CsSrI3/Eu2+ has very promising scintillation
properties for gamma-ray spectroscopy applications, but it has proven
difficult to grow high quality single crystals in large sizes. This
paper reports a composition-engineering strategy, in this case a combination
of off-stoichiometric melts and Eu2+ concentration optimization,
to obtain large-size CsSrI3/Eu2+ crystals with
excellent energy resolution. Crystals of a series of off-stoichiometric
compositions, Cs(1+x)(Sr,Eu)(1–x)I(3–x) (x = 0, 0.05, 0.06, and 0.1), were grown by the Bridgman
method. The Cs1.06Sr0.94I2.94/Eu2+ single crystal has the highest optical transmittance between
450 and 800 nm. Cs1.06Sr0.94I2.94 single crystals doped with 0.5, 1, 3, 5, and 7 mol % Eu2+ ions were also grown by the Bridgman method. The effects of Eu2+ concentration on the phase purity and optical and scintillation
properties were studied. X-ray diffraction patterns confirmed the
phase purity of all samples with the exception of a hydrate phase
formed during measurement. Increasing Eu2+ concentration
leads to longer decay components due to the effect of self-absorption.
An unexpected relationship was found between the Eu2+ concentration
and the appearance of two photopeaks in a pulse height spectrum acquired
under a single gamma-ray energy of 662 keV irradiation. The origins
of this phenomenon are proposed from experimental insights. The optimal
composition we developed achieved an excellent energy resolution of
3.4% for ϕ22 mm × 2 mm, 3.9% for ϕ22 mm × 15
mm, and 4.1% for ϕ22 mm × 19 mm at 662 keV. The results
of this paper lead to a better understanding of the effects of composition-engineering
in optimization of nonstoichiometric scintillator compounds.