InfoMetricsFiguresRef. ACS Physical Chemistry AuASAPArticle This publication is Open Access under the license indicated. Learn More CiteCitationCitation and abstractCitation and referencesMore citation options ShareShare onFacebookX (Twitter)WeChatLinkedInRedditEmailJump toExpandCollapse EditorialDecember 17, 2024Ultrafast Spectroscopy of Chemical TransformationsClick to copy article linkArticle link copied!Tanja Cuk*Tanja Cuk*email: [email protected]More by Tanja Cukhttps://orcid.org/0000-0002-1635-2946Jin Z. Zhang*Jin Z. Zhang*email: [email protected]More by Jin Z. Zhanghttps://orcid.org/0000-0003-3437-912XGemma Solomon*Gemma Solomon*email: [email protected]More by Gemma Solomonhttps://orcid.org/0000-0002-2018-1529Open PDFACS Physical Chemistry AuCite this: ACS Phys. Chem Au 2024, XXXX, XXX, XXX-XXXClick to copy citationCitation copied!https://pubs.acs.org/doi/10.1021/acsphyschemau.4c00100https://doi.org/10.1021/acsphyschemau.4c00100Published December 17, 2024 Publication History Received 27 November 2024Published online 17 December 2024editorial© 2024 American Chemical Society. This publication is licensed under CC-BY-NC-ND 4.0 . License Summary*You are free to share (copy and redistribute) this article in any medium or format within the parameters below:Creative Commons (CC): This is a Creative Commons license.Attribution (BY): Credit must be given to the creator.Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license*DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. This publication is licensed underCC-BY-NC-ND 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS Publications© 2024 American Chemical SocietySubjectswhat are subjectsArticle subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article.NickelPhotodissociationPhysical chemistryProbesUltrafast spectroscopySpecial IssuePublished as part of ACS Physical Chemistry Au special issue "Ultrafast Spectroscopy of Chemical Transformations".Chemical transformations have long been a focus of physical chemistry─whether initiated by heat, light, or charged particles like electrons. Such transformations often involve fundamental processes such as bond breaking and formation, energy transfer, proton transfer, and electron transfer that can occur on ultrafast time scales. These processes are critical to existing industry as well as emerging technologies including areas such as catalysts, energy conversion and storage, sensing, and optronics. In parallel, ultrafast probes of chemical transformations have continued to advance. New developments include new ways to combine ultrafast probes with in situ reactions, whether in the gas or condensed phase. Other advancements include development of probes that reach the attosecond time domain, spectroscopies that are multidimensional, and ultrafast pulses in the X-ray regions. To highlight recent advances in the field, we are pleased to present this ACS Physical Chemistry Au virtual special issue on "Ultrafast Spectroscopy of Chemical Transformations", which includes papers covering different aspects of ultrafast studies of dynamics of interest in physical chemistry.The Article by Lynam and Hunt et al. studies the solution phase structure, vibrational properties, and ultrafast relaxation dynamics of the precatalyst species Mn(ppy)(CO)4 in solution using ultrafast two-dimensional infrared (2D-IR) spectroscopy (DOI: 10.1021/acsphyschemau.4c00037). Time-resolved IR results reveal the presence of ultrafast (few ps) intramolecular vibrational energy redistribution between carbonyl stretching modes prior to vibrational relaxation, which is relatively solvent-insensitive and suggests limited solvent–solute interactions in the ground electronic state. The study provides a detailed picture of the complex potential energy surface, bonding and vibrational dynamics of Mn(ppy)(CO)4.The Letter by Schlenker et al. focuses on ultrafast pump–photolysis–probe transient absorption (TA) spectroscopy on the intermediate TAHzH· heptazinyl radical produced from an excited state proton-coupled electron transfer (PCET) reaction of trianisole heptazine (TAHz), as a monomeric analogue for carbon nitride, with 4-methoxyphenol (DOI: 10.1021/acsphyschemau.4c00030). The results demonstrate an optically gated photolysis that releases H· and regenerates ground state TAHz. The TAHzH· radical signature at 520 nm had a lifetime of 7.0 ps, and its photodissociation by the photolysis pulse is demonstrated by the ground state bleach recovery of the closed-shell neutral TAHz, as previously predicted as evidence of a dissociative πσ* state. This first experimental demonstration of photolysis of the TAHzH· heptazinyl radical through a repulsive πσ* state is a critical feature of the proposed reaction mechanisms involving water oxidation and CO2 reduction.The Letter by McCaslin and Ramasesha et al. investigates the ultrafast photodissociation of nickel tetracarbonyl─a prototypical metal–ligand model system at 197 nm using mid-infrared TA spectroscopy to probe the bound C═O stretching modes (DOI: 10.1021/acsphyschemau.4c00033). Evidence was found for the picosecond time scale production of highly vibronically excited nickel dicarbonyl and nickel monocarbonyl, in marked contrast with a prior investigation at 193 nm. Spectral evolution with a 50 ps time constant suggests an additional dissociation step, and the absence of any corresponding growth in signal strongly indicates the production of bare Ni, a heretofore unreported product from single-photon excitation of nickel tetracarbonyl.The Article by Burt and Warne et al. uses time-resolved extreme UV spectroscopy to investigate photodissociation within the iodobenzene C-band by photolyzing the carbon–iodine bond of iodobenzene at 200 nm and probing the ensuing dynamics at 10.3 nm (120 eV) over a 4 ps range (DOI: 10.1021/acsphyschemau.4c00036). Two product channels were observed and subsequently isolated using a global fitting method. Their onset times and energetics were assigned to distinct electron transfer dynamics initiated following site-selective ionization of the iodine photoproducts, enabling the electronic states of the phenyl fragments to be identified using a classical over-the-barrier model for electron transfer. In combination with previous theoretical work, a detailed picture was developed for the corresponding neutral photochemistry and photophysics.The paper by Tiwari et al. studies the impact of entasis caused by stress induced by the surrounding lattice on the excited state dynamics of a prototypical copper(I)-based photocatalyst in single crystal form (DOI: 10.1021/acsphyschemau.4c00047). Using femtosecond broadband TA spectroscopy, triplet state formation from the entactic state is studied and to be faster (∼3.9 ps) in crystals compared to solution (∼11.3 ps). The observed faster intersystem crossing in crystals hints toward the possible existence of distorted square planar geometry with higher spin–orbit coupling at the minima of the S1 state. The influence of entasis on vibrationally coherent photoinduced Jahn–Teller distortions was also discussed. The findings reveal the photophysical properties of the copper complex under lattice-induced stress, which may enhance the broader applicability of the entatic state concept in other transition metal systems.The Letter by Zhang et al. focuses on carrier spin dynamics in metal halide perovskite magic sized clusters (PMSCs) with unique optical and electronic properties (DOI: 10.1021/acsphyschemau.4c00051). The study found that for ultrasmall sized nanoclusters, electron-surface (of defect) scattering likely plays an important role in carrier spin relaxation. The electron spin lifetime is shorter in such PMSCs compared to similar perovskite quantum dots due to larger surface-to-volume ratio and increased electron-surface scattering.Somewhat different to ultrafast studies based on ultrafast lasers, the Perspective by Tickner, Singh, Zhivonitko and Telkki provides a review on the approach of "ultrafast" nuclear magnetic resonance (NMR) that uses spatial encoding to record an entire two-dimensional (2D) data set in just a single scan and can be applied to either Fourier-transform or Laplace-transform NMR (DOI: 10.1021/acsphyschemau.4c00042). Data acquisition times are significantly shorter than traditional 2D/Laplace NMR experiments, which allows monitoring of rapid chemical transformations. The Perspective also outlines the principles of ultrafast NMR and focuses on examples of its use to detect fast molecular conversions in situ with high temporal resolution, along with some future directions. It should be noted that the "ultrafast" time scale referred to here for NMR is on the millisecond to second time scales, which differs significantly from the ultrafast time scale based on lasers (fs and ps).Together, these articles provide a glimpse of recent activities in the study of ultrafast dynamics relevant to physical chemistry. Our thanks go to the authors for choosing to publish their work in ACS Physical Chemistry Au, and to the reviewers for their contributions to these papers. We hope you find these contributions as insightful as we have one can envision that the field of ultrafast studies in physical chemistry will continue to evolve and expand as a major subfield and contribute significantly to the development and advancement of chemistry.Author InformationClick to copy section linkSection link copied!Corresponding AuthorsTanja Cuk, Associate Editor, https://orcid.org/0000-0002-1635-2946, Email: [email protected]Jin Z. Zhang, Associate Editor, https://orcid.org/0000-0003-3437-912X, Email: [email protected]Gemma Solomon, Deputy Editor, https://orcid.org/0000-0002-2018-1529, Email: [email protected]NotesViews expressed in this editorial are those of the authors and not necessarily the views of the ACS.Cited By Click to copy section linkSection link copied!This article has not yet been cited by other publications.Download PDFFiguresReferences Get e-AlertsGet e-AlertsACS Physical Chemistry AuCite this: ACS Phys. Chem Au 2024, XXXX, XXX, XXX-XXXClick to copy citationCitation copied!https://doi.org/10.1021/acsphyschemau.4c00100Published December 17, 2024 Publication History Received 27 November 2024Published online 17 December 2024© 2024 American Chemical Society. This publication is licensed under CC-BY-NC-ND 4.0 . License Summary*You are free to share (copy and redistribute) this article in any medium or format within the parameters below:Creative Commons (CC): This is a Creative Commons license.Attribution (BY): Credit must be given to the creator.Non-Commercial (NC): Only non-commercial uses of the work are permitted. No Derivatives (ND): Derivative works may be created for non-commercial purposes, but sharing is prohibited. View full license*DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. Article Views-Altmetric-Citations-Learn about these metrics closeArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.Recommended Articles FiguresReferencesThis publication has no figures.This publication has no References.

Tanja Cuk

Jin Z. Zhang

Gemma Solomon

ACS Physical Chemistry Au

ACS Physical Chemistry Au是一本开放获取期刊，发表有关物理化学领域各方面原创性的基础和应用研究。该期刊出版了物理化学，生物物理化学，化学物理学，物理学，材料科学领域科学家和工程师感兴趣的原创实验，计算和理论研究。稿件接收的一个基本标准是可以提供新的物理见解或开发了具有广泛兴趣的新方法。

期刊收录研究方向：
分子，团簇和气溶胶；生物物理学，生物材料，液体和软物质；能源、材料和催化。
ACS Physical Chemistry Au is an open access journal, which publishes original, fundamental and applied research on all aspects of physical chemistry. The journal publishes new and original experimental, computational and theoretical research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An essential criterion for acceptance is that the manuscript provides new physical insight or develops new tools and methods of general interest. Some major topical areas include:

Molecules, Clusters and Aerosols; Biophysics, Biomaterials, Liquids and Soft Matter; Energy, Materials and Catalysis

ACS Physical Chemistry Au is an open access journal that focuses on original fundamental and applied research in the field of physical chemistry. The journal publishes original experimental, computational, and theoretical research related to physical chemistry, biophysical chemistry, chemical physics, physics, and materials science, aiming to provide new insights or develop widely relevant new methods for physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. A fundamental criterion for acceptance is that the manuscript offers new physical insights or develops new tools and methods of general interest. Major research areas include: Molecules, Clusters and Aerosols; Biophysics, Biomaterials, Liquids and Soft Matter; Energy, Materials and Catalysis.

《ACS Physical Chemistry Au》是一本开放获取期刊，专注于物理化学领域的原创基础和应用研究。该期刊发表与物理化学、生物物理化学、化学物理学、物理学及材料科学相关的原创实验、计算和理论研究，旨在为物理化学家、生物物理化学家、化学物理学家、物理学家、材料科学家和工程师提供新的研究视角或开发具有广泛兴趣的新方法。稿件接受的基本标准是提供新的物理见解或开发具有普遍意义的新工具和方法。主要研究方向包括：分子、团簇和气溶胶；生物物理学、生物材料、液体和软物质；能源、材料和催化。

Ultrafast Spectroscopy of Chemical Transformations

ivySCI AI Smartly Parses PDF, Answers Researchers' Questions, and Helps You Understand Papers in Seconds

Journal Info

Category	Quartile
CHEMISTRY, PHYSICAL	2