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揭示基于 LiErF4 的上转换纳米颗粒中 Er3+ 的激发态动力学

2025-05-28 17:25:06 来源：上海稀土协会责任编辑：管理员

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镧系元素（Ln3+）掺杂的上转换纳米粒子（UCNP）由于能够将低能近红外（NIR）光子转换为高能紫外光子和可见光子，因此在各种纳米光子和生物医学应用中受到了相当大的关注。传统的 UCNP 通常由 Ln3+掺杂水平低的惰性主体材料组成活化剂（例如，2 mol % Er3+和 0.5 mol % Tm3+）和敏化剂（例如，20 mol % Yb3+）以避免有害的浓度淬灭效应，然而，它受到少量 Ln3+的限制发射器、低上转换（UC）效率以及亮度不足，尤其是在单粒子级别。为了对抗浓度淬灭效应，策略包括表面钝化、表面重建 /晶格调制 /Ln3+的空间限制排放和染料致敏已经开发出来，产生了许多具有高浓度 Ln3+的高效 UCNP掺杂。具体来说，Ln3+由于大量的 Ln 与低掺杂 UCNP 相比，在高密度激发下，重掺杂 UCNP 已被证明可提供更高的 UC 效率和亮度3+可以收集和维持高功率激发能量的离子。此外，基于 Ln3+可以实现新的光学特性，例如高度非线性光子雪崩和上转换超荧光重度掺杂 UCNP。这些特性使 Ln3+重掺杂 UCNP 在许多前沿领域的应用很有吸引力，例如超分辨率成像、单分子跟踪和量子光学。

提高 UC 效率并释放 Ln3+ 的潜力重掺杂 UCNPs，对光物理学的基本理解，尤其是浓度猝灭机制至关重要。交叉弛豫（CR）和能量迁移（EM）被认为是 Ln3+ 中的两个主要猝灭途径重度掺杂的 UCNP。例如，Almutairi 等人证明 Er3+中的浓度淬灭富集 NaErF4UCNP 起源于能量迁移介导的通过 Er3+ 的耗散亚晶格到表面缺陷或高能振动基团。这种不利影响可以通过表面钝化得到有效缓解，从而在 980 nm 激发下以 10 W cm 的功率密度产生约 5.2% 的显着 UC 量子产率–2。Liu 和 Wang 等人证实，迁移介导的能量耗散到内部晶格缺陷在NaErF4@NaYF4，可以通过引入诱捕中心（例如 Tm3+）来限制激发能量。相反，Zhang 和 Chang 等人认为相邻 Er3+ 之间的 CR而不是长距离 EM 是 NaErF 中的主要淬火机制4@NaYF4CS UCNPs，而在低温（40 K）下抑制 CR 导致 UC 发光（UCL）增强超过 2 个数量级。这些未解决的争议凸显了 Ln3+ 中能量耗散路径的复杂性大量掺杂的 UCNP，突出了在这个不断发展的领域中需要系统调查的关键知识差距。具体来说，是 Ln3+ 的瞬态衰变动力学尽管它在阐明浓度淬灭现象方面至关重要，但与能量转移（ET）和 EM 相关的仍然难以捉摸，而且在很大程度上尚未得到探索。

在本文中，我们对 Er3+ 中的浓度猝灭效应进行了全面调查富含 LiErF4和 LiYF4@LiErF4@LiYF4（表示为 Y@100Er@Y）核心-外壳-外壳（CSS） UCNP，其中 Er3+离子在空间上被限制在中间层内。Er3+的瞬态衰变动力学和 Tm3+ 的效果通过温度依赖性光谱法对掺杂进行详细研究。据了解，Er3+由于 Er 的空间限制，离子在 Y@100Er@Y 中经历了扩散受限的 EM3+ 过程，而 Tm3+离子作为能量捕获中心可以有效抑制 Er 的长距离 EM3+并大大改善了 UCL 性能。

我们研究了 CSS UCNP 的夹心结构Y@100Er@Y，因为有充分的证据表明，夹层 CSS UCNP 的 UC 效率比普通 CS UCNP 高得多。为了调节 EM 过程并进一步增强 UCL，微量的 Tm3+将（0.2、0.5 和 1.0 mol%）掺杂，产生 LiYF4@LiErF4： x%Tm3+@LiYF4（表示为 Y@Er/xTm@Y）CSS UCNP 的正如我们之前报道的那样，Y@100Er@Y 和 Y@Er/xTm@Y CSS UCNP 是通过热分解方法合成的。图像显示，合成的 UCNPs 具有明确的菱形形态，LiYF 的平均尺寸从（49.9 × 35.1） nm 增加到4LiYF 为（77.1 × 42.3） nm4@LiErF4壳生长时Y@100Er@Y（表示为 Y@100Er）和（82.3 × 47.6） nm，揭示了夹层和外层的壳厚度分别为 ∼ 13.6 nm 和 ∼ 2.6 nm。高分辨率 TEM （HRTEM）图像显示清晰的晶格条纹，在四方 LiYF 的（101）平面上观察到的 d 间距为 0.46 nm4，表明所得 UCNP 的结晶度和相纯度很高，其强烈且索引良好的衍射峰到四方 LiYF 也证实了这一点4（JCPDS 第 77-0816 号）（图 S2）。通过高角度环形暗场扫描 TEM （HAADF-STEM）图像和能量色散 X 射线（EDX）元素映射鉴定了 UCNP 的多层 CSS 结构，分别显示出原子序数（Z）对比度的显着差异以及 Y 和 Er 在不同层中的均匀分布。微量的 Tm3+（0.2、0.5 和 1.0 mol %）掺杂对所得 UCNP 的结晶相和形态没有明显影响，表明合成具有良好的重现性。

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揭示基于 LiErF4 的上转换纳米颗粒中 Er3+ 的激发态动力学

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