Proceedings of Online school on Fundamentals of Semiconductive Quantum Dots (QDsSCHOOL)
DOI: https://doi.org/10.29363/nanoge.qdsschool.2021.004
Publication date: 30th April 2021
Semiconductor nanomaterials such as zero-dimensional quantum dots and two-dimensional quantum well-like nanoplatelets can be produced colloidally on large scale with precise control over ensemble optical properties. Quantum confinement in such systems offers size-tunable energy gap, strong photoluminescence, and, in some cases desirable properties such as optical gain and lasing. The role of thermal energy deposition and dissipation in these nanoscopic structures can impact including radiative rate and material stability, but has not been substantively probed. We have pursued ultrafast optical pump, X-ray diffraction probe experiments as well as optical studies on nanoparticle dispersions as functions of particle size, polytype, and pump intensity to examine lattice response. Shifts of diffraction peaks relate lattice heating and peak amplitude reduction conveys transient lattice disordering (or melting). Intraband and Auger-derived heating is clearly observed in lattice dynamics, and disordering is observed upon absorption of larger numbers of photons excitations per NC on average. Diffraction intensity recovery kinetics, attributable to recrystallization, occur over hundreds of picoseconds with slower recoveries for larger particles. Solid-solid phase transitions can also become apparent with disappearance/appearance of particular diffraction peaks.[1] Transient optical studies using mid-infrared pump photons can monitor thermalization timescales via vibrational excitation of ligands followed by heating of the inorganic core, thus revealing information regarding the inorganic-organic interface. These methods and findings suggest means to probe nanomaterial physical response, stability and transient electronic structure applications such as lasing and solid-state lighting.
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