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<p>Water’s surface tension shows a nonlinear temperature dependence, including a reentrant increase in the supercooled regime — a longstanding puzzle in physical chemistry. Using molecular dynamics simulations, we uncover a structural mechanism linking microscopic ordering to macroscopic interfacial behaviour. Surface tension arises from the interplay between <i>ρ</i>-states, characterised by O–H alignment under surface symmetry breaking, and tetrahedral <i>S</i>-states stabilised in the subsurface by negative pressure. Water’s surface tension <i>γ</i> is governed by the interplay of their anisotropies: at intermediate temperatures, <i>ρ</i>-state anisotropy saturates while <i>S</i>-states remain weakly anisotropic, slowing the growth of <i>γ</i>. Upon deeper supercooling, however, <i>S</i>-states acquire orientational order, amplifying anisotropy and producing the reentrant rise. This unified framework explains both inflection points of <i>γ</i>(<i>T</i>) and establishes a structural–mechanical link between local hydrogen-bond motifs and interfacial stress, with implications for nucleation, cryopreservation, and ferroelectric-like ordering, and extending beyond water to other network-forming liquids.</p>

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Competing hydrogen-bond orders drive water’s anomalous surface tension

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月20日

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  • Jiaxing Yuan,
  • Kun Qiu,
  • Gang Sun,
  • Hajime Tanaka

摘要

Water’s surface tension shows a nonlinear temperature dependence, including a reentrant increase in the supercooled regime — a longstanding puzzle in physical chemistry. Using molecular dynamics simulations, we uncover a structural mechanism linking microscopic ordering to macroscopic interfacial behaviour. Surface tension arises from the interplay between ρ-states, characterised by O–H alignment under surface symmetry breaking, and tetrahedral S-states stabilised in the subsurface by negative pressure. Water’s surface tension γ is governed by the interplay of their anisotropies: at intermediate temperatures, ρ-state anisotropy saturates while S-states remain weakly anisotropic, slowing the growth of γ. Upon deeper supercooling, however, S-states acquire orientational order, amplifying anisotropy and producing the reentrant rise. This unified framework explains both inflection points of γ(T) and establishes a structural–mechanical link between local hydrogen-bond motifs and interfacial stress, with implications for nucleation, cryopreservation, and ferroelectric-like ordering, and extending beyond water to other network-forming liquids.