Achieving High Quantum Efficiency in Mn5+ Activated Phosphors for NIR‐II Deep Bioimaging Application

Author:

Zhang Quan12ORCID,Yang Zetian3ORCID,Zhou Xinquan24,Delaey Maxime2ORCID,Wang Mingyuan1,Fu Ruining1,Lei Shuangying1,Vrielinck Henk5ORCID,Poelman Dirk2

Affiliation:

1. Key Laboratory of MEMS of Ministry of Education, School of Integrated Circuits Southeast University Nanjing 210096 China

2. LumiLab, Department of Solid State, Sciences Ghent University Krijgslaan 281‐S1 Ghent B‐9000 Belgium

3. Aviation Engineering School Air Force Engineering University Xi'an 710038 China

4. Key Laboratory of Luminescent Materials and School of Materials Science and Engineering South China University of Technology Guangzhou 510641 China

5. Defects in Semiconductors Research Group Department of Solid State Sciences Ghent University Krijgslaan, 281‐S1 Ghent B‐9000 Belgium

Abstract

AbstractMn5+ emission is a promising candidate for imaging deep tissue structures (e.g., vessels, tumors) in the second near‐infrared (NIR‐II, 1000–1350 nm) region. However, its practical application is impeded by the limited quantum efficiency of the available phosphors due to the unstable valence state of Mn5+. Herein, a novel strategy involving site competition is proposed to stabilize the Mn5+ state by the introduction of valence‐unstable Bi2+/3+. The results demonstrate that Bi3+ ions tend to occupy two different Ca2+ ion sites within the Ca6Ba(PO4)4O lattice. The incorporation of a small amount of Bi3+ effectively suppresses the amount of Mn2+ in Ca2+ sites. This is also confirmed by spectroscopic experiments and density function theory calculations. Notably, an ultra‐high internal quantum efficiency of 82.3% is achieved under excitation at 653 nm, surpassing more than twofold the previously reported value of 37.5% in Ca6Ba(PO4)4O: Mn5+. As a proof of concept, deep tissue imaging with a penetration depth of ≈2.8 cm is achieved using a self‐produced NIR‐II light‐emitting diodes device embedded with Ca6Ba(PO4)4O: 0.003Mn5+/0.003Bi3+ powder. These findings provide valuable insights into improving the luminescent properties associated with Mn5+ ions and pave the way for deep tissue imaging with high spatiotemporal resolution.

Funder

Fonds Wetenschappelijk Onderzoek

Publisher

Wiley

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