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  • Letter
  • Open Access

Electronic correlations influence on the anomalous constitutive law between the structure and spectra of hydrogen bonds

Rui Liu1, Xinrui Yang2, Famin Yu2, Depeng Zhang3,4, Lu Wang2, Ruhong Zhou5,6,7,*, and Zhigang Wang1,2,4,†

  • 1Key Laboratory of Material Simulation Methods & Software of Ministry of Education, College of Physics, Jilin University, Changchun 130012, China
  • 2Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China
  • 3Normal School, Shenyang University, Shenyang 110044, China
  • 4Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130023, China
  • 5Institute of Quantitative Biology, College of Life Sciences, Zhejiang University, Hangzhou 310058, China
  • 6Shanghai Institute for Advanced Study, Zhejiang University, Shanghai, China
  • 7Department of Chemistry, Columbia University, New York, New York, USA

  • *Contact author: rhzhou@zju.edu.cn
  • †Contact author: wangzg@jlu.edu.cn
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Phys. Rev. Research 6, L032019 – Published 25 July, 2024

DOI: https://doi.org/10.1103/PhysRevResearch.6.L032019

Abstract

Classical constitutive law between the structure and spectra has long been established in most physical processes and behaviors. Despite the emerging consensus, whether this law applies to microscopic systems adhering to quantum mechanics remains a fundamental and open question, due to limitations in even the most state-of-the-art experimental techniques. Here, we report an anomalous constitutive law of hydrogen bonds (X-H···Y) using a benchmark ab initio method. Notably, a donor X-H bond shortening occurred simultaneously with an unexpected redshift and enhanced intensity in IR spectra. The reason for donor X-H bond shortening is attributed to both the slowly increasing attractive force from the acceptor Y atom and the increasing short-range repulsive forces from other protons attached to the approaching acceptor Y atom. Furthermore, neither eliminating vibrational mixing nor introducing various physical effects make vibrational spectra respond to X-H bond shortening. Other structural-characterization NMR spectra provide robust evidence for this anomalous law. This anomalous law is ascribed to the interplay of electronic correlations. Our Letter thus inspires a reassessment of paradigms, which broadens the scope of microscopic behavior for finer control.

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Phys. Rev. Research 6, L032019– Published 25 July, 2024
  • Received 21 February 2024
  • Accepted 22 May 2024
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