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福建物構所釹摻雜LiLuF4近紅外納米發光材料電子結構研究獲進展

文章來源:福建物質結構研究所   發布時間:2019-03-22  【字號:     】  

  稀土摻雜近紅外納米發光材料由于深層生物組織穿透、無背景熒光干擾和對生物樣本損傷小等特點在生物成像和溫度傳感等領域具有重要的應用前景。Nd3+離子在介質材料中的光學性能主要取決于其局域態的電子結構和激發態動力學,對Nd3+基納米發光材料開展深入的光物理研究對其光學性能的優化及其在生物醫學領域的應用至關重要。然而,由于晶格內部和表面缺陷等影響,Nd3+離子在納米材料中通常存在多格位發光,導致其晶體場躍遷發射譜線復雜、難以區分。目前,在納米發光材料中揭示Nd3+離子發光中心的局域電子結構仍是該領域的一個技術挑戰。

  中國科學院福建物質結構研究所功能納米結構與組裝重點實驗室陳學元團隊在中科院戰略性先導科技專項、創新國際團隊以及鄭偉和黃萍主持的國家自然科學基金面上基金、中科院青促會、海西研究院“春苗”人才專項等支持下,首次在LiLuF4納米晶中揭示了Nd3+離子的局域電子能級結構。該團隊以Eu3+為結構探針,利用低溫高分辨光譜、時間分辨光譜和位置選擇光譜等先進的測試手段,揭示了稀土離子在LiLuF4納米晶中存在單一的光譜學S4位置對稱性,與其結晶學位置對稱性一致。通過Nd3+的低溫高分辨光譜和變溫光譜等測試手段,精確指認出36條源自Nd3+4F3/24IJJ = 9/2, 11/2, 13/2)晶體場躍遷的發射譜線,并確定了Nd3+4F3/24IJ組態的全部Stark子能級位置。進一步地,該團隊利用指認出的4F3/2兩個Stark子能級的躍遷強度與溫度的不同依賴關系,將LiLuF4:Nd3+納米晶作為近紅外納米熒光探針用于77-275 K低溫區間的高靈敏溫度探測,其最高相對靈敏度達到0.62% K-1,與此前報道的Nd3+摻雜納米熒光溫度計的最高值相當。該研究對發展高效Nd3+基近紅外納米熒光探針提供了理論基礎,也為稀土納米熒光探針在低溫探測領域的新應用指明了方向。相關結果314日在線發表于《先進科學》(Adv. Sci. 2019, 1802282. DOI: 10.1002/advs.201802282)。

  此前,陳學元團隊在稀土摻雜納米發光材料的發光物理和應用研究方面取得一系列進展。例如,發展高效LiLuF4:Yb,Er多層核殼結構上轉換納米晶,實現對腫瘤標志物β-hCG的高靈敏特異性檢測和腫瘤細胞的靶向熒光成像(Angew. Chem. Int. Ed. 2014, 53, 1252-1257; Sci. China Mater. 2015, 58, 156-177; Mater. Today Nano 2019, 5, 100031);設計合成NaCeF4:Er近紅外二區納米熒光探針,實現對人體血清中尿酸的高靈敏檢測及對小鼠深層組織高分辨成像(Chem. Sci. 2018, 9, 4682-4688

1. 基于LiLuF4:Nd3+近紅外納米熒光探針的溫度傳感

2. LiLuF4:Nd3+近紅外納米發光材料局域電子能級結構




(責任編輯:葉瑞優)

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