Crystallographic, optical, and electronic properties of the Cs2AgBi1-xInxBr6 double perovskite: understanding the fundamental photovoltaic efficiency challenges

ACS Energy Letters American Chemical Society 6:3 (2021) 1073-1081

Authors:

Laura Schade, Suhas Mahesh, George Volonakis, Marios Zacharias, Bernard Wenger, Felix Schmidt, Sameer Vajjala Kesava, Dharmalingam Prabhakaran, Mojtaba Abdi-Jalebi, Markus Lenz, Feliciano Giustino, Giulia Longo, Paolo Radaelli, Henry Snaith

Abstract:

We present a crystallographic and optoelectronic study of the double perovskite Cs2AgBi1–xInxBr6. From structural characterization we determine that the indium cation shrinks the lattice and shifts the cubic-to-tetragonal phase transition point to lower temperatures. The absorption onset is shifted to shorter wavelengths upon increasing the indium content, leading to wider band gaps, which we rationalize through first-principles band structure calculations. Despite the unfavorable band gap shift, we observe an enhancement in the steady-state photoluminescence intensity, and n-i-p photovoltaic devices present short-circuit current greater than that of neat Cs2AgBiBr6 devices. In order to evaluate the prospects of this material as a solar absorber, we combine accurate absorption measurements with thermodynamic modeling and identify the fundamental limitations of this system. Provided radiative efficiency can be increased and the choice of charge extraction layers are specifically improved, this material could prove to be a useful wide band gap solar absorber.

Modification of the van der Waals interaction at the Bi2Te3 and Ge(111) interface

Physical Review Materials American Physical Society 5 (2021) 024203

Authors:

K Nawa, D Kepaptsoglou, A Ghasemi, P Hasnip, G Bárcena-González, G Nicotra, Pl Galindo, Qm Ramasse, K Nakamura, B Kuerbanjiang, Thorsten Hesjedal, V Lazarov

Abstract:

We present a structural and density-functional theory study of the interface of the quasi-twin-free grown three-dimensional topological insulator Bi2Te3 on Ge(111). Aberration-corrected scanning transmission electron microscopy and electron energy-loss spectroscopy in combination with first-principles calculations show that the weak van der Waals adhesion between the Bi2Te3 quintuple layer and Ge can be overcome by forming an additional Te layer at their interface. The first-principles calculations of the formation energy of the additional Te layer show it to be energetically favorable as a result of the strong hybridization between the Te and Ge.

Spin-current mediated exchange coupling in MgO-based magnetic tunnel junctions

Physical Review B: Condensed Matter and Materials Physics American Physical Society 103:6 (2021) 064416

Authors:

Lukasz Gladczuk, L Gladczuk, P Dluzewski, K Lasek, P Aleshkevych, Db Burn, G van der Laan, Thorsten Hesjedal

Abstract:

Heterostructures composed of ferromagnetic layers that are mutually interacting through a nonmagnetic spacer are at the core of magnetic sensor and memory devices. In the present study, layer-resolved ferromagnetic resonance was used to investigate the coupling between the magnetic layers of a Co/MgO/Permalloy magnetic tunnel junction. Two magnetic resonance peaks were observed for both magnetic layers, as probed at the Co and Ni L3 x-ray absorption edges, showing a strong interlayer interaction through the insulating MgO barrier. A theoretical model based on the Landau-Lifshitz-Gilbert-Slonczewski equation was developed, including exchange coupling and spin pumping between the magnetic layers. Fits to the experimental data were carried out, both with and without a spin pumping term, and the goodness of the fit was compared using a likelihood ratio test. This rigorous statistical approach provides an unambiguous proof of the existence of interlayer coupling mediated by spin pumping.

Antiferromagnetic half-skyrmions and bimerons at room temperature

Nature Springer Nature 590:2021 (2021) 74-79

Authors:

Hariom Jani, Jheng-Cyuan Lin, Jiahao Chen, Jack Harrison, Francesco Maccherozzi, Jonathan Schad, Saurav Prakash, Chang-Beom Eom, A Ariando, T Venkatesan, Paolo G Radaelli

Abstract:

In the quest for post-CMOS technologies, ferromagnetic skyrmions and their anti-particles have shown great promise as topologically protected solitonic information carriers in memory-in-logic or neuromorphic devices. However, the presence of dipolar fields in ferromagnets, restricting the formation of ultra-small topological textures, and the deleterious skyrmion Hall effect when driven by spin torques have thus far inhibited their practical implementations. Antiferromagnetic analogues, which are predicted to demonstrate relativistic dynamics, fast deflection-free motion and size scaling have recently come into intense focus, but their experimental realizations in natural antiferromagnetic systems are yet to emerge. Here, we demonstrate a family of topological antiferromagnetic spin-textures in $\alpha$-Fe$_2$O$_3$ - an earth-abundant oxide insulator - capped with a Pt over-layer. By exploiting a first-order analogue of the Kibble-Zurek mechanism, we stabilize exotic merons-antimerons (half-skyrmions), and bimerons, which can be erased by magnetic fields and re-generated by temperature cycling. These structures have characteristic sizes in the range ~100 nm that can be chemically controlled via precise tuning of the exchange and anisotropy, with pathway to further scaling. Driven by current-based spin torques from the heavy-metal over-layer, some of these AFM textures could emerge as prime candidates for low-energy antiferromagnetic spintronics at room temperature.

Halide segregation in mixed-halide perovskites: influence of a-site cations

ACS Energy Letters American Chemical Society 6:2 (2021) 799-808

Authors:

Alexander Knight, Anna Juliane Borchert, Robert DJ Oliver, Jay Patel, Paolo G Radaelli, Henry Snaith, Michael B Johnston, Laura M Herz

Abstract:

Mixed-halide perovskites offer bandgap tunability essential for multijunction solar cells; however, a detrimental halide segregation under light is often observed. Here we combine simultaneous in situ photoluminescence and X-ray diffraction measurements to demonstrate clear differences in compositional and optoelectronic changes associated with halide segregation in MAPb(Br0.5I0.5)3 and FA0.83Cs0.17Pb(Br0.4I0.6)3 films. We report evidence for low-barrier ionic pathways in MAPb(Br0.5I0.5)3, which allow for the rearrangement of halide ions in localized volumes of perovskite without significant compositional changes to the bulk material. In contrast, FA0.83Cs0.17Pb(Br0.4I0.6)3 lacks such low-barrier ionic pathways and is, consequently, more stable against halide segregation. However, under prolonged illumination, it exhibits a considerable ionic rearrangement throughout the bulk material, which may be triggered by an initial demixing of A-site cations, altering the composition of the bulk perovskite and reducing its stability against halide segregation. Our work elucidates links between composition, ionic pathways, and halide segregation, and it facilitates the future engineering of phase-stable mixed-halide perovskites.