Quantum Chemical Study on Interstellar Synthesis of Cytosine by the Automated Reaction Path Search

Komatsu, Yu; Suzuki, Takeshi

doi:10.1021/acsearthspacechem.2c00198

Cited by 9 publications

(11 citation statements)

References 31 publications

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“…In this paper, we present the energetically favorable gas formation of CH 3 OCH 3 and HCOOCH 3 , as typical interstellar COMs, via neutral and radical reactions within electronic ground states using an unbiased reaction pathway search method based on transition state theory without specifying the reaction pathways in advance. Recently, we have applied this methodology for the possible interstellar synthesis of nucleobases, aromatic heterocyclic molecules, and we demonstrate here that the approach effectively elucidates and validates the complex chemical networks of COMs, where CH 3 OCH 3 and HCOOCH 3 are smaller molecules than nucleobases. Several formation mechanisms of interstellar CH 3 OCH 3 have been proposed in previous studies, and they are comparable with our results; however, the mechanism of HCOOCH 3 formation is not understood, and it is worthwhile to provide a theoretical base with the comprehensive search.…”

Section: Introductionmentioning

confidence: 78%

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

Komatsu,

Furuya

2023

ACS Earth Space Chem.

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Recent astronomical observations have shown that interstellar complex organic molecules (COMs) exist even in cold environments (∼10 K), while various interstellar COMs have conventionally been detected in hot gas (≳100 K) in the vicinity of high-mass and low-mass protostars. However, the formation pathway of each interstellar COM remains largely unclear. In this work, we demonstrate that an automated reaction path search based on transition state theory, which does not require predetermined pathways, is helpful for investigating the formation pathways of interstellar COMs in the gas phase. The exhaustive search within the electronic ground states helps elucidate the complex chemical formation pathways of COMs at low temperatures. Here we examine the formation pathways of dimethyl ether (CH3OCH3) and methyl formate (HCOOCH3), which are often detected in the cold and hot gas of star-forming regions. We have identified a barrierless and exothermic formation path of CH3OCH3 by reaction between neutral species; CH3O + CH3 → H2CO···CH4 → CH3OCH3 is the most efficient path in the large chemical network constructed by our automated reaction path search and is comparable to those of previous studies. For HCOOCH3, we obtain complex pathways initiated from reactions between neutral species; HCOO and CH3 generate HCOOCH3 and its isomers without external energy. However, we also identified competing reaction branches producing CO2 + CH4 and CH3COOH, which would be more efficient than the formation of HCOOCH3. Thus, the gas-phase formation of HCOOCH3 through reactions between neutral species would not be efficient compared to CH3OCH3 formation.

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Section: Introductionmentioning

confidence: 78%

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

Komatsu,

Furuya

2023

ACS Earth Space Chem.

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“…Similarly, Komatsu and Suzuki utilized this method to unearth a new reaction pathway capable of forming cytosine, a key component of DNA and RNA molecules, in space . These studies underline the importance of deploying a variety of computational approaches to simulate prebiotic reactions.…”

Section: Introductionmentioning

confidence: 99%

“…Similarly, Komatsu and Suzuki utilized this method to unearth a new reaction pathway capable of forming cytosine, a key component of DNA and RNA molecules, in space. 62 These studies underline the importance of deploying a variety of computational approaches to simulate prebiotic reactions. Such explorations are essential for enhancing our understanding of the chemical processes that engendered life and elucidating the formation pathways of these pivotal molecules.…”

Section: ■ Introductionmentioning

confidence: 99%

Exploring the Chemical Space of C₂H₃NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

Panda

Chiranjibi

Awasthi

et al. 2023

ACS Earth Space Chem.

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The emergence of life remains a profoundly intriguing scientific question. Understanding the chemical processes that led to life's inception is vital to unravelling this mystery. Recent discoveries of C 2 H 3 NO isomers in the interstellar medium have stimulated further exploration into their chemistry. In this study, we use density functional theory to probe the potential energy surface of C 2 H 3 NO isomers, resulting in the identification of 33 isomers, with eleven low-lying isomers found to have relative energies below 50 kcal mol −1 . To explore potential reaction pathways, we performed a bimolecular reaction analysis with HCN and H 2 CO using an artificial force-induced approach for the automated search and location of minimum energy paths and transition states. Our results predict Oxiran-2-ylazanide (9) and isocyanomethanol (48) to be the kinetically favored products. Our study serves as a significant contribution to the understanding of prebiotic chemistry and offers a crucial step toward unveiling the chemical processes that might have led to life's emergence in the universe.

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“…54 Similarly, Komatsu and Suzuki employed this approach to identify a new reaction pathway that could lead to the formation of cytosine, an essential component of DNA and RNA molecules, in space. 55 In light of these studies, it is evident that exploring various computational approaches to simulate prebiotic reactions is essential for advancing our knowledge of the chemical processes that gave rise to life and understanding the formation pathways of these key molecules.…”

Section: Introductionmentioning

confidence: 99%

Exploring the Chemical Space of C3H2NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

Panda

Chiranjibi²,

Awasthi

et al. 2023

Preprint

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The emergence of life remains one of the most intriguing scientific questions, and understanding the chemical processes that led to it is essential. Recent discoveries of C3H2NO isomers in the interstellar medium have motivated further exploration of this molecular formula. Here, we use density functional theory to explore the potential energy surface of C3H2NO isomers, including acyclic and cyclic structures, and identify twelve low-lying isomers. We then investigate bimolecular reaction with HCN and H2CO using an artificial force-induced automated search and transition state search for the minimal energy routes. Our results predict the formation of Oxiran- 2-ylazanide and (Z)2-aminoacetaldehyde as the kinetically and thermodynamically controlled products, respectively. These results provide insights into the potential formation of biomarkers such as N-methyleneformamide in the interstellar medium, which have been found in recent years. Our study contributes to prebiotic chemistry and offers a critical step toward understanding the chemical processes that led to the emergence of life in the universe.

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Quantum Chemical Study on Interstellar Synthesis of Cytosine by the Automated Reaction Path Search

Cited by 9 publications

References 31 publications

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

Exploring the Chemical Space of C₂H₃NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

Exploring the Chemical Space of C3H2NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

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Quantum Chemical Study on Interstellar Synthesis of Cytosine by the Automated Reaction Path Search

Cited by 9 publications

References 31 publications

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH3OCH3 and HCOOCH3

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH3OCH3 and HCOOCH3

Exploring the Chemical Space of C2H3NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

Exploring the Chemical Space of C3H2NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life

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The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

The Automated Reaction Pathway Search Reveals the Energetically Favorable Synthesis of Interstellar CH₃OCH₃ and HCOOCH₃

Exploring the Chemical Space of C₂H₃NO Isomers and Bimolecular Reactions with Hydrogen Cyanide and Formaldehyde: Insights into the Emergence of Life