The dynamics of chemical reactions in solution are of paramount importance in fields ranging from biology to materials science. Because the hydrogen-bond network and proton dynamics govern the behavior of aqueous solutions, they have been the subject of numerous studies over the years. Here, we report the observation of a previously unknown associative state in the hydroxide ion that forms when a proton from a neighboring water molecule approaches the hydroxide ion, utilizing resonant inelastic soft X-ray scattering (RIXS) and quantum dynamical simulations. State-of-the-art theoretical analysis reveals state mixing in the electronically excited states between aqueous hydroxide ions and the solvent. Our results give new insights into chemical bonding and excited-state dynamics in the aqueous environment. This investigation of associative states opens up new pathways for spectroscopic studies of chemical reaction dynamics and lays the foundation for directly accessing dynamic proton exchange in solution.
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http://dx.doi.org/10.1021/jacs.4c13453 | DOI Listing |
J Am Chem Soc
March 2025
Theoretical Chemistry and Biology, KTH Royal Institute of Technology, Stockholm 106 91, Sweden.
The dynamics of chemical reactions in solution are of paramount importance in fields ranging from biology to materials science. Because the hydrogen-bond network and proton dynamics govern the behavior of aqueous solutions, they have been the subject of numerous studies over the years. Here, we report the observation of a previously unknown associative state in the hydroxide ion that forms when a proton from a neighboring water molecule approaches the hydroxide ion, utilizing resonant inelastic soft X-ray scattering (RIXS) and quantum dynamical simulations.
View Article and Find Full Text PDFThroughout the Victorian era, the metaphor "living fossil" repeatedly crisscrossed social and scientific domains. The term existed in popular culture before and after Darwin's Origin. Most notably, it also operated as two distinct scientific concepts, one introduced by Darwin and another in cultural evolutionists' depiction of human living fossils.
View Article and Find Full Text PDFGenes Brain Behav
April 2025
Department of Psychology, University at Buffalo, Buffalo, New York, USA.
Addiction vulnerability is associated with the tendency to attribute incentive salience to reward predictive cues. Both addiction and the attribution of incentive salience are influenced by environmental and genetic factors. To characterize the genetic contributions to incentive salience attribution, we performed a genome-wide association study (GWAS) in a cohort of 1596 heterogeneous stock (HS) rats.
View Article and Find Full Text PDFMem Cognit
March 2025
Leuven Institute of Criminology, KU Leuven, Leuven, Belgium.
While generally reliable, human memory is susceptible to distortions such as false memories. This study investigates the relationships among the emotional valence of events, mood states, and the formation of false autobiographical memories, applying the blind implantation method. We examine the impact of positive and negative moods, combined with the emotional valence of events (negative vs.
View Article and Find Full Text PDFISA Trans
February 2025
College of Intelligent Systems Science and Engineering, Harbin Engineering University, Harbin 150001, China. Electronic address:
This study addresses the control challenges of distributed prescribed-time maneuvers for underactuated unmanned surface vessels (USVs) operating in affine formation under adverse conditions, including ocean disturbances, unmodeled dynamics, and denial-of-service (DoS) attacks. The research develops a control scheme that enables USVs to perform complex maneuvers such as translation, shearing, rotation, and scaling, despite intermittent communication failures due to periodic DoS attacks. The approach integrates a distributed prescribed-time observer (DPTO) for each vessel to monitor local time-varying desired states, coupled with an adaptive prescribed-time local tracking control (APTLTC) strategy that drives the USV to track the desired states.
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