refractory sulfur. One hypothesis is the formation of sulfur allotropes, particularly of the stable S8. However, experimental information about sulfur allotropes under astrochemically relevant conditions, needed to constrain their abundance, is lacking. Here, we report the laboratory far-infrared spectra of sulfur allotropes and examine their fragmentation pathways. The spectra, including that of cold, isolated S8 with three bands at 53.5, 41.3 and 21.1 µm, form a benchmark for computational modelling, which show a near-perfect match with the experiments. The experimental fragmentation pathways of sulfur allotropes, key information for astrochemical formation/destruction models, evidence a facile fragmentation of S8. These findings suggest the presence of sulfur allotropes distributions in interstellar space or in the atmosphere of planets, dependent on the environmental conditions.

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Infrared bands of neutral gas-phase carbon clusters in a broad spectral range

Abstract: The identification of species in the interstellar medium requires precise and molecule-specific spectroscopic information in the laboratory framework, in broad spectral ranges and under conditions relevant to interstellar environments. In...

Cited by 4 publications

References 54 publications

Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

A Low-Order Permutationally Invariant Polynomial Approach to Learning Potential Energy Surfaces Using the Bond-Order Charge-Density Matrix: Application to C_n Clusters for n = 3–10, 20

Laboratory infrared spectra and fragmentation chemistry of sulfur allotropes

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Infrared bands of neutral gas-phase carbon clusters in a broad spectral range

Abstract: The identification of species in the interstellar medium requires precise and molecule-specific spectroscopic information in the laboratory framework, in broad spectral ranges and under conditions relevant to interstellar environments. In...

Cited by 4 publications

References 54 publications

Growth Patterns of Carbon Clusters Cn (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

Growth Patterns of Carbon Clusters Cn (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

A Low-Order Permutationally Invariant Polynomial Approach to Learning Potential Energy Surfaces Using the Bond-Order Charge-Density Matrix: Application to Cn Clusters for n = 3–10, 20

Laboratory infrared spectra and fragmentation chemistry of sulfur allotropes

Contact Info

Product

Resources

About

Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

Growth Patterns of Carbon Clusters C_n (n = 2–60) Identified via ABCluster Searching and DFT Benchmarking

A Low-Order Permutationally Invariant Polynomial Approach to Learning Potential Energy Surfaces Using the Bond-Order Charge-Density Matrix: Application to C_n Clusters for n = 3–10, 20