53 research outputs found
Optical Properties of Organometallic Perovskite: An ab initio Study using Relativistic GW Correction and Bethe-Salpeter Equation
In the development of highly efficient photovoltaic cells, solid perovskite
systems have demonstrated unprecedented promise, with the figure of merit
exceeding nineteen percent of efficiency. In this paper, we investigate the
optical and vibrational properties of organometallic cubic perovskite
CH3NH3PbI3 using first-principles calculations. For accurate theoretical
description, we go beyond conventional density functional theory (DFT), and
calculated optical conductivity using relativist quasi-particle (GW)
correction. Incorporating these many-body effects, we further solve
Bethe-Salpeter equations (BSE) for excitons, and found enhanced optical
conductivity near the gap edge. Due to the presence of organic methylammonium
cations near the center of the perovskite cell, the system is sensitive to low
energy vibrational modes. We estimate the phonon modes of CH3NH3PbI3 using
small displacement approach, and further calculate the infrared absorption (IR)
spectra. Qualitatively, our calculations of low-energy phonon frequencies are
in good agreement with our terahertz measurements. Therefore, for both energy
scales (around 2 eV and 0-20 meV), our calculations reveal the importance of
many-body effects and their contributions to the desirable optical properties
in the cubic organometallic perovskites system.Comment: 5 pages, 4 figure
Monitoring Electron–Phonon Interactions in Lead-Halide Perovskites Using Time-Resolved THz Spectroscopy
Lead halide perovskite semiconductors have low-frequency phonon modes within the lead halide sublattice and thus are considered to be soft. The soft lattice is considered to be important in defining their interesting optoelectronic properties. Electron–phonon coupling governs hot-carrier relaxation, carrier mobilities, carrier lifetimes, among other important electronic characteristics. Directly observing the interplay between free charge carriers and phonons can provide details on how phonons impact these properties (e.g., exciton populations and other collective modes). Here, we observe a delicate interplay among carriers, phonons, and excitons in mixed-cation and mixed-halide perovskite films by simultaneously resolving the contribution of charge carriers and phonons in time-resolved terahertz photoconductivity spectra. We are able to observe directly the increase in phonon population during carrier cooling and discuss how thermal equilibrium populations of carriers and phonons modulate the carrier transport properties, as well as reduce the population of carriers within band tails. We are also able to observe directly the formation of free charge carriers when excitons interact with phonons and dissociate and to describe how free carriers and exciton populations exchange through phonon interactions. Finally, we also time-resolve how the carriers are screened via the Coulomb interaction at low and room temperatures. Our studies shed light on how charge carriers interact with the low-energy phonons and discuss implications
Evidence for Photoinduced Insulator-to-Metal transition in B-phase vanadium dioxide
10.1038/srep25538Scientific Reports62553
Ultrafast demagnetization dynamics at the M edges of magnetic elements observed using a tabletop high-harmonic soft X-ray source
We use few-femtosecond soft x-ray pulses from high-harmonic generation to extract element-specific demagnetization dynamics and hysteresis loops of a compound material for the first time. Using a geometry where high-harmonic beams are reflected from a magnetized Permalloy grating, large changes in the reflected intensity of up to 6% at the M absorption edges of Fe and Ni are observed when the magnetization is reversed. A short pump pulse is used to destroy the magnetic alignment, which allows us to measure the fastest, elementally specific demagnetization dynamics, with 55 fs time resolution. The use of high harmonics for probing magnetic materials promises to combine nanometer spatial resolution, elemental specificity, and femtosecond-to-attosecond time resolution, making it possible to address important fundamental questions in magnetism
Interface-induced magnetic coupling in multiferroic/ferromagnetic bilayer : an ultrafast pump-probe study
By use of optical pump-probe measurement, we study the relaxation dynamics of a multiferroic-ferromagnetic TbMnO3/La0.7Sr0.3MnO3 bilayer. The relaxation dynamics of both layers are well separated in time allowing us to investigate the magnetic coupling across the bilayer. We observe that the relaxation dynamics of the individual layers in the bilayer sample are the result of the interplay between the intrinsic magnetic order and the induced interfacial effect. Our data suggest the existence of induced ferromagnetic order in the TbMnO3 layer and antiferromagnetic order in the La0.7Sr0.3MnO3 layer.Published versio
Erratum: Optical properties of organometallic perovskite: An ab initio study using relativistic GW correction and Bethe-Salpeter equation
Original article: EPL, 108 (2014) 6701
Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions
Ultrashort pulses of extreme ultraviolet light from high-harmonic generation are a new tool for probing coupled charge, spin, and phonon dynamics with element specificity, attosecond pump-probe synchronization, and time resolution of a few femtoseconds in a tabletop apparatus. In this paper, we address an important question in magneto-optics that has implications for understanding magnetism on the fastest time scales: Is the signal from the transverse magneto-optical Kerr effect at the M2,3 edges of a magnetic material purely magnetic or is it perturbed by nonmagnetic artifacts? Our measurements demonstrate conclusively that transverse magneto-optical Kerr measurements at the M2,3 edges sensitively probe the magnetic state, with almost negligible contributions from the transient variation of the refractive index by the nonequilibrium hot-electron distribution. In addition, we compare pump-probe demagnetization dynamics measured by both high harmonics and conventional visible-wavelength magneto-optics and find that the measured demagnetization times are in agreement
Controlling the Competition between Optically Induced Ultrafast Spin-Flip Scattering and Spin Transport in Magnetic Multilayers
The study of ultrafast dynamics in magnetic materials provides rich opportunities for greater fundamental understanding of correlated phenomena in solid-state matter, because many of the basic microscopic mechanisms involved are as-yet unclear and are still being uncovered. Recently, two different possible mechanisms have been proposed to explain ultrafast laser induced magnetization dynamics: spin currents and spin-flip scattering. In this work, we use multilayers of Fe and Ni with different metals and insulators as the spacer material to conclusively show that spin currents can have a significant contribution to optically induced magnetization dynamics, in addition to spin-flip scattering processes. Moreover, we can control the competition between these two processes, and in some cases completely suppress interlayer spin currents as a sample undergoes rapid demagnetization. Finally, by reversing the order of the Fe/Ni layers, we experimentally show that spin currents are directional in our samples, predominantly flowing from the top to the bottom layer
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