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Register a new userSuppression of phonon-mediated hot carrier relaxation in type-II InAs/AlAs$_{x}$Sb$_{1-x}$ quantum wells: a practical route to hot carrier solar cells
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Added by
Vincent R Whiteside
Publication date
2015
fields
Physics
and research's language is
English
Authors
H. Esmaielpour
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InAs/AlAs$_{x}$Sb$_{1-x}$ quantum wells are investigated for their potential as hot carrier solar cells. Continuous wave power and temperature dependent photoluminescence indicate a transition in the dominant hot carrier relaxation process from conventional phonon-mediated carrier relaxation below 90 K to a regime where inhibited radiative recombination dominates the hot carrier relaxation at elevated temperatures. At temperatures below 90 K photoluminescence measurements are consistent with type-I quantum wells that exhibit hole localization associated with alloy/interface fluctuations. At elevated temperatures hole delocalization reveals the true type-II band alignment; where it is observed that inhibited radiative recombination due to the spatial separation of the charge carriers dominates hot carrier relaxation. This decoupling of phonon-mediated relaxation results in robust hot carriers at higher temperatures even at lower excitation powers. These results indicate type-II quantum wells offer potential as practical hot carrier systems.
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A type-II InAs/AlAs$_{0.16}$Sb$_{0.84}$ multiple-quantum well sample is investigated for the photoexcited carrier dynamics as a function of excitation photon energy and lattice temperature. Time-resolved measurements are performed using a near-infrared pump pulse, with photon energies near to and above the band gap, probed with a terahertz probe pulse. The transient terahertz absorption is characterized by a multi-rise, multi-decay function that captures long-lived decay times and a metastable state of for an excess-photon energy of $>100$ meV. For sufficient excess-photon energy, excitation of the metastable state is followed by a transition to the long-lived states. Excitation dependence of the long-lived states map onto a near-direct band gap ($E{_g}$) density of states with an Urbach tail below $E{_g}$. As temperature increases, the long-lived decay times increase $<E{_g}$, due to the increased phonon interaction of the unintentional defect states, and by phonon stabilization of the hot carriers $>E{_g}$. Additionally, Auger (and/or trap-assisted Auger) scattering above the onset of the plateau may also contribute to longer hot-carrier lifetimes. Meanwhile, the initial decay component shows strong dependence on excitation energy and temperature, reflecting the complicated initial transfer of energy between valence-band and defect states, indicating methods to further prolong hot carriers for technological applications.
We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1$T$-VSe$_2$. Ultrafast snapshots of the light-induced hot carrier dynamics and non-equilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. The hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of $(200 pm 40)$~fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasi-equilibrium state that is experimentally observed.
We present a time-resolved optical study of the dynamics of carriers and phonons in Ga_{1-x}Mn_{x}As layers for a series of Mn and hole concentrations. While band filling is the dominant effect in transient optical absorption in low-temperature-grown (LT) GaAs, band gap renormalization effects become important with increasing Mn concentration in Ga_{1-x}Mn_{x}As, as inferred from the sign of the absorption change. We also report direct observation on lattice vibrations in Ga1-xMnxAs layers via reflective electro-optic sampling technique. The data show increasingly fast dephasing of LO phonon oscillations for samples with increasing Mn and hole concentration, which can be understood in term of phonon scattering by the holes.
The relaxation dynamics of hot carriers in silicon (100) is studied via a novel holistic approach based on phase-resolved transient absorption spectroscopy with few-cycle optical pulses. After excitation by a sub-5 fs light pulse, strong electron-phonon coupling leads to an ultrafast momentum relaxation with time constant of 10 fs. The thermalization of the hot carriers occurs on a time constant of 150 fs, visible in the temporal evolution of the collision time as extracted from the Drude model. We find an increase of the collision time from 3 fs for the shortest timescales with a saturation at approximately 18 fs. Moreover, the optical effective mass of the hot carrier ensemble evolves on ultrafast timescales as well, with a bi-exponential decrease from 0.7 $m_e$ to about 0.125 $m_e$ and time constants of 4 fs and 58 fs. The presented information on the electron mass dynamics as well as the momentum-, energy-, and collision-scattering times with unprecedented time resolution is important for all hot carrier optoelectronic devices.
Extraction of non-equilibrium hot carriers generated by plasmon decay in metallic nanostructures is an increasingly exciting prospect for utilizing plasmonic losses, but the search for optimum plasmonic materials with long-lived carriers is ongoing. Transition metal nitrides are an exciting class of new plasmonic materials with superior thermal and mechanical properties compared to conventional noble metals, but their suitability for plasmonic hot carrier applications remains unknown. Here, we present fully first-principles calculations of the plasmonic response, hot carrier generation and subsequent thermalization of all group IV, V and VI transition metal nitrides, fully accounting for direct and phonon-assisted transitions as well as electron-electron and electron-phonon scattering. We find the largest frequency ranges for plasmonic response in ZrN, HfN and WN, between those of gold and silver, while we predict strongest absorption in the visible spectrum for the VN, NbN and TaN. Hot carrier generation is dominated by direct transitions for most of the relevant energy range in all these nitrides, while phonon-assisted processes dominate only below 1 eV plasmon energies primarily for the group IV nitrides. Finally, we predict the maximum hot carrier lifetimes to be around 10 fs for group IV and VI nitrides, a factor of 3 - 4 smaller than noble metals, due to strong electron-phonon scattering. However, we find longer carrier lifetimes for group V nitrides, comparable to silver for NbN and TaN, while exceeding 100 fs (twice that of silver) for VN, making them promising candidates for efficient hot carrier extraction.
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