Highlights

Emergence of mixing-induced polymorphic phase with higher mobility in alkylated layered organic semiconductors

Kiyoshi Nikaido, Satoru Inoue, Seiji Tsuzuki, Reiji Kumai, Hiroyuki Matsui, Kiyofumi Takaba, Saori Maki-Yonekura, Koji Yonekura, and Tatsuo Hasegawa

Phys. Rev. Materials 8, 115601 (2024) - Published 1 November, 2024

The fabrication of functional layers with desired molecular ordering is a fundamental challenge in organic electronic materials. In this study, the authors demonstrate that the layered crystalline order of alkylated organic semiconductors can be precisely controlled by mixing molecules with varying alkyl chain lengths, resulting in a nearly tenfold enhancement in hole mobility compared to the parent materials. Advanced structural analysis using electron diffraction reveals that the crystal structure of the mixing-induced phase is stabilized by alkyl chain interdigitation between molecular layers. This discovery presents a novel approach to structural control that does not rely solely on the development of new organic semiconductor molecules.

Characterizing the chemical potential disorder in the topological insulator (Bi1−xSbx)2Te3 thin films

Jens Brede, Mahasweta Bagchi, Adrian Greichgauer, Anjana Uday, Andrea Bliesener, Gertjan Lippertz, Roozbeh Yazdanpanah, Alexey Taskin, and Yoichi Ando

Phys. Rev. Materials 8, 104202 (2024) - Published 29 October, 2024

Compensation doping is a successful strategy to realize bulk-insulating topological insulators, but it comes at the cost of large chemical-potential fluctuations. Here, STM is used to map these fluctuations in (Bi1−xSbx)2Te3 thin films with varying Sb-concentration x. The fluctuation amplitude is found to be 5 – 14 meV in quasi-bulk-insulating films, but it increases to 30 – 40 meV in highly bulk-insulating films. Landau-level spectroscopy under perpendicular magnetic fields allows for identifying the Dirac point. At x ≈ 0.65, the Fermi level is found to lie within 10 meV from the Dirac point and yet the potential fluctuations are relatively modest at 14 meV.

Probing enhanced superconductivity in van der Waals polytypes of VxTaS2

Wojciech R. Pudelko, Huanlong Liu, Francesco Petocchi, Hang Li, Eduardo Bonini Guedes, Julia Küspert, Karin von Arx, Qisi Wang, Ron Cohn Wagner, Craig M. Polley, Mats Leandersson, Jacek Osiecki, Balasubramanian Thiagarajan, Milan Radović, Philipp Werner, Andreas Schilling, Johan Chang, and Nicholas C. Plumb

Phys. Rev. Materials 8, 104802 (2024) - Published 25 October, 2024

Interfacing different layer types of 2D materials is a promising route for developing quantum devices and exploring the fundamental physics of complex matter. In this work, the authors employ angle-resolved photoemission spectroscopy to elucidate the factors behind a strong enhancement of superconductivity that occurs when insulating 1T structural layers of the compound TaS2 are inserted between layers of its superconducting 2H polymorph, forming new bulk structures, such as the 4Hb polytype. Using a novel synthesis approach — vanadium intercalation — they demonstrate how the intercalant acts as a chemical knob, enabling precise manipulation of the material’s structural configurations. From detailed analysis of the spectral signatures of many-body interactions, the study reveals a substantial and highly momentum-dependent boost in electron-phonon coupling in the 4Hb phase, which is found to account for the elevated transition temperature.

Optically resolved exchange splittings in the doped van der Waals ferromagnet CrBr3:Yb3+

Thom J. Snoeren, Kimo Pressler, and Daniel R. Gamelin

Phys. Rev. Materials 8, 104410 (2024) - Published 23 October, 2024

The use of impurities to generate new properties in magnetic CrX3 compounds remains surprisingly underexplored. The authors report the magneto-optical properties of Yb3+-doped CrBr3, in which Yb3+ serves as a spin-bearing optical point defect. Their data reveal that ground- and excited-state Yb3+ spin degeneracies are spontaneously lifted through strong magnetic exchange with neighboring Cr3+ ions, such that individual Yb3+ spin transitions are resolved even at zero external field, and Yb3+ spins are easily manipulated via CrBr3 magnetization. The large Yb3+ spin splittings present unique opportunities for optical spin manipulation of point defects and highlight the use of impurities to add spin-photonic functionalities to this classic 2D van der Waals magnet.

Stretch-inactivated ion transport through subnanoporous two-dimensional membranes

Yechan Noh and Alex Smolyanitsky

Phys. Rev. Materials 8, L103001 (2024) - Published 3 October, 2024

Aqueous ions permeate subnanoscale pores in two-dimensional materials by leaping local energy barriers, not through simple diffusion. Depending on the local ion-pore and ion-solvent interactions, seemingly non-intuitive behaviors can arise. The authors combine molecular dynamics simulations, quantum-chemical calculations, and kinetic theory to demonstrate that electrostatically driven flow of aqueous alkali cations through subnanoscale pores can be inactivated by stretching the two-dimensional membrane hosting the pores. More specifically, they show that potassium transport significantly decreases in response to moderate membrane strain, while sodium transport increases. This behavior is attributed to a clearly observed strain-induced repulsive-to-attractive transition in the ion-pore electrostatic interactions.

Enhanced magnetization by defect-assisted exciton recombination in atomically thin CrCl3

Xin-Yue Zhang, Thomas K. M. Graham, Hyeonhu Bae, Yu-Xuan Wang, Nazar Delegan, Jonghoon Ahn, Zhi-Cheng Wang, Jakub Regner, Kenji Watanabe, Takashi Taniguchi, Minkyung Jung, Zdeněk Sofer, Fazel Tafti, David D. Awschalom, F. Joseph Heremans, Binghai Yan, and Brian B. Zhou

Phys. Rev. Materials 8, 104402 (2024) - Published 1 October, 2024

Optically controlled magnetism offers prospects for high efficiency information processing, but such investigations are often restricted to magnets with special readout properties. Here, the authors utilize nitrogen-vacancy (NV) center magnetometry to directly image the transient, photoinduced stray fields in a material proximal to the NV center. They discover that the antiferromagnetic layer magnetization in atomically thin CrCl3 is enhanced by exciton pumping, which they attribute to a charge transfer between water-related surface adsorbates and the spin-polarized conduction band during nonradiative exciton recombination. Their work demonstrates how defects can enhance 2D magnetism and broadens the study of photoinduced magnetic effects.

Magnetic compensation in Mn4−xCuxN films on SrTiO3(001) with noncollinear magnetic structures

Aoi Hatate, Tomohiro Yasuda, Kenta Amemiya, and Takashi Suemasu

Phys. Rev. Materials 8, L091403 (2024) - Published 25 September, 2024

Mn4N films are promising materials for ultrafast magnetization control via spin currents. Previous studies have shown that adding magnetic elements such as Ni or Co to these films induces magnetization compensation (MC) at room temperature. The authors now demonstrate that ferrimagnetic Mn4N films can also achieve MC at room temperature with a small addition of Cu, marking the first instance of MC being induced by doping with a non-magnetic element. X-ray magnetic circular dichroism and magnetization measurements further reveal that the magnetic structure of Cu-doped Mn4N films differs from that of their Ni- or Co-doped counterparts.

Topological Hall effect induced by chiral fluctuations in ErMn6Sn6

Kyle Fruhling, Alenna Streeter, Sougata Mardanya, Xiaoping Wang, Priya Baral, Oksana Zaharko, Igor I. Mazin, Sugata Chowdhury, William D. Ratcliff, and Fazel Tafti

Phys. Rev. Materials 8, 094411 (2024) - Published 24 September, 2024

The topological Hall effect can emerge in a material either statically due to the formation of skyrmions or dynamically due to thermal fluctuations. ErMn6Sn6 undergoes a field-induced ferrimagnetic to antiferromagnetic phase transition. At the boundary of this phase transition there is an intermediate phase which is predicted to provide the right environment for the emergence of a significant dynamic topological Hall effect. Therefore, ErMn6Sn6 provides a testbed to investigate the universality of thermal fluctuations as a mechanism of the topological Hall effect.

Impact of grain boundary energy anisotropy on grain growth

S. Kiana Naghibzadeh, Zipeng Xu, David Kinderlehrer, Robert Suter, Kaushik Dayal, and Gregory S. Rohrer

Phys. Rev. Materials 8, 093403 (2024) - Published 19 September, 2024

Recent observations of microstructure evolution during annealing revealed that grain growth not only reduces grain boundary area but also dissipates additional energy through a decrease in average grain boundary energy—a feature that isotropic simulations with uniform energy assumption fail to predict. The authors use a threshold dynamics model incorporating anisotropic grain boundary energies to simulate the observed grain growth of polycrystalline Ni. The model predicts an increase in the relative area of low-energy twin boundaries and a decrease in average boundary energy. This study highlights that realistic simulation of grain growth in polycrystals requires anisotropic grain boundary energy implementation.

Intrinsic origins of broad luminescence in melt-grown ZnGa2O4 single crystals

Ymir K. Frodason, Augustinas Galeckas, Vegard S. Olsen, Philip M. Weiser, Zbigniew Galazka, Chris G. Van de Walle, and Lasse Vines

Phys. Rev. Materials 8, 094604 (2024) - Published 18 September, 2024

The authors present a detailed theoretical study of the optical behavior of native defects in zinc gallium oxide based on configuration coordinate diagrams derived from hybrid functional calculations. The resulting predicted luminescence lines are compared with low-temperature photoluminescence spectra measured on zinc gallium oxide single crystals grown from the melt. Based on this comparison, self-trapped holes, Zn antisites, Zn vacancies, and their complexes with Ga antisites are put forward as potential origins of the observed luminescence.

High mobility charge transport in a multicarrier altermagnet CrSb

Takahiro Urata, Wataru Hattori, and Hiroshi Ikuta

Phys. Rev. Materials 8, 084412 (2024) - Published 29 August, 2024

Altermagnets are unconventional type of magnetic materials with intriguing properties. CrSb is particularly important because of its high ordering temperature and large spin-splitting energy. Here, the authors measured the magnetotransport properties of CrSb. Employing focused-ion-beam machining, they prepared micro-sized lamellar samples to measure all independent Hall tensor components. The Hall resistivity was highly non-linear at low temperatures, but an anomalous Hall effect was ruled out by symmetry-based considerations. Instead, the magnetotransport properties are well explained by a multicarrier effect. Notably, the analysis revealed the presence of carriers with the highest mobility reported for altermagnets so far.

Single crystal growth, chemical defects, magnetic and transport properties of antiferromagnetic topological insulators (Ge1−δ−xMnx)2Bi2Te5 (x≤0.47, 0.11≤δ≤0.20)

Tiema Qian, Chaowei Hu, J. Green, Erxi Feng, Huibo Cao, and Ni Ni

Phys. Rev. Materials 8, 084203 (2024) - Published 27 August, 2024

To explore new magnetic topological insulators, the authors grew high quality single crystals of (Ge1−δ−xMnx)2Bi2Te5 (GeMn225) (x ≤ 0.47, 0.11 ≤ δ ≤ 0.20) by flux and chemical vapor transport methods. Elemental analysis and diffraction data reveal Ge/Bi site mixing and Ge vacancies, with Mn atoms occupying the inner two layers. The x=0.47 sample exhibits bilayer A-type antiferromagnetism with the easy axis along the c-axis below 10.8 K. Compared to MnBi2Te4, it shows enhanced effective interlayer AFM exchange and much reduced uniaxial anisotropy. This study highlights the potential of these materials for investigating emergent phenomena, including the layer Hall and quantum metric nonlinear Hall effects.

Differing vibrational properties of halide and chalcogenide perovskite semiconductors and impact on optoelectronic performance

Kevin Ye, Matan Menahem, Tommaso Salzillo, Florian Knoop, Boyang Zhao, Shanyuan Niu, Olle Hellman, Jayakanth Ravichandran, R. Jaramillo, and Omer Yaffe

Phys. Rev. Materials 8, 085402 (2024) - Published 20 August, 2024

There is motivation to develop materials with photovoltaic performance comparable to halide perovskites but without the drawbacks of instability and toxicity. Chalcogenide perovskites are interesting because they have a tunable direct band gap and are very stable, but their optoelectronic properties are not yet well understood. This study of Raman and photoluminescence spectroscopy of BaZrS3 and CsPbBr3 single-crystal samples reveals differences in their vibrational properties and explores how these differences affect nonradiative recombination rates. The results suggest that the usefulness of chalcogenide perovskites for photovoltaics will hinge on continued progress in defect control.

Direct evidence of induced magnetic moment in Se and the role of misplaced Mn in MnBi2Se4-based intrinsic magnetic topological insulator heterostructures

R. Fukushima, V. N. Antonov, M. M. Otrokov, T. T. Sasaki, R. Akiyama, K. Sumida, K. Ishihara, S. Ichinokura, K. Tanaka, Y. Takeda, D. P. Salinas, S. V. Eremeev, E. V. Chulkov, A. Ernst, and T. Hirahara

Phys. Rev. Materials 8, 084202 (2024) - Published 15 August, 2024

Although intrinsic magnetic topological insulator heterostructures are thought to be an ideal system to examine the interplay of topology and magnetism, unintended disorder can alter their property. In this study, the authors combine atom-resolved characterization as well as theoretical calculation and investigate the structural and magnetic properties of heterostructures formed by MnBi2Se4 and Bi2Se3. They clarify the magnetic coupling between Mn atoms placed at different sites and furthermore, detect a clear magnetic signal in the nonmagnetic element Se, providing direct evidence of its magnetic interaction with Mn. This study highlights the need to examine the magnetism of each atom carefully in these systems.

Deformation and failure of glassy polymer-polymer interfaces compatibilized by linear multiblock copolymers

Ryan P. Collanton and Kevin D. Dorfman

Phys. Rev. Materials 8, 075604 (2024) - Published 16 July, 2024

When two different polymers are blended, they form phase-separated emulsions with weak interfaces. These recycled materials are inferior to the original plastics, posing a fundamental challenge for recycling mixed plastic waste streams. An emerging solution to this problem is the addition of a multiblock copolymer compatibilizer to “stitch together” the interface. Using coarse-grained molecular dynamics simulations, Collanton and Dorfman examined how interfacial toughness is impacted by the number of blocks in the compatibilizer and the copolymer loading, connecting the microstructural features of the interface to its failure mechanism.

Two-step aging dynamics in enzymatic milk gels

Julien Bauland, Gouranga Manna, Thibaut Divoux, and Thomas Gibaud

Phys. Rev. Materials 8, L072601 (2024) - Published 9 July, 2024

In this study, the authors take advantage of the emergence time-resolved mechanical spectroscopy to investigate the formation and aging of enzymatic milk gels, made of soft natural colloids. By coupling rheometric measurements with structural characterizations, they reveal two sequential steps in the aging process. First, the open particulate network rapidly matures into a compact network, increasing gel elasticity and evolving the viscoelastic spectrum. Second, the microstructure “freezes” at a critical time, after which aging proceeds through contact-driven mechanisms. This two-step aging process is crucial for industrial cheese processing and contrasts with the aging of hard particle colloidal gels, where the overall network structure remains constant throughout aging.

Effects of mechanical stress, chemical potential, and coverage on hydrogen solubility during hydrogen-enhanced decohesion of ferritic steel grain boundaries: A first-principles study

Abril Azócar Guzmán and Rebecca Janisch

Phys. Rev. Materials 8, 073601 (2024) - Published 1 July, 2024

Hydrogen embrittlement severely impacts structural materials such as iron and its alloys. This study aims to understand hydrogen-enhanced decohesion in ferritic steel grain boundaries (GBs). Density functional theory calculations are carried out to investigate the influence of H on the decohesion of the Σ5(310)[001] and Σ3(112)[1-10] symmetrical tilt GBs in body-centered cubic (bcc) Fe and Fe+X systems, where X = C, Cr, V, or Mn. The findings indicate that higher local concentrations of hydrogen significantly reduce GB cohesive strength, especially at the Σ5 GB. However, at finite stress, the Σ3 GB becomes more favorable for hydrogen segregation, suggesting hydrogen redistribution due to stresses in the microstructure can enhance hydrogen resistance.

La4Co4X (X=Pb, Bi, Sb): A demonstration of antagonistic pairs as a route to quasi-low-dimensional ternary compounds

Tyler J. Slade, Nao Furukawa, Matthew Dygert, Siham Mohamed, Atreyee Das, Weiyi Xia, Cai-Zhuang Wang, Sergey L. Bud'ko, and Paul C. Canfield

Phys. Rev. Materials 8, 064401 (2024) - Published 3 June, 2024

Low or quasi reduced-dimensional crystal structures are associated with enhanced electronic correlations and emergent quantum behavior. Despite wide interest, identification of new material examples remains restricted by the lack of chemical rules for predicting the structure of extended solids. The authors present the antagonistic pairs approach to discover intermetallic compounds with reduced dimensional structural motifs. By using a pair of strongly immiscible atoms (an antagonistic pair) with a mutually compatible third element, they show that ternary compounds can be formed in which the compatible third element separates the immiscible elements into distinct crystallographic substructures. Quasi-low dimensional structural units, such as sheets, chains, or clusters are the consequence of the immiscible atoms trying to avoid close contact in the solid state. As an example, the authors outline the discovery of La4Co4X (X = Pb, Bi, Sb), a family of intermetallic compounds in which the La separates the highly immiscible Co-Pb or Co-Bi atoms into a quasi-layered structure. They anticipate that their approach is a generalizable design principle for discovering new materials and new structure types containing low-dimensional substructures.

Large spontaneous magneto-thermoelectric effect in epitaxial thin films of the topological kagome ferromagnet Fe3Sn

Shun'ichiro Kurosawa, Tomoya Higo, Shota Saito, Ryota Uesugi, and Satoru Nakatsuji

Phys. Rev. Materials 8, 054206 (2024) - Published 28 May, 2024

This study investigates the anomalous Nernst effect (ANE), a novel technique to convert heat into electricity utilizing the magnetic and topological properties of materials. Unlike the Seebeck effect, ANE employs established thin-film technology to develop practical thermoelectric devices. We have successfully fabricated high-quality (0001)-oriented epitaxial films of the topological kagome ferromagnet Fe3Sn and characterized their thermoelectric properties. These films exhibit a large “zero-field” ANE signal of ~3 µV/K at room temperature due to large magneto-crystalline anisotropy as well as the shape anisotropy for in-plane magnetization arrangements, making them ideal for applications such as heat flux sensors and energy harvesters. This breakthrough in utilizing Fe3Sn films not only advances the understanding of ANE in topological magnets but also paves the way for the design of high-performance thermoelectric devices.

Fermiology and transport properties of the candidate topological crystalline insulator SrAg4Sb2

J. Green, Eve Emmanouilidou, Harry W. T. Morgan, William T. Laderer, Chaowei Hu, Jonathan Loera, Anastassia N. Alexandrova, and Ni Ni

Phys. Rev. Materials 8, 054205 (2024) - Published 23 May, 2024

Inspired by the nonmagnetic topological materials database, the authors investigated the 3D fermiology and band topology of the Topological Crystalline Insulator (TCI) candidate SrAg4Sb2. The fermiology, revealed by angular-dependent quantum oscillations, shows excellent agreement with first-principles calculations. Symmetry and topology analysis result in two potential sets of topological invariants, suggesting the emergence of crystal-symmetry-protected gapless Dirac surface states either on the as-grown ab planes or on both the ab planes and as-grown mirror planes. Their findings provide evidence that SrAg4Sb2 is a promising TCI for exploring topological surface states protected by crystal symmetry.

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