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At least 55 records · Page 3

Enriching 2D transition metal borides via MB XMenes (M = Fe, Co, Ir): Strong correlation and magnetism

Recently, two-dimensional (2D) FeSe-like anti-MXenes (or XMenes), composed of late d-block transition metal M and p-block nonmetal X elements, have been both experimentally and theoretically investigated. Here, we select three 2D borides FeB, CoB and IrB for a deeper investigation by including strong correlation effects, as a fertile ground for understanding and applications. Using a combination of Hubbard corrected first-principles calculations and Monte Carlo simulations, FeB and CoB are found to be ferro- and anti-ferro magnetic, contrasting with the non-magnetic nature of IrB. The metallic FeB XMene monolayer, superior to most of the MXenes or MBenes, exhibits robust ferromagnetism, driven by intertwined direct-exchange and super-exchange interactions between adjacent Fe atoms. The predicted Curie temperature ($T$ C ) of the FeB monolayer via the Heisenberg model reaches an impressive 425 K, with the easy-axis oriented out-of-plane and high magnetic anisotropic energy (MAE). The asymmetry in the spin-resolved transmission spectrum induces a thermal spin current, providing an opportunity for spin filtration. In conclusion, this novel 2D FeB material is expected to hold great promise as an information storage medium and find applications in emerging spintronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Percolative phase transition in few-layered MoSe 2 field-effect transistors using Co and Cr contacts

The metal-to-insulator phase transition (MIT) in two-dimensional (2D) materials under the influence of a gating electric field has revealed interesting electronic behavior and the need for a deeper fundamental understanding of electron transport processes, while attracting much interest in the development of next-generation electronic and optoelectronic devices. Although the mechanism of the MIT in 2D semiconductors is a topic under debate in condensed matter physics, our work demonstrates the tunable percolative phase transition in few-layered MoSe 2 field-effect transistors (FETs) using different metallic contact materials. Here, we attempted to understand the MIT through temperature-dependent electronic transport measurements by tuning the carrier density in a MoSe 2 channel under the influence of an applied gate voltage. In particular, we have examined this phenomenon using the conventional chromium (Cr) and ferromagnetic cobalt (Co) as two metal contacts. For both Cr and Co, our devices demonstrated n-type behavior with a room-temperature field-effect mobility of 16 cm 2 V −1 s −1 for the device with Cr-contacts and 92 cm 2 V −1 s −1 for the device with Co-contacts, respectively. Further, with low temperature measurements at 50 K, the mobilities increased significantly to 65 cm 2 V −1 s −1 for the device with Cr and 394 cm 2 V −1 s −1 for the device with Co-contacts. By fitting our experimental data to the percolative phase transition theory, the temperature-dependent conductivity data show a transition from an insulating-to-metallic behavior at a bias of ∼28 V for Cr-contacts and ∼20 V for Co-contacts. This cross-over of the conductivity can be attributed to an increase in carrier density as a function of the gate bias in temperature-dependent transfer characteristics. By extracting the critical exponents, we find that the transport behavior in the device with Co-contacts aligns closely with the 2D percolation theory. In contrast, the devices with Cr-contacts deviate significantly from the 2D limit at low temperatures.

36 MATERIALS SCIENCE↗

Mesoscale Magnetostructural Phase Separation in Fe‐deficient Fe 5 GeTe 2

Two-dimensional van der Waals ferromagnet Fe 5-x GeTe 2 (F5GT) is promising for spintronic applications due to its high Curie temperature, layered structure, and ability to host complex magnetic textures. However, the origin of its sample-dependent magnetic anisotropy remains unclear, hindering control of its magnetic behavior. Here, we use spatially resolved cryogenic scanning transmission electron microscopy (STEM) to correlatively map magnetism, lattice structure, and chemistry across atomic-to-micron scales. We reveal that only mesoscale, not nanoscale, inclusions of a Fe-deficient secondary phase significantly modify magnetic behavior, establishing a previously unrecognized critical length scale. This phase separation, induced by quenching, leads to in-plane magnetic anisotropy, while slow cooling confines separation to a few nanometers and preserves out-of-plane anisotropy. These findings reconcile prior inconsistencies and establish a predictive framework for tuning magnetism in F5GT through thermal processing, with broader implications for controlling anisotropy in other two-dimensional magnetic materials.

2D ferromagnets↗

Mechanical, electronic, optical, piezoelectric and ferroic properties of strained graphene and other strained monolayers and multilayers: an update

Abstract This is an update of a previous review (Naumis et al 2017 Rep. Prog. Phys. 80 096501). Experimental and theoretical advances for straining graphene and other metallic, insulating, ferroelectric, ferroelastic, ferromagnetic and multiferroic 2D materials were considered. We surveyed (i) methods to induce valley and sublattice polarisation ( P ) in graphene, (ii) time-dependent strain and its impact on graphene’s electronic properties, (iii) the role of local and global strain on superconductivity and other highly correlated and/or topological phases of graphene, (iv) inducing polarisation P on hexagonal boron nitride monolayers via strain, (v) modifying the optoelectronic properties of transition metal dichalcogenide monolayers through strain, (vi) ferroic 2D materials with intrinsic elastic ( σ ), electric ( P ) and magnetic ( M ) polarisation under strain, as well as incipient 2D multiferroics and (vii) moiré bilayers exhibiting flat electronic bands and exotic quantum phase diagrams, and other bilayer or few-layer systems exhibiting ferroic orders tunable by rotations and shear strain. The update features the experimental realisations of a tunable two-dimensional Quantum Spin Hall effect in germanene, of elemental 2D ferroelectric bismuth, and 2D multiferroic NiI 2 . The document was structured for a discussion of effects taking place in monolayers first, followed by discussions concerning bilayers and few-layers, and it represents an up-to-date overview of exciting and newest developments on the fast-paced field of 2D materials.

Physics↗

Quantum octets in high mobility pentagonal two-dimensional PdSe 2

Two-dimensional (2D) materials have drawn immense interests in scientific and technological communities, owing to their extraordinary properties and their tunability by gating, proximity, strain and external fields. For electronic applications, an ideal 2D material would have high mobility, air stability, sizable band gap, and be compatible with large scale synthesis. Here we demonstrate air stable field effect transistors using atomically thin few-layer PdSe 2 sheets that are sandwiched between hexagonal BN (hBN), with large saturation current > 350 μA/μm, and high field effect mobilities of ~ 700 and 10,000 cm 2 /Vs at 300 K and 2 K, respectively. At low temperatures, magnetotransport studies reveal unique octets in quantum oscillations that persist at all densities, arising from 2-fold spin and 4-fold valley degeneracies, which can be broken by in-plane and out-of-plane magnetic fields toward quantum Hall spin and orbital ferromagnetism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interplay of electronic structure, magnetism, strain, and defects in carbide $\mathrm{MX}$enes

We report the two-dimensional (2D) magnetic and semiconducting materials, including carbide MXenes, are in high demand for magneto-electronic devices and applications. Here, we report a first-principles study of electronic structure and magnetism of a Ti 2 C MXene, its derivatives Ti 2 CT 2 (T = -F, -O, -OH, -H), and the effect of single vacancy defects (25% C, 12.5% O, and 12.5% and 5.5% Ti) and transition metal (V, Cr, Mn, and Co) dopings. The MAX phase Ti 2 AlC is a non-magnetic (NM) metal which upon removal of Al layer forms a pristine Ti 2 C MXene with A-type antiferromagnetic (AFM) semiconductor having reliable transition temperature (T N = 41K) predicted by the Heisenberg model. All the functionalized MXenes are stable as NM metal except for Ti 2 CO 2 which remains semiconducting with NM ground state. The significant effect of spin–orbit coupling (SOC) is evident in the band structure forming Dirac-like cones and band inversions near the Fermi level. Depending upon the type of vacancy defects Ti 2 CO 2 is NM metal and ferromagnetic (FM) metal. The transition metal (TM) doped MXenes fulfill FM Stoner criterion. The V- and Co-doped MXenes are metals, whereas Cr- and Mn-doped are half-metal and semiconductor.

2D magnetism↗

Spin–Phonon Coupling in Ferromagnetic Monolayer Chromium Tribromide

Novel 2D magnets exhibit intrinsic electrically tunable magnetism down to the monolayer limit, which has significant value for nonvolatile memory and emerging computing device applications. In these compounds, spin–phonon coupling (SPC) typically plays a crucial role in magnetic fluctuations, magnon dissipation, and ultimately establishing long-range ferromagnetic order. However, a systematic understanding of SPC in 2D magnets that combines theory and experiment is still lacking. Here in this work, monolayer chromium tribromide is studied to investigate SPC in 2D magnets via Raman spectroscopy and first principle calculations. The experimental Curie temperature and phonon shifts are found to be in good agreement with the numerical simulations. Specifically, it is demonstrated how magnetic exchange interactions affect phonon vibrations, which helps establish design fundamentals for 2D magnetic materials and other related devices.

36 MATERIALS SCIENCE↗

Novel self-assembled two-dimensional layered oxide structure incorporated with Au nanoinclusions towards multifunctionalities

Two-dimensional (2D) layered oxides have recently attracted wide attention owing to the strong coupling among charges, spins, lattice, and strain, which allows great flexibility and opportunities in structure designs as well as multifunctionality exploration. In parallel, plasmonic hybrid nanostructures exhibit exotic localized surface plasmon resonance (LSPR) providing a broad range of applications in nanophotonic devices and sensors. A hybrid material platform combining the unique multifunctional 2D layered oxides and plasmonic nanostructures brings optical tuning into the new level. Here, a novel self-assembled Bi 2 MoO 6 (BMO) 2D layered oxide incorporated with plasmonic Au nanoinclusions has been demonstrated via one-step pulsed laser deposition (PLD) technique. Comprehensive microstructural characterizations, including scanning transmission electron microscopy (STEM), differential phase contrast imaging (DPC), and STEM tomography, have demonstrated the high epitaxial quality and particle-in-matrix morphology of the BMO-Au nanocomposite film. DPC-STEM imaging clarifies the magnetic domain structures of BMO matrix. Three different BMO structures including layered supercell (LSC) and superlattices have been revealed which is attributed to the variable strain states throughout the BMO-Au film. Owing to the combination of plasmonic Au and layered structure of BMO, the nanocomposite film exhibits a typical LSPR in visible wavelength region and strong anisotropy in terms of its optical and ferromagnetic properties. This study opens a new avenue for developing novel 2D layered complex oxides incorporated with plasmonic metal or semiconductor phases showing great potential for applications in multifunctional nanoelectronics devices.

36 MATERIALS SCIENCE↗

Short-Range Crystalline Order-Tuned Conductivity in Cr 2 Si 2 Te 6 van der Waals Magnetic Crystals

Two-dimensional magnetic materials (2DMMs) are significant not only for studies on the nature of 2D long-range magnetic order but also for future spintronic devices. Of particular interest are 2DMMs where spins can be manipulated by electrical conduction. Whereas Cr 2 Si 2 Te 6 exhibits magnetic order in few-layer crystals, its large band gap inhibits electronic conduction. Here we show that the defect-induced short-range crystal order in Cr 2 Si 2 Te 6 , on the length scale below 0.6 nm, induces a substantially reduced band gap and robust semiconducting behavior down to 2 K that turns to metallic above 10 GPa. Our results in this work will be helpful in designing conducting states in 2DMMs and call for spin-resolved measurement of the electronic structure in exfoliated ultrathin crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Writing and Detecting Topological Charges in Exfoliated Fe 5– x GeTe 2

Fe 5–x GeTe 2 is a promising two-dimensional (2D) van der Waals (vdW) magnet for practical applications, given its magnetic properties. These include Curie temperatures above room temperature, and topological spin textures–TST (both merons and skyrmions), responsible for a pronounced anomalous Hall effect (AHE) and its topological counterpart (THE), which can be harvested for spintronics. Here, we show that both the AHE and THE can be amplified considerably by just adjusting the thickness of exfoliated Fe 5–x GeTe 2 , with THE becoming observable even in zero magnetic field due to a field-induced unbalance in topological charges. Using a complementary suite of techniques, including electronic transport, Lorentz transmission electron microscopy, and micromagnetic simulations, we reveal the emergence of substantial coercive fields upon exfoliation, which are absent in the bulk, implying thickness-dependent magnetic interactions that affect the TST. We detected a “magic” thickness t ≈ 30 nm where the formation of TST is maximized, inducing large magnitudes for the topological charge density (~6.45 × 10 20 cm –2 ), and the concomitant anomalous (ρ xy A,max ≃22.6 μΩ cm) and topological (ρ xy u,T 1≃5 μΩ cm) Hall resistivities at T ≈ 120 K. These values for ρ xy A,max and ρ xy u,T are higher than those found in magnetic topological insulators and, so far, the largest reported for 2D magnets. Furthermore, the hitherto unobserved THE under zero magnetic field could provide a platform for the writing and electrical detection of TST aiming at energy-efficient devices based on vdW ferromagnets.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Computational discovery of two-dimensional rare-earth iodides: promising ferrovalley materials for valleytronics

Two-dimensional Ferrovalley materials with intrinsic valley polarization are rare but highly promising for valley-based nonvolatile random access memory and valley filter devices. These ferromagnetic materials exhibit valleys at or near the Fermi level with intrinsic magnetism. The strong coupling between magnetism and spin–orbit coupling induces intrinsic valley polarization. Using Kinetically Limited Minimization, an unconstrained crystal structure prediction algorithm, and prototype sampling based on first-principles calculations, we have discovered new Ferrovalley materials, rare-earth iodides RI 2 , where R is a rare-earth element belonging to Sc, Y, or La-Lu, and I is Iodine. The rare-earth iodides are layered and demonstrate either 2H, 1T, or 1T d phase as the ground state in bulk, analogous to transition metal dichalcogenides (TMDCs). The calculated exfoliation energy of monolayers (MLs) is comparable to that of graphene and TMDCs, suggesting possible experimental synthesis. The MLs in the 2H phase exhibit ferromagnetism due to unpaired electrons in d and f orbitals. Throughout the rare-earth series, d bands have valley polarization at K and $\overline{K}$ points in the Brillouin zone in the vicinity of the Fermi level. Large intrinsic valley polarization in the range of 15–143 meV without external stimuli is observed in these Ferrovalley materials, which can be enhanced further by applying an in-plane bi-axial strain. These valleys can selectively be probed and manipulated for information storage and processing, potentially offering superior performance beyond conventional electronics and spintronics. Here we further show that the 2H ferromagnetic phase of RI 2 MLs possesses non-zero Berry curvature and exhibits anomalous valley Hall effect with considerable anomalous Hall conductivity. Our work will incite exploratory synthesis of the predicted Ferrovalley materials and their application in valleytronics and beyond.

2D materials↗

Lithiation bridged molecular conducting magnets

Combining ferromagnetism and metallic conductivity has been extensively studied in contemporary materials science. However, building such multifunctionalities in molecular chemistry is particularly challenging, on which two collective properties are long considered as mutually exclusive. Here, we report molecular conducting magnet consisting of two-dimensional graphene and molecular planar magnetic networks bridged by electrochemical lithiation, exhibiting the co-existence of distinct magnetism and conductivity and magneto-electric coupling effects. Here, the room temperature magnetoresistance and magnetoelectric coupling coefficient of such complex solid reach 10.7% and 1.77 V/Oe cm, respectively, which can be further tailored by modulating the interaction between graphene and molecular magnetic network. In addition, the graphene passivation simultaneously introduces environmental stability of molecular mag-nets. The electrochemical lithiation offers a pathway towards coupling magnetism and conductivity in molecular complexes.

2D organic complexes↗

Spin–Phonon Coupling and Magnetic Transition in an Organic Molecule Intercalated Cr 2 Ge 2 Te 6

The manipulation of spin–phonon coupling in both formations and explorations of magnetism in two-dimensional van der Waals ferromagnetic semiconductors facilitates unprecedented prospects for spintronic devices. The interlayer engineering with spin–phonon coupling promises controllable magnetism via organic cation intercalation. Here, in this study, spectroscopic evidence reveals the intercalation effect on the intrinsic magnetic and electronic transitions in quasi-two-dimensional Cr 2 Ge 2 Te 6 using tetrabutyl ammonium (TBA + ) as the intercalant. The temperature evolution of Raman modes, E g 3 and A g 1 , along with the magnetization measurements, unambiguously captures the enhancement of the ferromagnetic Curie temperature in the intercalated heterostructure. Moreover, the E g 4 mode highlights the increased effect of spin–phonon interaction in magnetic-order-induced lattice distortion. Combined with the first-principle calculations, we observed a substantial number of electrons transferred from TBA + to Cr through the interface. The interplay between spin–phonon coupling and magnetic ordering in van der Waals magnets appeals for further understanding of the manipulation of magnetism in layered heterostructures.

2D magnet↗

ZrTe2/CrTe2: an epitaxial van der Waals platform for spintronics

Abstract The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2D ferromagnet (1T-CrTe 2 ) and a topological semimetal (ZrTe 2 ). We find that one unit-cell (u.c.) thick 1T-CrTe 2 grown epitaxially on ZrTe 2 is a 2D ferromagnet with a clear anomalous Hall effect. In thicker samples (12 u.c. thick CrTe 2 ), the anomalous Hall effect has characteristics that may arise from real-space Berry curvature. Finally, in ultrathin CrTe 2 (3 u.c. thickness), we demonstrate current-driven magnetization switching in a full vdW topological semimetal/2D ferromagnet heterostructure device.

36 MATERIALS SCIENCE↗

Emergence of electric-field-tunable interfacial ferromagnetism in 2D antiferromagnet heterostructures

Van der Waals (vdW) magnet heterostructures have emerged as new platforms to explore exotic magnetic orders and quantum phenomena. Here, we study heterostructures of layered antiferromagnets, CrI 3 and CrCl 3 , with perpendicular and in-plane magnetic anisotropy, respectively. Using magneto-optical Kerr effect microscopy, we demonstrate out-of-plane magnetic order in the CrCl 3 layer proximal to CrI 3 , with ferromagnetic interfacial coupling between the two. Such an interlayer exchange field leads to higher critical temperature than that of either CrI 3 or CrCl 3 alone. We further demonstrate significant electric-field control of the coercivity, attributed to the naturally broken structural inversion symmetry of the heterostructure allowing unprecedented direct coupling between electric field and interfacial magnetism. These findings illustrate the opportunity to explore exotic magnetic phases and engineer spintronic devices in vdW heterostructures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Tuning of the magnetotransport properties of a spin-polarized 2D electron system using visible light

We report on the effects of visible light on the low temperature electronic properties of the spin-polarized two dimensional electron system (2DES) formed at the interfaces between LaAlO 3 , EuTiO 3 and (001) SrTiO 3 . A strong, persistent modulation of both longitudinal and transverse conductivity was obtained using light emitting diodes (LEDs) with emissions at different wavelengths in the visible spectrum range. In particular, Hall effect data show that visible light induces a non-volatile electron filling of bands with mainly 3 dxz,yz character, and at the same time an enhancement of the anomalous Hall effect associated to the magnetic properties of the system. Accordingly, a suppression of the weak-anti localization corrections to the magneto-conductance is found, which correlates with an enhancement of the spin-polarization and of the ferromagnetic character of 2DES. The results establish the LED-induced photo-doping as a viable route for the control of the ground state properties of artificial spin-polarized oxide 2DES.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic properties of intercalated quasi-2D Fe 3-x GeTe 2 van der Waals magnet

Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe 3-x GeTe 2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (T C ~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the T C remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a room temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into quasi-2D FGT. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements, in combination with vdW-corrected ab initio calculations, suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner and has the potential to be extended to bilayer and few-layer vdW magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Effects of thin metal contacts on few-layer van der Waals ferrielectric CuInP 2 S 6

Out-of-plane polarized ferroelectric materials in a capacitive structure provide a key component for several technological applications. Furthermore, two-dimensional materials are expected to aid in the quest for both ultrathin and flexible electronics. Of the various two-dimensional ferroelectrics with out-of-plane polarization, CuInP 2 S 6 is special in that the Cu atoms are highly mobile and it has been shown to possess both low- and high-polarization states. Here, using density-functional-theory calculations, we explore the stabilization of the ferroelectric state for several prototypical metal contacts (Gr, Ni, Cu, Au, and Ag). In all cases, we find that the ferroelectric state can be stabilized at fewer layers than in the freestanding case. For all of the considered conventional metal contacts, we also find the existence of a quasi-ferroelectric state that stabilizes a polar phase for thicknesses greater than two layers of CIPS. In the cases of Au and Ag, interfacial alignment and strain can be used to stabilize ferroelectricity at the bilayer limit. Furthermore, we find that the strength of the interaction between the contact and CuInP 2 S 6 also leads to stabilization of the high-polarization state when ferroelectricity is stabilized. Lastly, energy-barrier calculations show that the system is still switchable in the presence of contact doping from the metal contacts.

2D materials↗