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Second-Harmonic-Generation Switching via Pressure-Suppressed Dynamical Disorder.

Dequan Jiang1, Xingxing Jiang2, Xue Zhang3

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Researchers discovered pressure-induced second-harmonic-generation (SHG) switching in ammonium chloride (NH4Cl) via a dynamic disorder-order phase transition. This material exhibits record-breaking reversible switching and unique triplet switching behavior for optical applications.

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Area of Science:

  • Materials Science
  • Crystallography
  • Nonlinear Optics

Background:

  • Second-harmonic-generation (SHG) switching is crucial for optical switches and bistable storage.
  • Temperature-induced phase transitions are known for SHG switching, but pressure-induced mechanisms are less explored and often lack sensitivity.
  • Developing pressure-sensitive materials with reliable switching is essential for advanced photonic devices.

Purpose of the Study:

  • To investigate pressure-induced "dynamical disorder-order" phase transitions for triggering SHG and SHG switching in NH4Cl.
  • To explore the potential of NH4Cl as a pressure-sensitive material for optical switching applications.
  • To understand the underlying mechanism of pressure-driven SHG switching and its cyclicity.

Main Methods:

  • In situ high-pressure X-ray diffraction (XRD) to analyze structural changes.
  • Molecular vibrational spectroscopy and Brillouin scattering to study phase transitions.
  • Optical spectroscopy to measure SHG response across various wavelengths.
  • Molecular dynamics simulations to elucidate the role of hydrogen bonding.

Main Results:

  • NH4Cl exhibits a pressure-induced "dynamical disorder-order" phase transition at 1 GPa, triggering SHG.
  • The material shows reversible "off-on" SHG switching for up to 50 cycles, a record for pressure-driven materials.
  • A second SHG "on-off" switching occurs at 14 GPa, making NH4Cl the first triplet SHG "off-on-off" switching material.
  • N-H···Cl hydrogen bonding plays a critical role in the pressure-induced mechanism.

Conclusions:

  • Pressure-induced "dynamical disorder-order" phase transition is an effective strategy for SHG switching in NH4Cl.
  • NH4Cl demonstrates high sensitivity, cyclicity, and unique multistate switching behavior under pressure.
  • The findings provide insights for designing novel multistable SHG switching materials for photoswitches and information storage.