丙酮酸的单重态-三重态间隙。

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-10-01 DOI:10.1021/jacs.5c13075

E Michi Burrow,Javier Carmona-García,Connor J Clarke,Basile F E Curchod,Jan R R Verlet

{"title":"丙酮酸的单重态-三重态间隙。","authors":"E Michi Burrow,Javier Carmona-García,Connor J Clarke,Basile F E Curchod,Jan R R Verlet","doi":"10.1021/jacs.5c13075","DOIUrl":null,"url":null,"abstract":"Understanding the gas-phase photochemistry of pyruvic acid is crucial to assessing its role and evolution in the atmosphere and relies on knowledge of the relative energy gaps between the atmospherically relevant excited electronic states of the molecule. However, accurate determination of these gaps, particularly between the lowest excited singlet and triplet states, has remained elusive due to the challenge of directly interrogating triplet states of the isolated molecule. In this work, we combine anion photoelectron spectroscopy and computational photochemistry to determine that the adiabatic S1-T1 energy gap of pyruvic acid is 0.29 ± 0.04 eV. This study provides a reference value for the singlet-triplet energy gap of pyruvic acid and validates an approach that combines theory and experiment to determine energy gaps for volatile organic compounds of atmospheric interest.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"7 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The Singlet-Triplet Gap of Pyruvic Acid.\",\"authors\":\"E Michi Burrow,Javier Carmona-García,Connor J Clarke,Basile F E Curchod,Jan R R Verlet\",\"doi\":\"10.1021/jacs.5c13075\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Understanding the gas-phase photochemistry of pyruvic acid is crucial to assessing its role and evolution in the atmosphere and relies on knowledge of the relative energy gaps between the atmospherically relevant excited electronic states of the molecule. However, accurate determination of these gaps, particularly between the lowest excited singlet and triplet states, has remained elusive due to the challenge of directly interrogating triplet states of the isolated molecule. In this work, we combine anion photoelectron spectroscopy and computational photochemistry to determine that the adiabatic S1-T1 energy gap of pyruvic acid is 0.29 ± 0.04 eV. This study provides a reference value for the singlet-triplet energy gap of pyruvic acid and validates an approach that combines theory and experiment to determine energy gaps for volatile organic compounds of atmospheric interest.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"7 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.5c13075\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.5c13075","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

摘要

了解丙酮酸的气相光化学对于评估其在大气中的作用和演变至关重要，并且依赖于分子的大气相关激发态之间的相对能隙的知识。然而，精确地确定这些间隙，特别是最低激发单重态和三重态之间的间隙，由于直接询问孤立分子的三重态的挑战，仍然是难以捉摸的。本文将阴离子光电子能谱与计算光化学相结合，确定了丙酮酸的绝热S1-T1能隙为0.29±0.04 eV。本研究为丙酮酸的单重态-三重态能隙提供了参考价值，并验证了一种理论与实验相结合的方法来确定大气中挥发性有机化合物的能隙。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

The Singlet-Triplet Gap of Pyruvic Acid.

Understanding the gas-phase photochemistry of pyruvic acid is crucial to assessing its role and evolution in the atmosphere and relies on knowledge of the relative energy gaps between the atmospherically relevant excited electronic states of the molecule. However, accurate determination of these gaps, particularly between the lowest excited singlet and triplet states, has remained elusive due to the challenge of directly interrogating triplet states of the isolated molecule. In this work, we combine anion photoelectron spectroscopy and computational photochemistry to determine that the adiabatic S1-T1 energy gap of pyruvic acid is 0.29 ± 0.04 eV. This study provides a reference value for the singlet-triplet energy gap of pyruvic acid and validates an approach that combines theory and experiment to determine energy gaps for volatile organic compounds of atmospheric interest.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.