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Multi-Noncentrosymmetric Polar Order in 2D Hybrid Lead Chloride with Broadband Emission and High-Temperature Second-Harmonic Generation Switching

28 October 2024

Title: Multi-Noncentrosymmetric Polar Order in 2D Hybrid Lead Chloride with Broadband Emission and High-Temperature Second-Harmonic Generation Switching

Authors: M. Mączka, J.K. Zaręba, A. Gągor, K. Fedoruk-Piskorska, D. Stefańska, D. Drozdowski, M. Ptak, A. Sieradzki

Journal: ACS Applied Materials & Interfaces

DOI: 10.1021/acsami.4c14244

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In their recent article, prof. Mączka’s group employed an organic amine halogenation strategy to induce polar order in a 2D lead bromide perovskite. The grown CPA2PbBr4 single crystals (CPA= 3-chloropropylammonium) have been studied using thermal, X-ray diffraction, Raman, pyroelectric current, dielectric and optical methods. They showed that in the 80-400 K range CPA2PbBr4 features one centrosymmetric and three polar phases. The high-temperature phase transition near 350 K is of a ferroelectric nature. CPA2PbCl4 features negative linear thermal expansion and broadband emission, which is white above 180 K. Remarkably, CPA2PbCl4 also demonstrates high-temperature SHG on−off switching with a high contrast ratio of 300:1 along with good switching stability. The researchers also proposed a new method to quantify the thermal responsiveness of SHG-switchable materials using the time requirement parameter. They proposed that for most real-life applications, the time requirement parameter should be in the range of single seconds, which would require materials with very narrow thermal hysteresis.

Overall, the reported findings show that the halogenation strategy has led to the discovery of a rare example of an RP perovskite exhibiting coexistence of white-light emission, SHG onoff thermal bistability, ferroelectricity, and negative linear thermal expansion.

Highlights:

  • Novel 2D lead chloride perovskite has been synthesized
  • This compound possesses three polar phases, exhibits ferroelectric properties and broadband emission
  • It also demonstrates high-temperature SHG on−off switching with a high contrast ratio along with good switching stability
  • SHG study also sets new standards for the field of SHG switching by providing a method to quantify the thermal responsiveness of SHG-switchable materials using the time requirement parameter

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