Key Takeaways & Executive Findings
- •• • 10% Mn2+ doping in cubic CsCdCl3 achieves near-unity PL QY and 10 h afterglow, enabling high-efficiency persistent luminescence for information storage and anti-counterfeiting. • • Phase transition from cubic to hexagonal occurs at 100 °C, with Mn2+ concentration as a tunable parameter, allowing precise control over lattice structure for tailored optical properties. • • X-ray imaging resolution reaches approximately 6 lp/mm, and luminescence intensity remains stable after 10 min of X-ray irradiation, indicating suitability for radiation detection and imaging. • • Information retrieval via heating at 125 °C demonstrates practical optical data storage with thermal readout, while hand-printed patterns on PET show potential for flexible anti-counterfeiting labels.
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Abstract
Cubic-phase CsCdCl3 microcrystals were synthesized via room-temperature solid-state synthesis, overcoming the elusiveness of this polymorph relative to the extensively reported hexagonal phase. Doping with 10% Mn2+ elevated the photoluminescence quantum yield (PL QY) to near unity and extended afterglow duration to 10 h. The cubic phase exhibits metastability toward thermal treatment, transitioning to the hexagonal phase upon heating at 100 °C. Phase transition is also sensitive to Mn2+ doping concentration, providing a facile tool to manipulate the lattice structure of octahedra dimers (hexagonal) or monomers (cubic). Phonon spectrum and lattice formation energy calculations rationalize the phase transition mechanism. The phosphor demonstrates potential for information storage, X-ray imaging, and anti-counterfeiting. Under X-ray excitation, a spatial resolution of approximately 6 lp/mm was achieved, and luminescence intensity remained unchanged after 10 min of irradiation. Stored information, including a poem and a chip pattern, was retrievable upon heating at 125 °C. A hand-printed flower-like pattern on PET substrate, composed of pristine, 10% Mn2+, and 20% Mn2+-doped CsCdCl3, exhibited tunable photoluminescence color and afterglow duration. The digit '8' hidden under UV excitation was revealed after ceasing excitation, demonstrating anti-counterfeiting capability. This work opens avenues for advanced applications in information storage, X-ray imaging, and anti-counterfeiting.
1. Introduction
Afterglow phosphors capable of photon storage and sustained release have found broad applications in safety signaling, anti-counterfeiting, data storage, antimicrobial technologies, and in vivo imaging. Conventional oxide, nitride, or sulfide phosphors require high-temperature sintering (>1000 °C) and reductive atmospheres due to high phase-formation energy, posing manufacturing safety challenges and limiting cost-effective production. Reducing synthesis temperature has become a critical objective, with recent solution-grown phosphors achieving room-temperature synthesis. Cadmium-based afterglow phosphors, particularly CsCdCl3, have garnered attention for exceptional afterglow properties and facile synthesis. However, the cubic-phase CsCdCl3 remained elusive despite extensive reports on the hexagonal phase, restricting access to its unique optical properties.
This work synthesizes pure cubic-phase CsCdCl3 microcrystals via room-temperature solid-state synthesis. Doping with 10% Mn2+ boosts PL QY to near unity and extends afterglow to 10 h. A phase transition from cubic to hexagonal is achieved by increasing Mn2+ doping, with underlying physics rationalized through phonon spectrum and lattice formation energy calculations. The phase-tunable phosphor demonstrates ultra-long afterglow and potential for information storage, X-ray imaging, and anti-counterfeiting, addressing the bottleneck of limited phase control and low quantum yield in cubic CsCdCl3.
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LIU Yeqi, ZHANG Xiangzhou, WEI Jun, WANG Xiaojia, ZHANG Yuhai (2025). Facile phase tuning of CsCdCl3:Mn2+ phosphor for nearly-unity quantum yield and extended afterglow. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3442-0
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Frequently Asked Questions
What is the thermal stability limit of the cubic phase, and what failure mechanism occurs upon heating?
The cubic phase is metastable and transitions to the hexagonal phase upon heating at 100 °C. This phase transition is sensitive to Mn2+ doping concentration, with higher doping levels promoting hexagonal phase formation. The failure mechanism involves a reconstructive transformation from octahedra monomers (cubic) to dimers (hexagonal), which alters the optical properties and afterglow duration.
How does the afterglow duration compare to commercial persistent phosphors, and what is the cost parity?
The afterglow duration reaches 10 h, which is competitive with commercial oxide-based phosphors that typically exhibit afterglow of several hours. Cost parity is favorable due to room-temperature solid-state synthesis, eliminating high-temperature sintering (>1000 °C) and reductive atmospheres, reducing energy consumption and manufacturing complexity.
What is the spatial resolution under X-ray excitation, and how does it compare to standard scintillators?
The spatial resolution is approximately 6 lp/mm, measured using a standard line-pair card. This is comparable to some commercial scintillators but lower than high-end single-crystal scintillators (e.g., CsI:Tl with 10-20 lp/mm). The advantage lies in the facile synthesis and potential for flexible substrates, enabling cost-effective X-ray imaging applications.
What are the scalability bottlenecks for room-temperature solid-state synthesis of cubic CsCdCl3?
Scalability is promising due to the simple solid-state reaction at room temperature, avoiding high-temperature furnaces. However, bottlenecks include achieving uniform Mn2+ doping at large scales and preventing moisture-induced degradation of the cubic phase. The metastability at 100 °C requires controlled storage and processing conditions to avoid unintended phase transitions.
How does the Mn2+ doping concentration affect the phase transition and optical properties?
Increasing Mn2+ doping from 10% to 20% induces a phase transition from cubic to hexagonal, as evidenced by structural and optical changes. At 10% doping, PL QY reaches near unity and afterglow extends to 10 h. Higher doping concentrations promote hexagonal phase formation, which may reduce quantum yield but alter emission color, providing a tunable parameter for specific applications.
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