Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400085, India.
Homi Bhabha National Institute, Anushaktinagar, Mumbai 400094, India.
ACS Appl Mater Interfaces. 2021 Jan 20;13(2):3481-3490. doi: 10.1021/acsami.0c21099. Epub 2020 Dec 21.
Nanocrystals having single-band red emission under near-infrared (NIR) excitation through the upconversion process offer great advantages in terms of enhanced cellular imaging in and experiments in the biological window (600-900 nm), as a security ink, in photothermal therapy (PTT), in photodynamic therapy (PDT), and so forth but are challenging for materials scientists. In this work, we report for the first time the preparation of a super bright red emitter at 655 nm from monodispersed NaErF:0.5%Tm@NaYF:20%Yb nanocrystals (core@active shell). This phosphor exhibits 35 times stronger photoluminescence as compared to NaErF:0.5%Tm@NaYF (core@inactive shell). Here, an Er-enriched host matrix works simultaneously as an activator and a sensitizer under NIR excitation. Upconversion red emission at 655 nm arises due to the electronic transition of Er via the involvement of a three-photon absorption (expected to be a two-photon absorption), which has been confirmed via a power-dependent luminescence study. Tm ions incorporated into the core with the active shell act as trapping centers, which promote the red band emission via the back-energy transfer process. Moreover, the active shell containing Yb ions efficiently transfers the energy to the Er-enriched core, which suppresses the nonradiative channel rate, and Tm ions act as trapping centers, which reduce the luminescence quenching via reduction of energy migration to the surface of the host lattice. Also, we have shown the potential applications of these nanocrystals: cellular imaging through downconversion and upconversion processes and security ink.
通过上转换过程在近红外 (NIR) 激发下具有单带红光发射的纳米晶体在增强细胞成像方面具有很大的优势,在生物窗口(600-900nm)中进行 和 实验、作为安全油墨、光热疗法 (PTT)、光动力疗法 (PDT) 等,但对材料科学家来说具有挑战性。在这项工作中,我们首次报道了由单分散 NaErF:0.5%Tm@NaYF:20%Yb 纳米晶体(核@活性壳)制备超亮红色发射器 655nm 的情况。与 NaErF:0.5%Tm@NaYF(核@非活性壳)相比,这种荧光粉的光致发光强度要强 35 倍。在这里,富 Er 主体基质在 NIR 激发下同时作为激活剂和敏化剂。655nm 的上转换红光发射归因于 Er 的电子跃迁,涉及三光子吸收(预计为双光子吸收),这已通过依赖于功率的发光研究得到证实。掺入具有活性壳的核中的Tm 离子作为捕获中心,通过反向能量转移过程促进红光带发射。此外,含有 Yb 离子的活性壳有效地将能量转移到富 Er 的核中,这抑制了非辐射通道速率,并且 Tm 离子作为捕获中心,通过减少能量向宿主晶格表面的迁移来减少发光猝灭。此外,我们展示了这些纳米晶体的潜在应用:通过下转换和上转换过程进行细胞成像和安全油墨。