Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.275
Publication date: 16th December 2024
The ability to control the emission of individual nanocrystals through external electric fields has garnered significant interest in the field of quantum technology. Among the most promising materials for quantum emitters are colloidal lead halide perovskite nanocrystals due to near unity quantum yields and their flexibility in size, shape, and composition engineering. An external electric field induces the quantum-confined Stark Effect (QCSE), which is expected to result in a reduced overlap of the electron and hole wavefunction and an energy shift of the bandgap. This allows to extract polarizability and permanent dipole moment, the latter affecting, e.g., the Rashba effect in lead halide perovskite nanocrystals. Moreover, the field-induced tuning of the excitonic fine structure[1] in single nanocrystals may pave the path for single or entangled photon emitters.
Here, we present an approach of polarization-resolved photoluminescence (PL) spectroscopy on highly anisotropic, single CsPbBr3 nanorods (NRs) for exploring the QCSE under a well-defined angle between crystal axes and electric field[2]. A polarizability of 23 meV/(MV/cm)2 and a permanent dipole of 6.4*10-30 Cm could be extracted, e.g., for a single CsPbBr3 NR aligned at 65° relative to an applied electric field of up to ± 333 kV/cm. We observe a clear correlation between energy shift, spectral line width, and PL intensity under the influence of the QCSE. A detailed analysis on a statistically relevant number of NRs revealed an interesting correlation between PL intensity and polarizability: The higher the PL intensity, the lower the polarizability. Comparing aged NRs with low PL intensities with freshly synthesized ones shows that 44% of the aged NRs reveal a polarizability larger than our error bar (i.e., > 3 meV/(MV/cm)2, whereas only 7% of the fresh NRs show a similar finding. Our work thus highlights new insights and challenges in terms of modulating single lead halide perovskite nanocrystals in directional electric fields.
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