Shared posts

30 Jan 11:38

Scalable high yield exfoliation for monolayer nanosheets

by Zhuyuan Wang

Nature Communications, Published online: 16 January 2023; doi:10.1038/s41467-022-35569-8

Top-down exfoliation is one of the most promising approaches for the scalable production of 2D materials, but the current techniques are limited by low yield of monolayers. Here, the authors report the exfoliation of graphene and other layered materials via viscous-polymer-assisted ball-milling, leading to a production of graphene products with monolayer percentage up to 97.9% at a yield of 78.3%.
30 Jan 11:38

Phonon-mediated room-temperature quantum Hall transport in graphene

by Daniel Vaquero

Nature Communications, Published online: 19 January 2023; doi:10.1038/s41467-023-35986-3

Monolayer graphene can support the quantum Hall effect up to room temperature. Here, the authors provide evidence that graphene encapsulated in hexagonal boron nitride realizes a novel transport regime where dissipation in the quantum Hall phase is mediated predominantly by electron-phonon scattering rather than disorder scattering.
30 Jan 11:37

General low-temperature growth of two-dimensional nanosheets from layered and nonlayered materials

by Biao Qin

Nature Communications, Published online: 19 January 2023; doi:10.1038/s41467-023-35983-6

Chemical vapor deposition (CVD) is a versatile method to synthesize 2D materials, but usually requires high growth temperatures. Here, the authors report a BiOCl-assisted CVD approach to grow 2D nanosheets from 27 different layered and nonlayered materials at temperatures <500 °C, which are compatible with back-end-of-the-line industrial processes.
30 Jan 11:34

Interplay between superconductivity and the strange-metal state in FeSe

by Xingyu Jiang

Nature Physics, Published online: 16 January 2023; doi:10.1038/s41567-022-01894-4

Superconductivity can emerge from a strange-metal state, but the exact relationship between them is unknown. Now, quantitative measurements reveal the dependence of resistivity in the strange metal on the superconducting transition temperature.
30 Jan 11:33

Observation of spin-momentum locked surface states in amorphous Bi2Se3

by Paul Corbae

Nature Materials, Published online: 16 January 2023; doi:10.1038/s41563-022-01458-0

The authors present evidence suggesting that amorphous Bi2Se3 displays topological properties, signalling a new regime for the pursuit of topological matter.
30 Jan 11:32

A superconducting quantum simulator based on a photonic-bandgap metamaterial | Science

A superconducting qubit-metamaterial system creates a scalable lattice quantum simulator.
30 Jan 11:31

[ASAP] Metal Halide Perovskite Heterostructures: Blocking Anion Diffusion with Single-Layer Graphene

by Matthew P. Hautzinger, Emily K. Raulerson, Steven P. Harvey, Tuo Liu, Daniel Duke, Xixi Qin, Rebecca A. Scheidt, Brian M. Wieliczka, Alan J. Phillips, Kenneth R. Graham, Volker Blum, Joseph M. Luther, Matthew C. Beard, and Jeffrey L. Blackburn

TOC Graphic

Journal of the American Chemical Society
DOI: 10.1021/jacs.2c12441
30 Jan 11:25

Room-temperature magnetoresistance in an all-antiferromagnetic tunnel junction

by Peixin Qin

Nature, Published online: 18 January 2023; doi:10.1038/s41586-022-05461-y

A new exchange-bias effect between two different antiferromagnetic layers enables the fabrication of all-antiferromagnetic structures that have a large room-temperature tunnelling magnetoresistance and potential applications for ultrafast memory technologies.
30 Jan 11:25

Non-epitaxial single-crystal 2D material growth by geometric confinement

by Ki Seok Kim

Nature, Published online: 18 January 2023; doi:10.1038/s41586-022-05524-0

Geometric confinement on arbitrary substrates promotes, without epitaxial seeding, the layer-by-layer growth of two-dimensional single-crystal monolayers and bilayers of transition metal dichalcogenides.
30 Jan 11:25

In-plane charged domain walls with memristive behaviour in a ferroelectric film

by Zhongran Liu

Nature, Published online: 18 January 2023; doi:10.1038/s41586-022-05503-5

The direct observation of in-plane charged domain walls in BiFeO3 ferroelectric films a few nanometres thick, their deterministic creation, manipulation and annihilation by applied voltage, as well the demonstration of their memristive functionality is reported.
30 Jan 11:22

[ASAP] In Situ Imaging of an Anisotropic Layer-by-Layer Phase Transition in Few-Layer MoTe2

by Chia-Hao Lee, Huije Ryu, Gillian Nolan, Yichao Zhang, Yangjin Lee, Siwon Oh, Hyeonsik Cheong, Kenji Watanabe, Takashi Taniguchi, Kwanpyo Kim, Gwan-Hyoung Lee, and Pinshane Y. Huang

TOC Graphic

Nano Letters
DOI: 10.1021/acs.nanolett.2c04550
30 Jan 11:10

Chip-scale acoustics gets amped up

by Siddhartha Ghosh

Nature Electronics, Published online: 16 January 2023; doi:10.1038/s41928-022-00910-y

An acoustoelectric amplifier based on a three-layer heterostructure design could be used to create all-acoustic radiofrequency microsystems.
30 Jan 11:10

Non-reciprocal acoustoelectric microwave amplifiers with net gain and low noise in continuous operation

by Lisa Hackett

Nature Electronics, Published online: 16 January 2023; doi:10.1038/s41928-022-00908-6

Three-layer heterostructures consisting of an indium gallium arsenide semiconducting film, a lithium niobate piezoelectric film, and a silicon substrate can be used to create acoustoelectric amplifiers that operate at gigahertz frequencies with large non-reciprocal gain and low noise in continuous operation.
30 Jan 09:35

Electrical Interrogation of Thickness‐Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI2

by Dmitry Lebedev, Jonathan Tyler Gish, Ethan Skyler Garvey, Teodor Kosev Stanev, Junhwan Choi, Leonidas Georgopoulos, Thomas Wei Song, Hong Youl Park, Kenji Watanabe, Takashi Taniguchi, Nathaniel Patrick Stern, Vinod Kumar Sangwan, Mark Christopher Hersam
Electrical Interrogation of Thickness-Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI2

A fabrication protocol is presented that achieves electrically conductive devices from the ambient-reactive 2D antiferromagnetic semiconductor NiI2. The resulting gate-tunable transistors show band-like electronic transport at cryogenic temperatures, allowing electrical probing of the thickness-dependent multiferroic phase transition temperature of NiI2 from 59 K (bulk) to 28 K (monolayer).


Abstract

2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto-electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient-reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient-reactive 2D antiferromagnetic semiconductor NiI2. The resulting gate-tunable transistors show band-like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI2, revealing a Hall mobility of 15 cm2 V−1 s−1 at 1.7 K. These devices also allow direct electrical probing of the thickness-dependent multiferroic phase transition temperature of NiI2 from 59 K (bulk) to 28 K (monolayer).

30 Jan 09:34

Recent Advances in Mechanically Transferable III‐Nitride Based on 2D Buffer Strategy

by Wurui Song, Qi Chen, Kailai Yang, Meng Liang, Xiaoyan Yi, Junxi Wang, Jinmin Li, Zhiqiang Liu
Recent Advances in Mechanically Transferable III-Nitride Based on 2D Buffer Strategy

This study reviews the current state of III-nitride synthesis on different 2D materials for a variety of flexible applications, meanwhile identifying key advances in this rapidly accelerating field. The focus of this study is to provide guidelines on the exfoliation of epitaxial layers using 2D materials, with the aim of fabricating flexible nitride devices.


Abstract

Group III-nitrides have attracted significant attention in recent years for their wide tunable band-gaps and excellent optoelectronic capabilities, which are advantageous for several applications including light-emitting diodes, lasers, photodetectors, and large-size low-cost power electronic devices. However, conventional epitaxy accompanied by the covalent bond formation renders the transfer of nitride epilayers difficult, thereby limiting the application potential of nitrides in wearable and flexible electronics. Furthermore, interfacial covalent bonds also limit substrate selection and hinder the development of heterogeneous integration between nitrides and other material systems. 2D materials can mitigate these problems significantly. On the one hand, due to the weak van der Waals forces between the layers of 2D materials, influences of lattice mismatch can be avoided to improve crystal quality. On the other hand, delamination and transfer of nitride epilayers can be achieved easily. Therefore, this study focuses on providing comprehensive guidelines regarding the exfoliation of epitaxial layers using 2D materials to provide new design freedoms for nitride devices. Different 2D buffers and release layers have also been discussed. Furthermore, the limitations, promising solutions, future directions, and applicability of this strategy to flexible nitride devices are presented.

30 Jan 09:31

The Atomic Drill Bit: Precision Controlled Atomic Fabrication of 2D Materials

by Matthew G. Boebinger, Courtney Brea, Li‐Ping Ding, Sudhajit Misra, Olugbenga Olunloyo, Yiling Yu, Kai Xiao, Andrew R. Lupini, Feng Ding, Guoxiang Hu, Panchapakesan Ganesh, Stephen Jesse, Raymond R. Unocic
The Atomic Drill Bit: Precision Controlled Atomic Fabrication of 2D Materials

Through direct and automated control over the electron beam scan pathway profile in an aberration-corrected scanning transmission electron microscope, metallic 1D–2D edge heterostructures are fabricated with atomic precision in semiconducting MoS2. This atomic fabrication workflow paves the way for precision controlled atomic fabrication of functional nanomaterials.


Abstract

The ability to deterministically fabricate nanoscale architectures with atomic precision is the central goal of nanotechnology, whereby highly localized changes in the atomic structure can be exploited to control device properties at their fundamental physical limit. Here, an automated, feedback-controlled atomic fabrication method is reported and the formation of 1D–2D heterostructures in MoS2 is demonstrated through selective transformations along specific crystallographic orientations. The atomic-scale probe of an aberration-corrected scanning transmission electron microscope (STEM) is used, and the shape and symmetry of the scan pathway relative to the sample orientation are controlled. The focused and shaped electron beam is used to reliably create Mo6S6 nanowire (MoS-NW) terminated metallic-semiconductor 1D–2D edge structures within a pristine MoS2 monolayer with atomic precision. From these results, it is found that a triangular beam path aligned along the zig-zag sulfur terminated (ZZS) direction forms stable MoS-NW edge structures with the highest degree of fidelity without resulting in disordering of the surrounding MoS2 monolayer. Density functional theory (DFT) calculations and ab initio molecular dynamic simulations (AIMD) are used to calculate the energetic barriers for the most stable atomic edge structures and atomic transformation pathways. These discoveries provide an automated method to improve understanding of atomic-scale transformations while opening a pathway toward more precise atomic-scale engineering of materials.

30 Jan 09:31

Unravelling the Interfacial Dynamics of Bandgap Funneling in Bismuth‐Based Halide Perovskites (Adv. Mater. 2/2023)

by Yunqi Tang, Chun Hong Mak, Jun Zhang, Guohua Jia, Kuan‐Chen Cheng, Haisheng Song, Mingjian Yuan, Shijun Zhao, Ji‐Jung Kai, Juan Carlos Colmenares, Hsien‐Yi Hsu
Unravelling the Interfacial Dynamics of Bandgap Funneling in Bismuth-Based Halide Perovskites (Adv. Mater. 2/2023)

Interfacial Dynamics

In article number 2207835, Hsien-Yi Hsu and co-workers systematically study interfacial dynamics of bandgap funnelling in MA3Bi2Cl9−x I x perovskites using temperature-dependent transient photoluminescence and electrochemical voltammetric techniques. The photophysical and (photo)electrochemical phenomena of solid–solid and solid–liquid interfaces are therefore confirmed. The importance of this work is to explore the intrinsic and interfacial properties of semiconductor materials for elucidating the correlation between material characterization and device performance.


30 Jan 09:30

Controlled Adhesion of Ice—Toward Ultraclean 2D Materials

by Haijun Liu, Quoc Huy Thi, Ping Man, Xin Chen, Tianren Chen, Lok‐Wing Wong, Shan Jiang, Lingli Huang, Tiefeng Yang, Ka‐Ho Leung, Tsz‐Tung Leung, Shan Gao, Honglin Chen, Chun‐Sing Lee, Min Kan, Jiong Zhao, Qingming Deng, Thuc Hue Ly
Controlled Adhesion of Ice—Toward Ultraclean 2D Materials

Novel ice-aided transfer, ice-stamp transfer, and ice cleaning methods, completely free from polymer and solvents, are developed to yield ultrahigh quality and exceptional cleanliness in 2D materials, which will contribute to technological revolutions in 2D materials, and their associated structures and devices.


Abstract

The scalable 2D device fabrication and integration demand either the large-area synthesis or the post-synthesis transfer of 2D layers. While the direct synthesis of 2D materials on most targeted surfaces remains challenging, the transfer approach from the growth substrate onto the targeted surfaces offers an alternative pathway for applications and integrations. However, the current transfer techniques for 2D materials predominantly involve polymers and organic solvents, which are liable to contaminate or deform the ultrasensitive atomic layers. Here, novel ice-aided transfer and ice-stamp transfer methods are developed, in which water (ice) is the only medium in the entire process. In practice, the adhesion between various 2D materials and ice can be well controlled by temperature. Through such controlled adhesion of ice, it is shown that the new transfer methods can yield ultrahigh quality and exceptional cleanliness in transferred 2D flakes and continuous 2D films, and are applicable for a wide range of substrates. Furthermore, beyond transfer, ice can also be used for cleaning the surfaces of 2D materials at higher temperatures. These novel techniques can enable unprecedented ultraclean 2D materials surfaces and performances, and will contribute to the upcoming technological revolutions associated with 2D materials.

30 Jan 09:25

Widely Tunable Berry Curvature in the Magnetic Semimetal Cr1+δTe2

by Yuita Fujisawa, Markel Pardo‐Almanza, Chia‐ Hsiu Hsu, Atwa Mohamed, Kohei Yamagami, Anjana Krishnadas, Guoqing Chang, Feng‐Chuan Chuang, Khoong Hong Khoo, Jiadong Zang, Anjan Soumyanarayanan, Yoshinori Okada
Widely Tunable Berry Curvature in the Magnetic Semimetal Cr1+δTe2

A self-intercalated transition metal dichalcogenide Cr1+δTe2 is shown to be a unique magnetic semimetal enabling widely tunable k-space Berry curvature near Fermi energy. The door has been opened for probing and tailoring the intertwined Berry curvature physics in real and momentum space in Cr1+δTe2 epitaxial thin films and their heterostructures.


Abstract

Magnetic semimetals have increasingly emerged as lucrative platforms hosting spin-based topological phenomena in real and momentum spaces. Cr1+ δ Te2 is a self-intercalated magnetic transition metal dichalcogenide (TMD), which exhibits topological magnetism and tunable electron filling. While recent studies have explored real-space Berry curvature effects, similar considerations of momentum-space Berry curvature are lacking. Here, the electronic structure and transport properties of epitaxial Cr1+ δ Te2 thin films are systematically investigated over a range of doping, δ (0.33 – 0.71). Spectroscopic experiments reveal the presence of a characteristic semi-metallic band region, which shows a rigid like energy shift with δ. Transport experiments show that the intrinsic component of the anomalous Hall effect (AHE) is sizable and undergoes a sign flip across δ. Finally, density functional theory calculations establish a link between the doping evolution of the band structure and AHE: the AHE sign flip is shown to emerge from the sign change of the Berry curvature, as the semi-metallic band region crosses the Fermi energy. These findings underscore the increasing relevance of momentum-space Berry curvature in magnetic TMDs and provide a unique platform for intertwining topological physics in real and momentum spaces.

30 Jan 09:21

Substitutional p‐Type Doping in NbS2–MoS2 Lateral Heterostructures Grown by MOCVD

by Zhenyu Wang, Mukesh Tripathi, Zahra Golsanamlou, Poonam Kumari, Giuseppe Lovarelli, Fabrizio Mazziotti, Demetrio Logoteta, Gianluca Fiori, Luca Sementa, Guilherme Migliato Marega, Hyun Goo Ji, Yanfei Zhao, Aleksandra Radenovic, Giuseppe Iannaccone, Alessandro Fortunelli, Andras Kis
Substitutional p-Type Doping in NbS2–MoS2 Lateral Heterostructures Grown by MOCVD

p-Type NbS2–MoS2 lateral heterostructures with a high on/off current ratio are synthesized by a one-step metal–organic chemical vapor deposition (MOCVD) method with Nb dopants present in the monolayer MoS2. The heterostructure provides a platform to explore the instructive interface of substitutional doped TMDC materials and 2D metal–semiconductor heterojunctions, which paves a prospective way to designing innovative nanoscale devices and complementary metal–oxide–semiconductor (CMOS)-like 2D circuits.


Abstract

Monolayer MoS2 has attracted significant attention owing to its excellent performance as an n-type semiconductor from the transition metal dichalcogenide (TMDC) family. It is however strongly desired to develop controllable synthesis methods for 2D p-type MoS2, which is crucial for complementary logic applications but remains difficult. In this work, high-quality NbS2–MoS2 lateral heterostructures are synthesized by one-step metal–organic chemical vapor deposition (MOCVD) together with monolayer MoS2 substitutionally doped by Nb, resulting in a p-type doped behavior. The heterojunction shows a p-type transfer characteristic with a high on/off current ratio of ≈104, exceeding previously reported values. The band structure through the NbS2–MoS2 heterojunction is investigated by density functional theory (DFT) and quantum transport simulations. This work provides a scalable approach to synthesize substitutionally doped TMDC materials and provides an insight into the interface between 2D metals and semiconductors in lateral heterostructures, which is imperative for the development of next-generation nanoelectronics and highly integrated devices.

30 Jan 09:20

Unveiling Charge‐Transport Mechanisms in Electronic Devices Based on Defect‐Engineered MoS2 Covalent Networks

by Stefano Ippolito, Francesca Urban, Wenhao Zheng, Onofrio Mazzarisi, Cataldo Valentini, Adam G. Kelly, Sai Manoj Gali, Mischa Bonn, David Beljonne, Federico Corberi, Jonathan N. Coleman, Hai I. Wang, Paolo Samorì
Unveiling Charge-Transport Mechanisms in Electronic Devices Based on Defect-Engineered MoS2 Covalent Networks

Covalent networks of transition metal dichalcogenides (TMDs) represent an efficient strategy to reduce the interflake junction resistance in thin-film devices. This multiscale investigation reveals that the molecular structure of the linker is crucial to control the overall charge-transport mechanisms. This work highlights the great potential of defect engineering for the fabrication of high-performance devices based on covalent TMD networks.


Abstract

Device performance of solution-processed 2D semiconductors in printed electronics has been limited so far by structural defects and high interflake junction resistance. Covalently interconnected networks of transition metal dichalcogenides potentially represent an efficient strategy to overcome both limitations simultaneously. Yet, the charge-transport properties in such systems have not been systematically researched. Here, the charge-transport mechanisms of printed devices based on covalent MoS2 networks are unveiled via multiscale analysis, comparing the effects of aromatic versus aliphatic dithiolated linkers. Temperature-dependent electrical measurements reveal hopping as the dominant transport mechanism: aliphatic systems lead to 3D variable range hopping, unlike the nearest neighbor hopping observed for aromatic linkers. The novel analysis based on percolation theory attributes the superior performance of devices functionalized with π-conjugated molecules to the improved interflake electronic connectivity and formation of additional percolation paths, as further corroborated by density functional calculations. Valuable guidelines for harnessing the charge-transport properties in MoS2 devices based on covalent networks are provided.

30 Jan 09:20

All‐Transfer Electrode Interface Engineering Toward Harsh‐Environment‐Resistant MoS2 Field‐Effect Transistors

by Yonghuang Wu, Zeqin Xin, Zhibin Zhang, Bolun Wang, Ruixuan Peng, Enze Wang, Run Shi, Yiqun Liu, Jing Guo, Kaihui Liu, Kai Liu
All-Transfer Electrode Interface Engineering Toward Harsh-Environment-Resistant MoS2 Field-Effect Transistors

Harsh-environment-resistant MoS2 field-effect transistors are demonstrated by engineering the electrode–channel interfaces with an all-transfer technique of van der Waals electrodes. The intact and defect-free interfaces not only reduce the Schottky barrier height at electrodes, but enable high resistances of the MoS2 devices to humid, oxidizing, and high-temperature environments, surpassing the devices with other kinds of electrodes.


Abstract

Nanoscale electronic devices that can work in harsh environments are in high demand for wearable, automotive, and aerospace electronics. Clean and defect-free interfaces are of vital importance for building nanoscale harsh-environment-resistant devices. However, current nanoscale devices are subject to failure in these environments, especially at defective electrode–channel interfaces. Here, harsh-environment-resistant MoS2 transistors are developed by engineering electrode–channel interfaces with an all-transfer of van der Waals electrodes. The delivered defect-free, graphene-buffered electrodes keep the electrode–channel interfaces intact and robust. As a result, the as-fabricated MoS2 devices have reduced Schottky barrier heights, leading to a very large on-state current and high carrier mobility. More importantly, the defect-free, hydrophobic graphene buffer layer prevents metal diffusion from the electrodes to MoS2 and the intercalation of water molecules at the electrode–MoS2 interfaces. This enables high resistances of MoS2 devices with all-transfer electrodes to various harsh environments, including humid, oxidizing, and high-temperature environments, surpassing the devices with other kinds of electrodes. The work deepens the understanding of the roles of electrode–channel interfaces in nanoscale devices and provides a promising interface engineering strategy to build nanoscale harsh-environment-resistant devices.

30 Jan 09:15

Evidence of frustrated magnetic interactions in a Wigner–Mott insulator

by Yanhao Tang

Nature Nanotechnology, Published online: 16 January 2023; doi:10.1038/s41565-022-01309-8

Electrons in two-dimensional semiconductor moiré materials experience competing magnetic interactions. Magneto-optical measurements of moiré devices with controlled screening of the Coulomb interactions now evidence a Wigner–Mott insulating state with frustrated magnetic interactions.
30 Jan 09:15

Electrochemically modulated interaction of MXenes with microwaves

by Meikang Han

Nature Nanotechnology, Published online: 16 January 2023; doi:10.1038/s41565-022-01308-9

Modulating the interaction of a thin film with microwaves is realized using the electrochemical behaviours of various MXenes.
13 Jan 06:22

[ASAP] Highly Tunable Lateral Homojunction Formed in Two-Dimensional Layered CuInP2S6 via In-Plane Ionic Migration

by Huanfeng Zhu, Jialin Li, Qiang Chen, Wei Tang, Xinyi Fan, Fan Li, and Linjun Li

TOC Graphic

ACS Nano
DOI: 10.1021/acsnano.2c09280
13 Jan 06:22

[ASAP] Critical Role of Surface Termination of Sapphire Substrates in Crystallographic Epitaxial Growth of MoS2 Using Inorganic Molecular Precursors

by Younghee Park, Chaehyeon Ahn, Jong-Guk Ahn, Jee Hyeon Kim, Jaehoon Jung, Juseung Oh, Sunmin Ryu, Soyoung Kim, Seung Cheol Kim, Taewoong Kim, and Hyunseob Lim

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ACS Nano
DOI: 10.1021/acsnano.2c08983
13 Jan 06:22

Exciton density waves in Coulomb-coupled dual moiré lattices

by Yihang Zeng

Nature Materials, Published online: 12 January 2023; doi:10.1038/s41563-022-01454-4

The realization of strongly correlated bosons in a solid-state lattice is challenging. Here, the authors trap interlayer excitons in an angle-aligned WS2/bilayer WSe2/WS2 multilayer moiré lattice and observe correlated insulating states.
13 Jan 06:18

[ASAP] Stability and Strength of Monolayer Polymeric C60

by Bo Peng

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Nano Letters
DOI: 10.1021/acs.nanolett.2c04497
13 Jan 06:18

[ASAP] Spontaneous Biskyrmion Lattice in a Centrosymmetric Rhombohedral Rare-Earth Magnet with Easy-Plane Anisotropy

by Shulan Zuo, Kaiming Qiao, Ying Zhang, Tongyun Zhao, Chengbao Jiang, and Baogen Shen

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Nano Letters
DOI: 10.1021/acs.nanolett.2c04001
13 Jan 05:47

A Machine‐Learning‐Based Approach for Solving Atomic Structures of Nanomaterials Combining Pair Distribution Functions with Density Functional Theory

by Magnus Kløve, Sanna Sommer, Bo B. Iversen, Bjørk Hammer, Wilke Dononelli
A Machine-Learning-Based Approach for Solving Atomic Structures of Nanomaterials Combining Pair Distribution Functions with Density Functional Theory

Determination of crystal structures of nanocrystalline compounds is a great challenge in solid-state chemistry. In this work, an algorithm is introduced, which is able to determine the crystal structure of an unknown compound by means of an on-the-fly trained machine learning model that combines density functional calculations with comparison of calculated and measured pair distribution functions for global optimization.


Abstract

Determination of crystal structures of nanocrystalline or amorphous compounds is a great challenge in solid-state chemistry and physics. Pair distribution function (PDF) analysis of X-ray or neutron total scattering data has proven to be a key element in tackling this challenge. However, in most cases, a reliable structural motif is needed as a starting configuration for structure refinements. Here, an algorithm that is able to determine the crystal structure of an unknown compound by means of an on-the-fly trained machine learning model, which combines density functional theory calculations with comparison of calculated and measured PDFs for global optimization in an artificial landscape, is presented. Due to the nature of this landscape, even metastable configurations and stacking disorders can be identified.