Dissecting the hydrogen bond network of water: Charge transfer and nuclear quantum effects

IF 44.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2024-10-24 DOI:10.1126/science.ads4369

Mischa Flór, David M. Wilkins, Miguel de la Puente, Damien Laage, Giuseppe Cassone, Ali Hassanali, Sylvie Roke

引用次数: 0

Abstract

The molecular structure of water is dynamic, with intermolecular (H)-bond interactions being modified by both electronic charge transfer and nuclear quantum effects (NQEs). Electronic charge transfer and NQEs potentially change under acidic / basic conditions, but such details have not been measured. Here, we developed correlated vibrational spectroscopy, a symmetry-based method that distinctively separates interacting from non-interacting molecules in self- and cross-correlation spectra, giving access to previously inaccessible information. We found that OH − donated ~8% more negative charge to the H-bond network of water and H 3 O + accepted ~4% less negative charge from the H-bond network of water. D 2 O had ~9% more H-bonds compared to H 2 O, and acidic solutions displayed more dominant NQEs than basic ones.

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剖析水的氢键网络：电荷转移和核量子效应

水的分子结构是动态的，分子间（H）键的相互作用受电子电荷转移和核量子效应（NQEs）的影响。在酸性/碱性条件下，电子电荷转移和核量子效应可能会发生变化，但这些细节尚未得到测量。在此，我们开发了相关振动光谱法，这是一种基于对称性的方法，可在自相关和交叉相关光谱中将相互作用分子与非相互作用分子区分开来，从而获取以前无法获取的信息。我们发现，OH - 从水的 H 键网络中捐献的负电荷比水多 ~8% ，而 H 3 O + 从水的 H 键网络中接受的负电荷比水少 ~4%。D 2 O 的 H 键比 H 2 O 多 9%，酸性溶液比碱性溶液显示出更主要的 NQE。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

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