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[Rb4Cl][Cd11In9Se26]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics.

Pengzhi Xie1,2, Qixian Ren2, Junwei Feng2

  • 1Xinjiang Key Laboratory of Energy Storage and Photoelectrocatalytic Materials; College of Chemistry and Chemical Engineering, Xinjiang Normal University, Urumqi, 830054, China.

Dalton Transactions (Cambridge, England : 2003)
|June 25, 2026
PubMed
Summary

Controlling the arrangement of T2 supertetrahedra in crystals is key for strong nonlinear optical (NLO) responses. This study uses zero-dimensional guests to align these units, enhancing NLO properties in new infrared crystals.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • Macroscopic nonlinear optical (NLO) properties are highly sensitive to the crystal lattice arrangement of building units like T2 supertetrahedra.
  • Disordered orientations lead to cancellation of microscopic hyperpolarizabilities, significantly reducing NLO coefficients.
  • Previous efforts focused on alkali and alkaline earth metals to regulate T2 supertetrahedron polymerization.

Purpose of the Study:

  • To investigate the use of zero-dimensional (0D) guest species within salt-inclusion chalcogenides (SICs) to control the orientation of T2 supertetrahedra.
  • To synthesize and characterize a novel SIC, [Rb4Cl][Cd11In9Se26], by tuning the 3D host framework with a 0D guest polycation.
  • To evaluate the impact of guest-induced alignment on the NLO performance of the synthesized material.

Main Methods:

  • Synthesis of the salt-inclusion chalcogenide [Rb4Cl][Cd11In9Se26] by incorporating a 0D [Rb4Cl]3+ polycation into a [Cd11In9Se26]3- host framework.
  • Utilizing experimental measurements and theoretical calculations to analyze the structural and optical properties.
  • Employing first-principles calculations to determine the NLO coefficients.

Main Results:

  • The 0D [Rb4Cl]3+ polycation successfully induced highly uniform orientational alignment of T2 supertetrahedral units within the 3D host framework.
  • The synthesized SIC [Rb4Cl][Cd11In9Se26] exhibits a bandgap of 1.70 eV.
  • Calculated NLO coefficients include d15 = d31 = -10.845 pm V-1, d24 = d32 = -9.957 pm V-1, and d33 = 14.757 pm V-1.

Conclusions:

  • Zero-dimensional guest species can effectively modulate the alignment of 3D host frameworks in crystal structures.
  • This strategy offers a promising new approach for designing high-performance infrared (IR) nonlinear optical (NLO) crystals.
  • The synthesized [Rb4Cl][Cd11In9Se26] demonstrates significant potential for NLO applications.