Highly Concentrated, Zwitterionic Ligand-Capped Mn2+:CsPb(BrxCl1–x)3 Nanocrystals as Bright Scintillators for Fast Neutron Imaging,ACS Energy Letters

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Highly Concentrated, Zwitterionic Ligand-Capped Mn2+:CsPb(BrxCl1–x)3 Nanocrystals as Bright Scintillators for Fast Neutron Imaging
ACS Energy Letters ( IF 19.3 ) Pub Date : 2021-11-12 , DOI: 10.1021/acsenergylett.1c01923
Federico Montanarella _{1,

2} , Kyle M McCall _{1,

2} , Kostiantyn Sakhatskyi _{1,

2} , Sergii Yakunin _{1,

2} , Pavel Trtik ₃ , Caterina Bernasconi _{1,

2} , Ihor Cherniukh _{1,

2} , David Mannes ₃ , Maryna I Bodnarchuk _{1,

2} , Markus Strobl ₃ , Bernhard Walfort ₄ , Maksym V Kovalenko _{1,

2}

Affiliation

Fast neutron imaging is a nondestructive technique for large-scale objects such as nuclear fuel rods. However, present detectors are based on conventional phosphors (typically microcrystalline ZnS:Cu) that have intrinsic drawbacks, including light scattering, γ-ray sensitivity, and afterglow. Fast neutron imaging with colloidal nanocrystals (NCs) was demonstrated to eliminate light scattering. While lead halide perovskite (LHP) FAPbBr₃ NCs emitting brightly showed poor spatial resolution due to reabsorption, the Mn²⁺-doped CsPb(BrCl)₃ NCs with oleyl ligands had higher resolution because of large apparent Stokes shift but insufficient concentration for high light yield. In this work, we demonstrate a NC scintillator that features simultaneously high quantum yields, high concentrations, and a large apparent Stokes shift. In particular, we use long-chain zwitterionic ligand capping in the synthesis of Mn²⁺-doped CsPb(BrCl)₃ NCs that allows for attaining very high concentrations (>100 mg/mL) of colloids. The emissive behavior of these ASC18-capped NCs was carefully controlled by compositional tuning that permitted us to select for high quantum yields (>50%) coinciding with Mn-dominated emission for minimal self-absorption. These tailored Mn²⁺:CsPb(BrCl)₃ NCs demonstrated over 8 times brighter light yield than their oleyl-capped variants under fast neutron irradiation, which is competitive with that of near-unity FAPbBr₃ NCs, while essentially eliminating self-absorption. Because of their rare combination of concentrations above 100 mg/mL and high quantum yields, along with minimal self-absorption for good spatial resolution, Mn²⁺:CsPb(BrCl)₃ NCs have the potential to displace ZnS:Cu as the leading scintillator for fast neutron imaging.

中文翻译：

高浓度、两性离子配体封端的 Mn2+:CsPb(BrxCl1–x)3 纳米晶体作为快速中子成像的明亮闪烁体

快中子成像是一种用于大型物体（如核燃料棒）的无损技术。然而，目前的探测器基于传统的磷光体（通常是微晶 ZnS:Cu），这些磷光体具有固有的缺陷，包括光散射、γ 射线敏感性和余辉。使用胶体纳米晶体 (NCs) 进行的快速中子成像被证明可以消除光散射。虽然卤化铅钙钛矿 (LHP) FAPbBr ₃ NCs 由于重吸收而显示出较差的空间分辨率，但 Mn ²⁺掺杂的 CsPb(BrCl) ₃具有油基配体的 NC 具有更高的分辨率，因为明显的斯托克斯位移大，但浓度不足以获得高光产率。在这项工作中，我们展示了一种 NC 闪烁体，它同时具有高量子产率、高浓度和大的明显斯托克斯位移。特别是，我们在合成 Mn ²⁺掺杂的 CsPb(BrCl) ₃ NC 时使用长链两性离子配体封端，从而获得非常高浓度 (>100 mg/mL) 的胶体。这些 ASC18 封端的 NCs 的发射行为是通过成分调整仔细控制的，这使我们能够选择高量子产率 (>50%) 与 Mn 主导的发射相吻合，以实现最小的自吸收。这些定制的 Mn ²⁺ :CsPb(BrCl) ₃在快速中子照射下，NCs 显示出比其油基封端的变体高 8 倍以上的光输出，这与接近统一的 FAPbBr ₃ NCs具有竞争力，同时基本上消除了自吸收。由于 Mn ²⁺ :CsPb(BrCl) ₃ NCs罕见地结合了超过 100 mg/mL 的浓度和高量子产率，以及最小的自吸收以获得良好的空间分辨率，因此有可能取代 ZnS:Cu 作为主要闪烁体用于快速中子成像。

更新日期：2021-12-10

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