Observation of an Associative State in Aqueous Hydroxide
(2025) In Journal of the American Chemical Society 147(11). p.9190-9197- Abstract
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... (More)
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.
(Less)
- author
- organization
- publishing date
- 2025
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of the American Chemical Society
- volume
- 147
- issue
- 11
- pages
- 8 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:40064888
- scopus:86000490829
- ISSN
- 0002-7863
- DOI
- 10.1021/jacs.4c13453
- language
- English
- LU publication?
- yes
- id
- 4095706c-0152-4cac-a4d4-0e94e3993fa6
- date added to LUP
- 2025-06-27 11:27:05
- date last changed
- 2025-07-11 11:58:37
@article{4095706c-0152-4cac-a4d4-0e94e3993fa6, abstract = {{<p>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.</p>}}, author = {{Yin, Zhong and Krasnov, Pavel and Thürmer, Stephan and Chatzigeorgiou, Evanthia and Cui, Yitao and Yamazoe, Kosuke and Miyawaki, Jun and Tokushima, Takashi and Såthe, Conny and Gråsjö, Johan and Harada, Yoshihisa and Polyutov, Sergey P. and Wörner, Hans Jakob and Odelius, Michael and Gelmukhanov, Faris and Rubensson, Jan Erik and Kimberg, Victor}}, issn = {{0002-7863}}, language = {{eng}}, number = {{11}}, pages = {{9190--9197}}, publisher = {{The American Chemical Society (ACS)}}, series = {{Journal of the American Chemical Society}}, title = {{Observation of an Associative State in Aqueous Hydroxide}}, url = {{http://dx.doi.org/10.1021/jacs.4c13453}}, doi = {{10.1021/jacs.4c13453}}, volume = {{147}}, year = {{2025}}, }