The
study and development in recent years of hybrid (organic–inorganic)
halide perovskite materials have given them an unprecedented opportunity
for direct ionizing radiation detection, given their large attenuation
coefficient and sufficient charge carrier mobility lifetime product.
The use of single crystals, considered as model materials, allows
us to investigate their intrinsic properties. Characterizations under
X-ray illumination of detector devices based on methylammonium lead
tribromide (MAPbBr3) single crystals, obtained by optimized
growths, show good sensitivity but high dark current density. To improve
this critical parameter, while using MAPbBr3 as the base
material, we employ anion engineering within the halide elements.
We present here mixed halide perovskite crystals, with bromide partially
replaced with chloride, obtained through optimized growths using modified
inverse temperature crystallization in dimethylformamide, leading
to high-quality single crystals of the general formula MAPb(Br1–x
Cl
x
)3. Six chlorine contents are targeted and carefully determined
experimentally via energy-dispersive X-ray analysis and X-ray powder
diffraction. For each composition, several crystals are synthesized
and used to prepare X-ray detection devices. Their optoelectronic
properties are determined under standard X-ray medical conditions
and hint at the existence of an optimal composition. MAPb(Br0.85Cl0.15)3 exhibits the best sensitivity with
a value of S ≈ 3 μC mGyair
–1 cm–2 for RQA5 spectral quality
and the lowest dark current density with a value of J
dark ≈ 22 nA mm–2, both recorded
at a 50 V mm–1 electric field. This sensitivity
value doubles our own MAPbBr3 single crystal device and
is higher than that of CsI(Tl)- or a-Se-based flat panels. The present
work broadens the benefits and drawbacks of employing halide engineering
in perovskite materials to improve the optoelectronic performance
under high-energy radiation.