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Register a new userUltrafast polarization control of zero-bias photocurrent and terahertz emission in hybrid organic perovskites
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Methylammonium lead iodide (MAPI) is a benchmark hybrid organic perovskite material, which is used for the low-cost, printed solar cells with over 20 percent power conversion efficiency. Yet, the nature of light-matter interaction in MAPI as well as the exact physical mechanism behind device operation is currently debated. Here we report room temperature, ultrafast photocurrent and freespace terahertz (THz) emission generation from unbiased MAPI induced by 150 fs light pulses. Polarization dependence of the observed photoresponse is consistent with the Bulk Photovoltaic Effect (BPVE) caused by a combination of injection and shift currents. We believe that this observation of can shed light on low recombination, and long carrier diffusion lengths due to indirect bandgap. Moreover, ballistic by nature shift and injection BPVE photocurrents may enable third generation perovskite solar cells with efficiency that exceed the Shockley_Queisser limit. Our observations also open new venues for perovskite spintronics and tunable THz sources.
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For a class of 2D hybrid organic-inorganic perovskite semiconductors based on $pi$-conjugated organic cations, we predict quantitatively how varying the organic and inorganic component allows control over the nature, energy and localization of carrier states in a quantum-well-like fashion. Our first-principles predictions, based on large-scale hybrid density-functional theory with spin-orbit coupling, show that the interface between the organic and inorganic parts within a single hybrid can be modulated systematically, enabling us to select between different type-I and type-II energy level alignments. Energy levels, recombination properties and transport behavior of electrons and holes thus become tunable by choosing specific organic functionalizations and juxtaposing them with suitable inorganic components.
Behaving like atomically-precise two-dimensional quantum wells with non-negligible dielectric contrast, the layered HOIPs have strong electronic interactions leading to tightly bound excitons with binding energies on the order of 500 meV. These strong interactions suggest the possibility of larger excitonic complexes like trions and biexcitons, which are hard to study numerically due to the complexity of the layered HOIPs. Here, we propose and parameterize a model Hamiltonian for excitonic complexes in layered HOIPs and we study the correlated eigenfunctions of trions and biexcitons using a combination of diffusion Monte Carlo and very large variational calculations with explicitly correlated Gaussian basis functions. Binding energies and spatial structures of these complexes are presented as a function of the layer thickness. The trion and biexciton of the thinnest layered HOIP have binding energies of 35 meV and 44 meV, respectively, whereas a single exfoliated layer is predicted to have trions and biexcitons with equal binding enegies of 48 meV. We compare our findings to available experimental data and to that of other quasi-two-dimensional materials.
The hybrid organic inorganic perovskites (HOIPs) have attracted much attention for their potential applications as novel optoelectronic devices. Remarkably, the Rashba band splitting, together with specific spin orientations in k space (i.e., spin texture), has been found to be relevant for the optoelectronic performances. In this work, by using first principles calculations and symmetry analyses, we study the electric polarization, magnetism, and spin texture properties of the antiferromagnetic (AFM) HOIP ferroelectric TMCM_MnCl3 (TMCM = (CH3)3NCH2Cl, trimethylchloromethyl ammonium). This recently synthesized compound is a prototype of order disorder and displacement-type ferroelectric with a large piezoelectric response, high ferroelectric transition temperature, and excellent photoluminescence properties [You et al., Science 357, 306 (2017)]. The most interesting result is that the inversion symmetry breaking coupled to the spin orbit coupling gives rise to a Rashba-like band splitting and a related robust persistent spin texture (PST) and/or typical spiral spin texture, which can be manipulated by tuning the ferroelectric or, surprisingly, also by the AFM magnetic order parameter. The tunability of spin texture upon switching of AFM order parameter is largely unexplored and our findings not only provide a platform to understand the physics of AFM spin texture but also support the AFM HOIP ferroelectrics as a promising class of optoelectronic materials.
Bulk quantum materials based on zero-dimensional (0D) lead-free organic tin halide perovskites have been developed for the first time, which give broadband Gaussian-shaped and strongly Stokes shifted emissions with quantum efficiencies of up to near-unity at room temperature due to excited state structural reorganization.
Terahertz spin waves could be generated on-demand via all-optical manipulation of magnetization by femtosecond laser pulse. Here, we present an energy balance model, which explains the energy transfer rates from laser pulse to electron bath coupled with phonon, spin, and magnetization of five different magnetic metallic thin films: Iron, Cobalt, Nickel, Gadolinium and Ni$_{2}$MnSn Heusler alloy. Two types of transient magnetization dynamics emerge in metallic magnetic thin films based on their Curie temperatures (T$_{C}$): type I (Fe, Co, and Ni with T$_{C}$ > room temperature, RT) and type II films (Gd and Ni$_{2}$MnSn with T$_{C}$ $approx$ RT). We study the effect of laser fluence and pulse width for single Gaussian laser pulses and the effect of metal film thickness on magnetization dynamics. Spectral dynamics show that broadband spin waves up to 24 THz could be generated by all-optical manipulation of magnetization in these nanofilms.
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