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2.
Nano Lett ; 24(3): 890-896, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38198643

RESUMO

Motivated by the recent developments in moiré superlattices of van der Waals magnets and the desire to control the magnetic interactions of α-RuCl3, here we present a comprehensive theory of the long-range ordered magnetic phases of twisted bilayer α-RuCl3. Using a combination of first-principles calculations and atomistic simulations, we show that the stacking-dependent interlayer exchange gives rise to an array of magnetic phases that can be realized by controlling the twist angle. In particular, we discover a complex hexagonal domain structure in which multiple zigzag orders coexist. This multidomain order minimizes the interlayer energy while enduring the energy cost due to domain wall formation. Further, we show that quantum fluctuations can be enhanced across the phase transitions. Our results indicate that magnetic frustration due to stacking-dependent interlayer exchange in moiré superlattices can be exploited to tune quantum fluctuations and the magnetic ground state of α-RuCl3.

3.
J Am Chem Soc ; 146(6): 3640-3645, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38294831

RESUMO

We report the discovery of a novel form of Ruddlesden-Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase La3Ni2O7 adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO6 octahedra alternate in a "1313" sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imam variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at T ≈ 134 K. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer La3Ni2O7 with Tc as high as 80 K above 14 GPa.

5.
Nat Commun ; 14(1): 1468, 2023 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-36928184

RESUMO

The layered square-planar nickelates, Ndn+1NinO2n+2, are an appealing system to tune the electronic properties of square-planar nickelates via dimensionality; indeed, superconductivity was recently observed in Nd6Ni5O12 thin films. Here, we investigate the role of epitaxial strain in the competing requirements for the synthesis of the n = 3 Ruddlesden-Popper compound, Nd4Ni3O10, and subsequent reduction to the square-planar phase, Nd4Ni3O8. We synthesize our highest quality Nd4Ni3O10 films under compressive strain on LaAlO3 (001), while Nd4Ni3O10 on NdGaO3 (110) exhibits tensile strain-induced rock salt faults but retains bulk-like transport properties. A high density of extended defects forms in Nd4Ni3O10 on SrTiO3 (001). Films reduced on LaAlO3 become insulating and form compressive strain-induced c-axis canting defects, while Nd4Ni3O8 films on NdGaO3 are metallic. This work provides a pathway to the synthesis of Ndn+1NinO2n+2 thin films and sets limits on the ability to strain engineer these compounds via epitaxy.

6.
Sci Rep ; 12(1): 17864, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36284152

RESUMO

We provide a set of computational experiments based on ab initio calculations to elucidate whether a cuprate-like antiferromagnetic insulating state can be present in the phase diagram of the low-valence layered nickelate family (R[Formula: see text]Ni[Formula: see text]O[Formula: see text], R= rare-earth, [Formula: see text]) in proximity to half-filling. It is well established that at [Formula: see text] filling the infinite-layer ([Formula: see text]) nickelate is metallic, in contrast to cuprates wherein an antiferromagnetic insulator is expected. We show that for the Ruddlesden-Popper (RP) reduced phases of the series (finite n) an antiferromagnetic insulating ground state can naturally be obtained instead at [Formula: see text] filling, due to the spacer RO[Formula: see text] fluorite slabs present in their structure that block the c-axis dispersion. In the [Formula: see text] nickelate, the same type of solution can be derived if the off-plane R-Ni coupling is suppressed. We show how this can be achieved if a structural element that cuts off the c-axis dispersion is introduced (i.e. vacuum in a monolayer of RNiO[Formula: see text], or a blocking layer in multilayers formed by (RNiO[Formula: see text])[Formula: see text]/(RNaO[Formula: see text])[Formula: see text]).

7.
Nature ; 602(7898): 601-605, 2022 02.
Artigo em Inglês | MEDLINE | ID: mdl-35197619

RESUMO

Multiferroic materials have attracted wide interest because of their exceptional static1-3 and dynamical4-6 magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization through various mechanisms, such as the spin-current or the inverse Dzyaloshinskii-Moriya effect3,7. This intrinsic coupling between the magnetic and dipolar order parameters results in high-strength magnetoelectric effects3,8. Two-dimensional materials possessing such intrinsic multiferroic properties have been long sought for to enable the harnessing of magnetoelectric coupling in nanoelectronic devices1,9,10. Here we report the discovery of type-II multiferroic order in a single atomic layer of the transition-metal-based van der Waals material NiI2. The multiferroic state of NiI2 is characterized by a proper-screw spin helix with given handedness, which couples to the charge degrees of freedom to produce a chirality-controlled electrical polarization. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Combining birefringence and second-harmonic-generation measurements with theoretical modelling and simulations, we detect a highly anisotropic electronic state that simultaneously breaks three-fold rotational and inversion symmetry, and supports polar order. The evolution of the optical signatures as a function of temperature and layer number surprisingly reveals an ordered magnetic polar state that persists down to the ultrathin limit of monolayer NiI2. These observations establish NiI2 and transition metal dihalides as a new platform for studying emergent multiferroic phenomena, chiral magnetic textures and ferroelectricity in the two-dimensional limit.

8.
Nat Mater ; 21(2): 160-164, 2022 02.
Artigo em Inglês | MEDLINE | ID: mdl-34811494

RESUMO

Since the discovery of high-temperature superconductivity in copper oxide materials1, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials2. One prime materials platform has been the rare-earth nickelates and, indeed, superconductivity was recently discovered in the doped compound Nd0.8Sr0.2NiO2 (ref. 3). Undoped NdNiO2 belongs to a series of layered square-planar nickelates with chemical formula Ndn+1NinO2n+2 and is known as the 'infinite-layer' (n = ∞) nickelate. Here we report the synthesis of the quintuple-layer (n = 5) member of this series, Nd6Ni5O12, in which optimal cuprate-like electron filling (d8.8) is achieved without chemical doping. We observe a superconducting transition beginning at ~13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd6Ni5O12 interpolates between cuprate-like and infinite-layer nickelate-like behaviour. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors that can be tuned via both doping and dimensionality.


Assuntos
Elétrons , Supercondutividade , Temperatura Alta
9.
Adv Mater ; 34(6): e2106222, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34813678

RESUMO

Named after the two-faced Roman god of transitions, transition metal dichalcogenide (TMD) Janus monolayers have two different chalcogen surfaces, inherently breaking the out-of-plane mirror symmetry. The broken mirror symmetry and the resulting potential gradient lead to the emergence of quantum properties such as the Rashba effect and the formation of dipolar excitons. Experimental access to these quantum properties, however, hinges on the ability to produce high-quality 2D Janus monolayers. Here, these results introduce a holistic 2D Janus synthesis technique that allows real-time monitoring of the growth process. This prototype chamber integrates in situ spectroscopy, offering fundamental insights into the structural evolution and growth kinetics, that allow the evaluation and optimization of the quality of Janus monolayers. The versatility of this method is demonstrated by synthesizing and monitoring the conversion of SWSe, SNbSe, and SMoSe Janus monolayers. Deterministic conversion and real-time data collection further aid in conversion of exfoliated TMDs to Janus monolayers and unparalleled exciton linewidth values are reached, compared to the current best standard. The results offer an insight into the process kinetics and aid in the development of new Janus monolayers with high optical quality, which is much needed to access their exotic properties.

10.
Nano Lett ; 21(15): 6633-6639, 2021 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-34339218

RESUMO

We present a comprehensive theory of the magnetic phases in twisted bilayer chromium trihalides through a combination of first-principles calculations and atomistic simulations. We show that the stacking-dependent interlayer exchange leads to an effective moiré field that is mostly ferromagnetic with antiferromagnetic patches. A wide range of noncollinear magnetic phases can be stabilized as a function of the twist angle and Dzyaloshinskii-Moriya interaction as a result of the competing interlayer antiferromagnetic coupling and the energy cost for forming domain walls. In particular, we demonstrate that for small twist angles various skyrmion crystal phases can be stabilized in both CrI3 and CrBr3. Our results provide an interpretation for the recent observation of noncollinear magnetic phases in twisted bilayer CrI3 and demonstrate the possibility of engineering further nontrivial magnetic ground states in twisted bilayer chromium trihalides.

11.
Inorg Chem ; 58(15): 10201-10208, 2019 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-31306005

RESUMO

We report a 2D material, KCu7P3, with a noncentrosymmetric structure (trigonal space group P31m, a = 6.9637(2) Å, c = 24.1338 (10) Å), which forms both from a molten potassium polyphosphide flux and from the elements. This phase consists of infinite [Cu7P3]- layers with hexagonal P sheets separated by K+ ions. The structure of the layers is unique but related to both Cu3P and the CaCu4P2 structure-types. Single-crystal refinement reveals extensive disorder within the Cu3P-like slabs. KCu7P3 is paramagnetic and exhibits a room temperature resistivity of ∼335 µΩ cm with a metal-like temperature dependence. The metallic character is supported by density functional theory electronic structure calculations. Hall and Seebeck effect measurements yield p-type behavior with a hole mobility of ∼15 cm2 V-1 s-1 at 300 K and a carrier concentration on the order of 1021 cm-3. KCu7P3 is chemically stable in ambient conditions, as well as in aqueous neutral and acidic solutions.

12.
J Am Chem Soc ; 140(29): 9193-9202, 2018 07 25.
Artigo em Inglês | MEDLINE | ID: mdl-29947508

RESUMO

We report an order-disorder phase transition in the 2D semiconductor KAg3Se2, which is a dimensionally reduced derivative of 3D Ag2Se. At ∼695 K, the room temperature ß-phase (CsAg3S2 structure type, monoclinic space group C2/ m) transforms to the high temperature α-phase (new structure type, hexagonal space group R3̅ m, a = 4.5638(5) Å, c = 25.4109(6) Å), as revealed by in situ temperature-dependent X-ray diffraction. Significant Ag+ ion disorder accompanies the phase transition, which resembles the low temperature (∼400 K) superionic transition in the 3D parent compound. Ultralow thermal conductivity of ∼0.4 W m-1 K-1 was measured in the "ordered" ß-phase, suggesting anharmonic Ag motion efficiently impedes phonon transport even without extensive disordering. The optical and electronic properties of ß-KAg3Se2 are modified as expected in the context of the dimensional reduction framework. UV-vis spectroscopy shows an optical band gap of ∼1 eV that is indirect in nature as confirmed by electronic structure calculations. Electronic transport measurements on ß-KAg3Se2 yielded n-type behavior with a high electron mobility of ∼400 cm2 V-1 s-1 at 300 K due to a highly disperse conduction band. Our results thus imply that dimensional reduction may be used as a design strategy to frustrate order-disorder phenomena while retaining desirable electronic and thermal properties.

13.
Am Ann Deaf ; 146(4): 355-65, 2001 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-11816860

RESUMO

The roles of interpreters in an inclusive classroom were examined through a qualitative, 3-year case study of three interpreters in an inclusive school. Interviews were conducted with interpreters, classroom teachers, special education teachers, and administrators. The interview data were supplemented with observations and field notes. Results indicate that in addition to sign interpreting between American Sign Language and speech, the interpreters clarified teacher directions, facilitated peer interaction, tutored the deaf children, and kept the teachers and special educators informed of the deaf children's progress. The interpreter/aides and the classroom teachers preferred this full-participant interpreter role, while the special educators and administrators preferred a translator role. Classroom teachers were more comfortable with full-time interpreters who knew the classroom routine, while the special educators and administrators feared that full-time interpreters fostered child and teacher dependence. These issues are discussed in terms of congruence with the Registry of Interpreters code of ethics and how integration of young children might be best facilitated.


Assuntos
Inclusão Escolar , Língua de Sinais , Ensino , Tradução , Humanos , Serviços de Saúde Escolar/normas
14.
J Deaf Stud Deaf Educ ; 4(3): 163-75, 1999.
Artigo em Inglês | MEDLINE | ID: mdl-15579885

RESUMO

This article provides an overview of key issues pertinent to an inclusive approach to the education of deaf students in order to establish a context for interpreting and integrating the articles in this issue. It discusses definitions of inclusion, integration, and mainstreaming from placement-related, philosophical, and pragmatic perspectives. The article provides demographic information pertinent to an inclusive approach. It also compares perspectives on inclusion in the general field of special education with those in the education of deaf and hard-of-hearing students. It considers the challenges of using an inclusive approach to achieve academic and social integration of students, as based on research on the learning and adjustment of deaf and hard-of-hearing students in regular classes. The article concludes with an overview of the topics addressed in the issue.

15.
J Deaf Stud Deaf Educ ; 4(3): 203-14, 1999.
Artigo em Inglês | MEDLINE | ID: mdl-15579888

RESUMO

The research examined one school's attempts to include and integrate deaf and hard-of-hearing children. Interviews with teachers and observations of classrooms over a 3-year period revealed the critical roles played by the special educators and the classroom teachers. The responsibilities of the special educators, the adaptations and accommodation made by the classroom teachers, issues regarding ownership and attitude of the classroom teachers, perceptions of the special educator role, and specific areas of concern expressed by the special educators and classroom teachers are described.

16.
J Deaf Stud Deaf Educ ; 4(3): 215-24, 1999.
Artigo em Inglês | MEDLINE | ID: mdl-15579889

RESUMO

This study examined the perceptions of teams of two teachers, one deaf and one hearing, team-teaching students who are deaf and hard-of-hearing (D/HH) in co-enrolled classrooms. Five teachers who had worked in teams and their supervisor were interviewed about their team-teaching experiences and their perception of the effectiveness of this approach. Informants' responses were videotaped, transcribed, and analyzed. From the interview data, four main categories were identified: (1) philosophy of education, (2) perception of roles, (3) benefits of team-teaching, and (4) challenges. Findings revealed that team-teaching in co-enrolled classrooms gave all students access to their own and each other's cultures, languages, and social identities; deaf and hearing people were seen to have equality of status and students who are D/HH were seen to benefit from teachers' high expectations.

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