期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 117, 期 52, 页码 32954-32961出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2012545117
关键词
supramolecular; encapsulation; THz spectroscopy; ab initio molecular dynamics; confined water
资金
- Deutsche Forschungsgemeinschaft (DFG) (German Research Foundation) under Germany's Excellence Strategy [EXC 2033, 390677874]
- DFG [GRK 2376, 331085229]
- European Research Council [695437]
- Office of Science, Office of Basic Energy Sciences of the US Department of Energy at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
- Division of Chemical Sciences, Geosciences, and Bioscience of the US Department of Energy at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
- NIH Postdoctoral Fellowship [1F32GM129933-01]
- Office of Science of the US Department of Energy [DE-AC02-05CH11231]
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [F32GM129933] Funding Source: NIH RePORTER
Water under nanoconfinement at ambient conditions has exhibited low-dimensional ice formation and liquid-solid phase transitions, but with structural and dynamical signatures that map onto known regions of water's phase diagram. Using terahertz (THz) absorption spectroscopy and ab initio molecular dynamics, we have investigated the ambient water confined in a supramolecular tetrahedral assembly, and determined that a dynamically distinct network of 9 +/- 1 water molecules is present within the nanocavity of the host. The low-frequency absorption spectrum and theoretical analysis of the water in the Ga4L612- host demonstrate that the structure and dynamics of the encapsulated droplet is distinct from any known phase of water. A further inference is that the release of the highly unusual encapsulated water droplet creates a strong thermodynamic driver for the high-affinity binding of guests in aqueous solution for the Ga4L612- supramolecular construct.
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