Abstract In high fluence applications of lead halide perovskites for light-emitting diodes and lasers, multi-polaron interactions and associated Auger recombination limit the device performance. However, the relationship of the ultrafast and strongly lattice coupled carrier dynamics to nanoscale heterogeneities has remained elusive. Here, in ultrafast visible-pump infrared-probe nano-imaging of the photoinduced carrier dynamics in triple cation perovskite films, a ~20 % variation in sub-ns relaxation dynamics with spatial disorder on tens to hundreds of nanometer is resolved. We attribute the non-uniform relaxation dynamics to the heterogeneous evolution of polaron delocalization and increasing scattering time. The initial high-density excitation results in faster relaxation due to strong many-body interactions, followed by extended carrier lifetimes at lower densities. These results point towards the missing link between the optoelectronic heterogeneity and associated carrier dynamics to guide synthesis and device engineering for improved perovskites device performance.
more »
« less
Ultrafast nanometric resolution spatiotemporal measurement of ambipolar diffusivity and carrier-phonon coupling in doped and undoped silicon
Understanding and determination of the ambipolar diffusivity of a semiconductor is fundamental for predicting device behavior and optimizing its performance. Ultrafast pump-probe measurements allow for the determination of energy carrier dynamics with sub-picosecond resolution. Due to the inherent diffusive nature of carriers, measurements with a high spatial resolution are needed, in addition to the traditional pump-probe system, to determine not only the carrier dynamics but also the spatial extent caused by carrier diffusion as well. In this work, a spatiotemporal measurement system with ultrafast temporal and nanometric spatial resolution, together with a comprehensive transport model, is used to determine the ambipolar diffusivity and carrier-phonon energy coupling time in both undoped and doped silicon. The results show that as the carrier density increases, the measured ambipolar diffusivity decreases with minimal variation in the carrier-phonon energy coupling time. In general, this work demonstrates an optical-based method for determining ambipolar diffusivity in a semiconductor material.
more »
« less
- Award ID(s):
- 2051525
- PAR ID:
- 10526056
- Publisher / Repository:
- APS
- Date Published:
- Journal Name:
- Applied Physics Letters
- Volume:
- 124
- Issue:
- 21
- ISSN:
- 0003-6951
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
We report a combined theoretical and experimental study on photocarrier dynamics in monolayer phosphorene and bulk black phosphorus. Samples of monolayer phosphorene and bulk black phosphorus were fabricated by mechanical exfoliation, identified according to their reflective contrasts, and protected by covering them with hexagonal boron nitride layers. Photocarrier dynamics in these samples was studied by an ultrafast pump–probe technique. The photocarrier lifetime of monolayer phosphorene was found to be about 700 ps, which is about 9 times longer than that of bulk black phosphorus. This trend was reproduced in our calculations based on ab initio nonadiabatic molecular dynamics combined with time-domain density functional theory in the Kohn–Sham representation, and can be attributed to the smaller bandgap and stronger nonadiabatic coupling in bulk. The transient absorption response was also found to be dependent on the sample orientation with respect to the pump polarization, which is consistent with the previously reported anisotropic absorption of phosphorene. In addition, an oscillating component of the differential reflection signal at early probe delays was observed in the bulk sample and was attributed to the layer-breathing phonon mode with an energy of about 1 meV and a decay time of about 1.35 ps. These results provide valuable information for application of monolayer phosphorene in optoelectronics.more » « less
-
LaPierre, Ray (Ed.)Abstract Recent advances in the growth of III-V semiconductor nanowires (NWs) hold great promise for nanoscale optoelectronic device applications. Recently, it was found that a small amount of nitrogen (N) incorporation in III-V semiconductor NWs can effectively red-shift their wavelength of operation and tailor their electronic properties for specific applications. However, understanding the impact of N incorporation on non-equilibrium charge carrier dynamics and transport in semiconducting NWs is critical in achieving efficient semiconducting NW devices. In this work, ultrafast optical pump-terahertz probe spectroscopy has been used to study non-equilibrium carrier dynamics and transport in Te-doped GaAsSb and dilute nitride GaAsSbN NWs, with the goal of correlating these results with electrical characterization of their equilibrium photo-response under bias and low-frequency noise characteristics. Nitrogen incorporation in GaAsSb NWs led to a significant increase in the carrier scattering rate, resulting in a severe reduction in carrier mobility. Carrier recombination lifetimes of 33 ± 1 picoseconds (ps) and 147 ± 3 ps in GaAsSbN and GaAsSb NWs, respectively, were measured. The reduction in the carrier lifetime and photoinduced optical conductivities are due to the presence of N-induced defects, leading to deterioration in the electrical and optical characteristics of dilute nitride NWs relative to the non-nitride NWs. Finally, we observed a very fast rise time of ~ 2 ps for both NW materials, directly impacting their potential use as high-speed photodetectors.more » « less
-
Pump–probe experiments at X-ray free-electron laser (XFEL) facilities are a powerful tool for studying dynamics at ultrafast and longer timescales. Observing the dynamics in diverse scientific cases requires optical laser systems with a wide range of wavelength, flexible pulse sequences and different pulse durations, especially in the pump source. Here, the pump–probe instrumentation available for measurements at the Single Particles, Clusters, and Biomolecules and Serial Femtosecond Crystallography (SPB/SFX) instrument of the European XFEL is reported. The temporal and spatial stability of this instrumentation is also presented.more » « less
-
Abstract Active nanostructured optical components show promise as potential building blocks for novel light‐based computing and data processing architectures. However, nanoscale all‐optical switches that have low activation powers and high‐contrast ultrafast switching have been elusive so far. Here, pump–probe measurements performed on amorphous‐Ge‐based micro‐resonator metasurfaces that exhibit strong resonant modes in the mid‐infrared are reported. Relative change is observed in transmittance of ΔT/T ≈ 1 with picosecond (down to τ ≈ 0.5 ps) free carrier relaxation rates, obtained with very low pump fluences of 50 μJ cm−2. These observations are attributed to efficient free carrier promotion, affecting light transmittance via high quality‐factor optical resonances, followed by an increased electron–phonon scattering of free carriers due to the amorphous crystal structure of Ge. Full‐wave simulations based on a permittivity model that describes free‐carrier damping through crystal structure disorder find excellent agreement with the experimental data. These findings offer an efficient and robust platform for all‐optical switching at the nanoscale.more » « less
An official website of the United States government

