Physisorption of Water on Graphene: Subchemical Accuracy from Many-Body Electronic Structure Methods

Wet
carbon interfaces are ubiquitous in the natural world and exhibit
anomalous properties, which could be exploited by emerging technologies.
However, progress is limited by lack of understanding at the molecular
level. Remarkably, even for the most fundamental system (a single
water molecule interacting with graphene), there is no consensus on
the nature of the interaction. We tackle this by performing an extensive
set of complementary state-of-the-art computer simulations on some
of the world’s largest supercomputers. From this effort a consensus
on the water–graphene interaction strength has been obtained.
Our results have significant impact for the physical understanding,
as they indicate that the interaction is weaker than predicted previously.
They also pave the way for more accurate and reliable studies of liquid
water at carbon interfaces.

浸润碳界面在自然界中广泛存在，且具备反常的独特性质，可被新兴技术加以开发利用。然而，当前相关研究进展受限于分子层面认知的匮乏。值得注意的是，即便针对最基础的模型体系——单个水分子与石墨烯（graphene）的相互作用，学界对其相互作用的本质仍未达成共识。对此，我们依托全球顶尖超级计算机集群，开展了大规模互补型的前沿计算机模拟实验。通过本项研究工作，我们最终就水-石墨烯相互作用强度达成了学界共识。研究结果显著深化了我们对该体系的物理认知：其相互作用强度弱于此前的理论预测。同时，本研究也为碳界面处液态水的高精度、高可靠性研究铺平了道路。