揭示基于 LiErF4 的上转换纳米颗粒中 Er3+ 的激发态动力学

基础金属	铜电解铜铜精矿铜管铜棒废铜铜排铜合金精铜杆再生铜杆铜板带铝铝土矿氧化铝电解铝铝辅料铝棒铝合金锭废铝铝杆铝型材铝板卷铅铅精矿铅锭铅蓄电池再生精铅还原铅废铅蓄电池铅合金锌锌精矿电解锌锌合金氧化锌锌粉锡锡精矿锡锭锡材镁
稀有金属	稀土稀土矿稀土氧化物稀土金属钕铁硼稀散金属锑铋铟锗镓硒钽锆贵金属白银钨钨精矿 APT(仲钨酸铵)钨粉碳化钨钨酸钠钨条钨铁钨材钼钼精矿工业氧化钼钼铁钼化工高纯三氧化钼钼金属钛钛精矿钛渣四氯化钛海绵钛钛金属钛白粉硒
新能源	锂锂矿锂化合物金属锂镍镍矿镍铁精炼镍镍盐高冰镍 MHP 钴电解钴钴粉氯化钴四氧化三钴硫酸钴钴中间品氧化钴碳酸钴钴酸锂锰锰矿电解锰电池级硫酸锰锂电正负极三元前驱体磷酸铁正极材料石油焦针状焦包覆沥青人造石墨硅碳负极硅氧负极硅

基础金属

铜电解铜铜精矿铜管铜棒废铜铜排铜合金精铜杆再生铜杆铜板带铝铝土矿氧化铝电解铝铝辅料铝棒铝合金锭废铝铝杆铝型材铝板卷铅铅精矿铅锭铅蓄电池再生精铅还原铅废铅蓄电池铅合金锌锌精矿电解锌锌合金氧化锌锌粉锡锡精矿锡锭锡材镁

稀有金属

稀土稀土矿稀土氧化物稀土金属钕铁硼 稀散金属锑铋铟锗镓硒钽锆 贵金属白银钨钨精矿 APT(仲钨酸铵)钨粉碳化钨钨酸钠钨条钨铁钨材钼钼精矿工业氧化钼钼铁钼化工高纯三氧化钼钼金属钛钛精矿钛渣四氯化钛海绵钛钛金属钛白粉硒

新能源

锂锂矿锂化合物金属锂镍镍矿镍铁精炼镍镍盐高冰镍 MHP 钴电解钴钴粉氯化钴四氧化三钴硫酸钴钴中间品氧化钴碳酸钴钴酸锂锰锰矿电解锰电池级硫酸锰 锂电正负极三元前驱体磷酸铁正极材料石油焦针状焦包覆沥青人造石墨硅碳负极硅氧负极硅

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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