Ultrafast and Radiation-Hard Lead Halide Perovskite Nanocomposite Scintillators.
Andrea ErroiSara MeccaMatteo L ZaffalonIsabel FrankFrancesco CarulliAlessia CemmiIlaria Di SarcinaDoriana DebellisFrancesca RossiFrancesca CovaKristof PauwelsMichele MauriJacopo PeregoValerio PinchettiAngiolina ComottiFrancesco MeinardiAnna VeddaEtiennette AuffrayLuca BeverinaSergio BrovelliPublished in: ACS energy letters (2023)
The use of scintillators for the detection of ionizing radiation is a critical aspect in many fields, including medicine, nuclear monitoring, and homeland security. Recently, lead halide perovskite nanocrystals (LHP-NCs) have emerged as promising scintillator materials. However, the difficulty of affordably upscaling synthesis to the multigram level and embedding NCs in optical-grade nanocomposites without compromising their optical properties still limits their widespread use. In addition, fundamental aspects of the scintillation mechanisms are not fully understood, leaving the scientific community without suitable fabrication protocols and rational guidelines for the full exploitation of their potential. In this work, we realize large polyacrylate nanocomposite scintillators based on CsPbBr 3 NCs, which are synthesized via a novel room temperature, low waste turbo-emulsification approach, followed by their in situ transformation during the mass polymerization process. The interaction between NCs and polymer chains strengthens the scintillator structure, homogenizes the particle size distribution and passivates NC defects, resulting in nanocomposite prototypes with luminescence efficiency >90%, exceptional radiation hardness, 4800 ph/MeV scintillation yield even at low NC loading, and ultrafast response time, with over 30% of scintillation occurring in the first 80 ps, promising for fast-time applications in precision medicine and high-energy physics. Ultrafast radioluminescence and optical spectroscopy experiments using pulsed synchrotron light further disambiguate the origin of the scintillation kinetics as the result of charged-exciton and multiexciton recombination formed under ionizing excitation. This highlights the role of nonradiative Auger decay, whose potential impact on fast timing applications we anticipate via a kinetic model.
Keyphrases
- room temperature
- energy transfer
- quantum dots
- reduced graphene oxide
- high resolution
- carbon nanotubes
- ionic liquid
- radiation induced
- solar cells
- visible light
- gold nanoparticles
- high speed
- sensitive detection
- mental health
- aqueous solution
- solid phase extraction
- human health
- highly efficient
- healthcare
- single molecule
- heavy metals
- clinical practice
- public health
- perovskite solar cells
- tissue engineering
- dna repair
- loop mediated isothermal amplification
- high efficiency
- real time pcr
- global health
- oxidative stress
- sewage sludge
- label free