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 th
e cooling rate of hot carriers in the material. To verify 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 $0.35 pm 0.03$ eV excess energy above the ${Delta}_1$ conduction band minimum. The nanoparticles have nominal 100 nm diameters with crystalline grain sized 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 ($2$ x $10^{19} cm^{-3}$ for the nanoparticles and $6$ x $10^{19} cm^{-3}$ for the thin film). The measured carrier-phonon and phonon-phonon scattering lifetimes for the polycrystalline nanoparticles are $870 pm 40$ fs and $17.5 pm 0.3$ ps, respectively, versus $195 pm 20$ fs and $8.1 pm 0.2$ ps, respectively, for the silicon thin film. The reduced scattering rates observed in the nanoparticles are consistent with the phonon bottleneck hypothesis.
Direct measurements of photoexcited carrier dynamics in nickel are made using few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy at the nickel M$_{2,3}$ edge. It is observed that the core-level absorption lineshape of photoex
cited nickel can be described by a Gaussian broadening ($sigma$) and a red shift ($omega_{s}$) of the ground state absorption spectrum. Theory predicts, and the experimental results verify that after initial rapid carrier thermalization, the electron temperature increase ($Delta T$) is linearly proportional to the Gaussian broadening factor $sigma$, providing quantitative real-time tracking of the relaxation of the electron temperature. Measurements reveal an electron cooling time for 50 nm thick polycrystalline nickel films of 640$pm$80 fs. With hot thermalized carriers, the spectral red shift exhibits a power-law relationship with the change in electron temperature of $omega_{s}proptoDelta T^{1.5}$. Rapid electron thermalization via carrier-carrier scattering accompanies and follows the nominal 4 fs photoexcitation pulse until the carriers reach a quasi-thermal equilibrium. Entwined with a <6 fs instrument response function, carrier thermalization times ranging from 34 fs to 13 fs are estimated from experimental data acquired at different pump fluences and it is observed that the electron thermalization time decreases with increasing pump fluence. The study provides an initial example of measuring electron temperature and thermalization in metals in real time with XUV light, and it lays a foundation for further investigation of photoinduced phase transitions and carrier transport in metals with core-level absorption spectroscopy.
Small polaron formation limits the mobility and lifetimes of photoexcited carriers in metal oxides. As the ligand field strength increases, the carrier mobility decreases, but the effect on the photoexcited small polaron formation is still unknown. E
xtreme ultraviolet transient absorption spectroscopy is employed to measure small polaron formation rates and probabilities in goethite ({alpha}-FeOOH) crystalline nanorods at pump photon energies from 2.2 to 3.1 eV. The measured polaron formation time increases with excitation photon energy from 70 {pm} 10 fs at 2.2 eV to 350 {pm} 30 fs at 2.6 eV, whereas the polaron formation probability (85 {pm} 10%) remains constant. By comparison to hematite ({alpha}-Fe2O3), an oxide analog, the role of ligand composition and metal center density in small polaron formation time is discussed. This work suggests that incorporating small changes in ligands and crystal structure could enable the control of photoexcited small polaron formation in metal oxides.
We propose the use of a silicon-core optical fiber for terahertz (THz) waveguide applications. Finite-difference time-domain simulations have been performed based on a cylindrical waveguide with a silicon core and silica cladding. High-resistivity si
licon has a flat dispersion over a 0.1 - 3 THz range, making it viable for propagation of tunable narrowband CW THz and possibly broadband picosecond pules of THz radiation. Simulations show the propagation dynamics and the integrated intensity, from which transverse mode profiles and absorption lengths are extraced. It is found that for 140 - 250 micron core diameters the mode is primarily confined to the core, such that the overall absorbance is only slightly less than in bulk polycrystalline silicon.
