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Characterization of Carrier Cooling Bottleneck in Silicon Nanoparticles by Extreme Ultraviolet (XUV) Transient Absorption Spectroscopy

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journal contribution
posted on 23.04.2021, 08:13 by Ilana J. Porter, Angela Lee, Scott K. Cushing, Hung-Tzu Chang, Justin C. Ondry, A. Paul Alivisatos, Stephen R. Leone
Silicon nanoparticles have the promise to surpass the theoretical efficiency limit of single-junction silicon photovoltaics by the creation of a “phonon bottleneck,” a theorized slowing of the cooling rate of hot optical phonons that in turn reduces the cooling rate of hot carriers in the material. Verifying the presence of a phonon bottleneck in silicon nanoparticles requires simultaneous resolution of electronic and structural changes at short timescales. Here, extreme ultraviolet transient absorption spectroscopy is used to observe the excited-state electronic and lattice dynamics in polycrystalline silicon nanoparticles following 800 nm photoexcitation, which excites carriers with 0.35 ± 0.03 eV excess energy above the Δ1 conduction band minimum. The nanoparticles have nominal 100 nm diameters with crystalline grain sizes of about ∼16 nm. The extracted carrier–phonon and phonon–phonon relaxation times of the nanoparticles are compared to those for a silicon (100) single-crystal thin film at similar carrier densities (2 × 1019 cm–3 for the nanoparticles and 6 × 1019 cm–3 for the film). The measured carrier–phonon and phonon–phonon scattering lifetimes for the polycrystalline nanoparticles are 870 ± 40 fs and 17.5 ± 0.3 ps, respectively, versus 195 ± 20 fs and 8.1 ± 0.2 ps, respectively, for the silicon thin film. The reduced scattering rates observed in the nanoparticles are consistent with the phonon bottleneck hypothesis.