Melt-Processable and Thermally Driven Self-Healing Luminescent Cu(I) Hybrid Metal Halides

Abstract

Despite the fascinating optical and electronic properties of emerging Cu(I) halides, their high melting points, irreversible decomposition, and intrinsic instability have hindered optoelectronic applications. Here, we designed novel Cu(I) halides, namely C 12 H 28 NCuCl 2 and C 20 H 48 N 2 Cu 4 Cl 6 , with significantly lower melting points (86 and 122 °C), enabling remarkable moldability. Intriguingly, this investigation demonstrates that the aging and luminescence-quenching phenomena observed in C 12 H 28 NCuCl 2 and C 20 H 48 N 2 Cu 4 Cl 6 crystals resulting from the air oxidation can be effectively reversed through controlled heat treatment. The resulting C 12 H 28 NCuCl 2 and C 20 H 48 N 2 Cu 4 Cl 6 crystals exhibit broadband emission with photoluminescence quantum yields of 74.78% and 46.52%, respectively. Furthermore, C 12 H 28 NCuCl 2 displays bright radioluminescence, showing an internal X-ray to light conversion efficiency of 36 506 photons/MeV under steady state X-ray illumination. The inherent melt processability of these materials empowers their transformation into diverse shapes suitable for practical applications. Herein, a sizable C 12 H 28 NCuCl 2 scintillator screen (∼10 cm × 7 cm) was successfully prepared through a melt-processing method, achieving X-ray imaging resolution of 9 line pairs per millimeter (9 lp/mm). This study demonstrates the potential of melt-processable Cu(I) halides to be applied in various applications, because of their unique properties, including facile processing, moldability, and high X-ray luminescence.

Amplified Circularly Polarized and X-ray-Excited Luminescence of Easily Separated Chiral Donor–Acceptor Binaphthalene Imides through a Conformation Locking Strategy

“…The successful activation of CPL properties by conformation locking encouraged us to explore another emerging function, i.e., X-ray excited luminescence, − which remains challenging for organic scintillators in terms of detection limit, scintillation lifetime, and photostability. , The XEL properties of (S)-C1 , C2 , C3 , and C6 and (S)-open single crystals were measured under an X-ray source, whose XEL spectra exhibited similar profiles in contrast to their PL spectra (Figures S10 and S11). Compared with (S)-open , all of the locked imides gave stronger XEL intensities, while (S)-C1 showed almost 30-fold amplification.…”

“…(b) Dose rate dependence of the XEL intensity of (S)-C1 in the range of 4.58 to 278 μGy s –1 in air. Detection limit (DL) is calculated using the 3σ/slope method . (c) Photostability of (S)-C1 under X-ray continuous irradiation near 30 min at a dose rate of 278 μGy s –1 in air.…”

“…The X-ray detection limit of (S)-C1 was then calculated to be about 0.25 μGy s −1 in air, which was about 22 times lower than the standard dosage for X-ray diagnostics (5.5 μGy air s −1 ). 41 Apart from the detection limit of the X-ray dosage, photostability is also a critical parameter for X-ray scintillators. The XEL intensity of (S)-C1 remained almost unchanged upon continuous X-ray irradiation near 30 min with a high dose rate of 278 μGy s −1 in air condition, indicating excellent X-ray photostability (Figure 4c).…”

“…The X-ray detection limit of (S)-C1 was then calculated to be about 0.25 μGy s –1 in air, which was about 22 times lower than the standard dosage for X-ray diagnostics (5.5 μGy air s –1 ) . Apart from the detection limit of the X-ray dosage, photostability is also a critical parameter for X-ray scintillators.…”

Enhanced Storage Capacity via Anion Substitution for Advanced Delayed X-ray Detection

“…Delayed X-ray detection is a promising solution to detect X-ray radiation when immediate detection is challenging, such as inspection of complex structures, cumulative dose of X-ray radiation, and monitoring the gradual degradation of nuclear materials. − Delayed X-ray detection utilizes optical information storage materials that can store X-ray energy and provide delayed information readout. − Lanthanide-doped fluoride nanocrystals (NCs) are an ideal storage material for recording X-ray radiation information because the X-ray radiation-induced Frankel defects can act as traps for storing X-ray energy. − Recently, Tb 3+ -activated NaLuF 4 NCs have been found to exhibit intense X-ray-induced afterglow for plate-free X-ray delayed detection by Liu’s group . However, the afterglow release under thermal disturbance at room temperature limits the stability of X-ray information storage; therefore, various functional designs to enhance the trap storage capacity are gradually being studied.…”