Hans Kraus

Abstract:

Metal-halide perovskite semiconductors have attracted intensive interest in the last decade, particularly for applications in photovoltaics. Low-energy optical phonons combined with significant crystal anharmonicity play an important role in charge-carrier cooling and scattering in these materials, strongly affecting their optoelectronic properties. We have observed optical phonons associated with Pb—I stretching in both MAPbI3 single crystals and polycrystalline thin films as a function of temperature by measuring their terahertz (THz) conductivity spectra with and without photoexcitation. An anomalous bond hardening was observed under above-bandgap illumination for both single-crystal and polycrystalline MAPbI3. First-principles calculations reproduced this photo-induced bond hardening and identified a related lattice contraction (photostriction), with the mechanism revealed as Pauli blocking. For single-crystal MAPbI3, phonon lifetimes were significantly longer and phonon frequencies shifted less with temperature, compared with polycrystalline MAPbI3. We attribute these differences to increased crystalline disorder, associated with grain boundaries and strain in the polycrystalline MAPbI3. Thus we provide fundamental insight into the photoexcitation and electron–phonon coupling in MAPbI3.

Abstract:

Applications that utilize scintillation detectors at low temperatures are growing in number. Many of these require materials with high light yield and a fast response. Here we report on the low-temperature characterisation of ZnSe doped with Al or Te, respectively. The X-ray luminescence and decay curves were measured over the 77–295 K temperature range, and alpha particle excitation was used to examine scintillation light output and decay kinetics over the range 9–295 K. A significant improvement of the scintillation characteristics was observed at cooling below 100 K. The scintillation light yield of the crystals increases by a factor about two, and the decay time constant decreases by almost an order of magnitude to 0.3–0.4 μs. These improvements enhance the potential of ZnSe-based crystals for application in cryogenic scintillation detectors of ionising radiation.