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.

Antiferromagnetic half-skyrmions and bimerons at room temperature

Nature Springer Nature 590:7844 (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 (complementary metal–oxide–semiconductor) technologies, driven by the need for improved efficiency and performance, topologically protected ferromagnetic ‘whirls’ such as skyrmions1,2,3,4,5,6,7,8 and their anti-particles have shown great promise as solitonic information carriers in racetrack memory-in-logic or neuromorphic devices1,9,10,11. However, the presence of dipolar fields in ferromagnets, which restricts the formation of ultrasmall topological textures3,6,8,9,12, and the deleterious skyrmion Hall effect, when skyrmions are driven by spin torques9,10,12, have thus far inhibited their practical implementation. Antiferromagnetic analogues, which are predicted to demonstrate relativistic dynamics, fast deflection-free motion and size scaling, have recently become the subject of intense focus9,13,14,15,16,17,18,19, but they have yet to be experimentally demonstrated in natural antiferromagnetic systems. Here we realize a family of topological antiferromagnetic spin textures in α-Fe2O3—an Earth-abundant oxide insulator—capped with a platinum overlayer. By exploiting a first-order analogue of the Kibble–Zurek mechanism20,21, we stabilize exotic merons and antimerons (half-skyrmions)8 and their pairs (bimerons)16,22, which can be erased by magnetic fields and regenerated by temperature cycling. These structures have characteristic sizes of the order of 100 nanometres and can be chemically controlled via precise tuning of the exchange and anisotropy, with pathways through which further scaling may be achieved. Driven by current-based spin torques from the heavy-metal overlayer, some of these antiferromagnetic textures could emerge as prime candidates for low-energy antiferromagnetic spintronics at room temperature1,9,10,11,23.

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.

Antiferromagnetic half-skyrmions and bimerons at room temperature

University of Oxford (2021)

Abstract:

The datasets included herein contain experimental results (X-ray absorption, dichroic photoemission electron microscopy, diffraction, magnetometry etc.) and related analysis for the investigation of antiferromagnetic topological textures. The processes used in the obtaining, reducing and analysing the datasets can be found in the Methods and Supplementary Information sections of the published manuscript.

Effects of magnetic dilution in the ferrimagnetic columnar ordered Sm2MnMnMn4-xTixO12 perovskites

PHYSICAL REVIEW B 102:21 (2020) ARTN 214428

Authors:

Anuradha M Vibhakar, Dmitry D Khalyavin, Pascal Manuel, Ran Liu, Kazunari Yamaura, Alexei A Belik, Roger D Johnson

Abstract:

© 2020 American Physical Society. Powder neutron-diffraction experiments have been employed to establish the effects of site-selective magnetic dilution in the Sm2MnMnMn4-xTixO12 A-site columnar ordered quadruple perovskite manganites (x=1, x=2, and x=3). We show that in all three compositions the Mn ions adopt a collinear ferrimagnetic structure below 27, 62, and 34 K, respectively. An unexpected increase in the ordering temperature was observed between the x=1 and x=2 samples, which indicates a considerable departure from mean-field behavior. This result is corroborated by large reductions in the theoretical ground-state magnetic moments observed across the series, which indicate the presence of spin fluctuations and/or disorder. We show that long-range magnetic order in the x=3 sample, which occurs below the percolation threshold for B-B exchange, can only be understood to arise if it is mediated via both A-B and B-B exchange, hence confirming the importance of A-B exchange interactions in these materials. Finally, we show that site-selective magnetic dilution enables the tuning of a ferrimagnetic compensation point and the introduction of temperature-induced magnetization reversal.