Effects of Co substitution on the structural and magnetic properties of Sr(Ni1−x_{1-x}Cox_x)2_2P2_2

Although SrNi$_2$P$_2$ adopts the common ThCr$_2$Si$_2$ structure for $T\geq 325$ K, being in an uncollapsed tetragonal (ucT) state, on cooling below 325 K it adopts a one-third collapsed orthorhombic (tcO) phase where one out of every three P-rows bond across the Sr layers. On the other hand, SrCo$_2$P$_2$ only exhibits the uncollapsed ThCr$_2$Si$_2$ structure from room temperature down to 1.8 K. Neither SrNi$_2$P$_2$ nor SrCo$_2$P$_2$ manifest magnetic transitions down to 50 mK and 2 K, respectively. In this work we report the effects of Co substitution in Sr(Ni$_{1-x}$Co$_x$)$_2$P$_2$, which allows for tuning the transition between the one-third collapsed and the uncollapsed structure. We find a rapid decrease of the one-third collapsed structural transition temperature with increasing Co fraction, until reaching full suppression for $x \geq 0.1$. Substitution levels in the range $0.11\leq x\leq 0.58$ show no signs of any transition down to 1.8 K in the magnetization or resistance measurements in the range $1.8\ \text{K}\leq T\leq 300\ \text{K}$. However, different magnetically ordered states emerge for $x\geq 0.65$, and disappear for $x\geq 0.99$, recovering the known paramagnetic properties of the parent compound SrCo$_2$P$_2$. These results are summarized in a phase diagram, built upon the characterization done on single crystals with different Co fraction. Both the magnetic and structural properties are compared to other systems with ThCr$_2$Si$_2$ structure that exhibit magnetic ordering and collapsed tetragonal transitions. The magnetic ordering and moment formation are well described by Takahashi's spin fluctuation theory of itinerant electron magnetism.Comment: 17 pages, 20 figure

Charge-order phase transition in the quasi one-dimensional organic conductor (TMTTF)2NO3

Low-dimensional organic conductors show a rich phase diagram, which has, despite all efforts, still some unexplored regions. Charge ordered phases present in many compounds of the (TMTTF)2X family are typically studied with their unique electronic properties in mind. An influence on the spin arrangement is, however, not expected at first glance. Here, we report temperature and angle dependent electron spin resonance (ESR) measurements on the quasi one-dimensional organic conductor (TMTTF)2NO3. We found that the (TMTTF)2NO3 compound develops a peculiar anisotropy with a doubled periodicity (ab′-plane) of the ESR linewidth below about TCO=(250±10) K. This behavior is similar to observations in the related compounds (TMTTF)2X (X=PF6, SbF6 and AsF6), where it has been attributed to relaxation processes of magnetically inequivalent sites in the charge-ordered state. For the structural analogous (TMTTF)2ClO4, known for the absence of charge order, such angular dependence of the ESR signal is not observed. Therefore, our ESR measurements lead us to conclude that a charge-order phase is stabilized in the title compound below TCO≈250 K.Deutsche ForschungsgemeinschaftProjekt DEA

Impact of Nematicity on the Relationship between Antiferromagnetic Fluctuations and Superconductivity in FeSe0.91S0.09 Under Pressure

The sulfur substituted FeSe system, FeSe$_{1-x}$S$_{x}$, provides a versatile platform for studying the relationship between nematicity, antiferromagnetism, and superconductivity. Here, by nuclear magnetic resonance (NMR) and resistivity measurements up to 4.73 GPa on FeSe$_{0.91}$S$_{0.09}$, we established the pressure($p$)-temperature($T$) phase diagram in which the nematic state is suppressed with pressure showing a nematic quantum phase transition (QPT) around $p$ = 0.5 GPa, two SC regions, separated by the QPT, appear and antiferromagnetic (AFM) phase emerges above $\sim$3.3 GPa. From the NMR results up to 2.1 GPa, AFM fluctuations are revealed to be characterized by the stripe-type wavevector which remains the same for the two SC regions. Furthermore, the electronic state is found to change in character from non-Fermi liquid to Fermi liquid around the nematic QPT and persists up to $\sim$ 2.1 GPa. In addition, although the AFM fluctuations correlate with $T_{\rm c}$ in both SC states, demonstrating the importance of the AFM fluctuations for the appearance of SC in the system, we found that, when nematic order is absent, $T_{\rm c}$ is strongly correlated with the AFM fluctuations, whereas $T_{\rm c}$ weakly depends on the AFM fluctuations when nematic order is present. Our findings on FeSe$_{0.91}$S$_{0.09}$ were shown to be applied to the whole FeSe$_{1-x}$S$_{x}$ system and also provide a new insight into the relationship between AFM fluctuations and SC in Fe-based superconductors.Comment: 10 pages, 10 figures including 4 pages and 6 figures of Supplementary Material, accepted for publication in Phys. Rev. B rapid communicatio

Synthesis, characterization, and incorporation of upconverting nanoparticles into a dental adhesive

The purpose of this study was to describe the synthesis, characterization, and functionalization of b-NaYF4:30%Yb/0.5%Tm upconverting nanocrystals for use as nanofillers in a dental adhesive and microscopically evaluate the interface between the particles and a commercial adhesive. The upconverting nanoparticles were synthesized and purified by thermal decomposition, and their chemical composition determined by energy dispersive X-Ray spectroscopy. The crystalline structure was characterized using X-Ray diffraction and morphology and size were observed with scanning and transmission electron microscopy. Upconverting emission was evaluated by spectrophotometry irradiating the particles with a 975 nm diode laser. Particles were functionalized with polyacrylic acid and the success was confirmed by measurement of Zeta Potential and transmission electron microscopy. The results of X-ray diffraction found a pure hexagonal phase crystalline pattern. Scanning electron microscopy showed uniform dispersion of hexagonal-shaped particles of approximately 150 nm. Upconversion emission was observed in 344 nm, 361 nm, 450 nm, 474nm, 646 nm, 803 nm. Functionalization success was confirmed by formation of a stable aqueous colloid with a Zeta potential of -29.5mV and the absence of voids in the particle-adhesive interface on the transmission electron microscopy images. The reported synthesis and functionalization process produced upconverting nanoparticles emitting photons within the blue spectral region (450 nm and 474 nm).Fil: Rocha Pacheco, Rafael. University Of Detroit Mercy; Estados UnidosFil: Garcia Flores, Ali Francisco. Universidad Federal do Abc; BrasilFil: Soto Montero, Jorge Rodrigo. Universidad de Costa Rica; Costa RicaFil: Lesseux, Guilherme Gorgen. Universidade Estadual de Campinas; BrasilFil: Rocha Acosta Lancelotti, Ailla Carla. Universidade Estadual de Campinas; BrasilFil: Martínez, Eduardo David. Universidade Estadual de Campinas; Brasil. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Unidad Ejecutora Instituto de Nanociencia y Nanotecnología. Unidad Ejecutora Instituto de Nanociencia y Nanotecnología - Nodo Bariloche | Comisión Nacional de Energía Atómica. Unidad Ejecutora Instituto de Nanociencia y Nanotecnología. Unidad Ejecutora Instituto de Nanociencia y Nanotecnología - Nodo Bariloche; ArgentinaFil: Rettori, Carlos. Universidad de Costa Rica; Costa RicaFil: Rodrigues Urbano, Ricardo. Universidade Estadual de Campinas; BrasilFil: Rueggeberg, Frederick Allen. No especifíca;Fil: Giannini, Marcelo. Universidade Estadual de Campinas; Brasi

Nuclear and electron magnetic resonance on strong correlated electron systems

Orientadores: Ricardo Rodrigues Urbano, Carlos RettoriTese (doutorado) - Universidade Estadual de Campinas, Instituto de Física Gleb WataghinResumo: Este trabalho teve por objetivo a investigação de sistemas com elétrons fortemente correlacionados via ressonância magnética nuclear (NMR) e eletrônica (ESR). Os seguintes sistemas foram investigados: i) o isolante Kondo SmB6 dopado com impurezas de Er3+ (via ESR), ii) compostos supercondutores à base de FeAs, da família BaFe 2As2 (via NMR) e, iii) o composto férmion pesado CeRhIn5 (via NMR em altos campos magnéticos). O estudo no composto de SmB6 via ESR (9.5 GHz) dos íons de Er3+ revelou um conjunto de quatro transições em baixa temperatura com uma anisotropia que não corresponde à esperada para transições entre níveis de campo cristalino cúbico. Mostramos que o efeito Jahn-Teller (JT) dinâmico associado a vibrações anarmônicas dos íons de Er3+ nos interstícios dos octaedros de B na rede de SmB6 explica a anisotropia das transições finas em baixa temperatura e concorda com o comportamento térmico da intensidade destas linhas de ressonância. Como resultado deste trabalho, ficou então proposta uma nova interpretação dos resultados sob a luz de um efeito de rattling anarmônico dos íons de Er3+ na matriz. Nenhum efeito de isolante topológico tipo Kondo foi evidenciado nos experimentos de ESR. Para os compostos de BaFe2As2 puro e com pouca substituição química (~ 0.5%) de Mn, Co e Cu realizamos um estudo detalhado da evolução das transições de alta temperatura, estrutural e magnética, que ocorrem no diagrama de fase dessa família de supercondutores. Combinando experimentos de NMR para o 75As em altos campos magnéticos, difração de raios-X de alta resolução e calor especíco mostramos que a fase ortorrômbica é estabilizada por flutuações magnéticas via acoplamento magneto elástico e que o ajuste do ângulo entre as ligações de As-Fe-As é o parâmetro mais relevante para a supressão das temperaturas de transição estrutural e magnética. Logo, este ajuste estrutural leva a um rearranjo da ocupação dos orbitais 3d do Fe aumentando a ocupação nos orbitais planares (3dxy), condição fundamental para que a fase supercondutora se forme nestes materiais. Já para o composto de CeRhIn5 investigamos a transição quântica induzida por campo magnético que ocorre em torno de 30 T (~ 1 K) neste material via NMR do 115In em ultra altos campos magnéticos. Observamos uma alteração no knight-shift associado ao In(1), que ocupa os planos de CeIn3. Apesar de nenhum efeito evidente na forma de linha, há um knight-shift líquido de 2.3% através da transição em Bc ~ 30 T. Isto demonstra uma mudança efetiva na densidade de estados no nível de Fermi consistente com a reconstrução da superfície de Fermi em torno de 30 T previamente reportada por medidas de oscilações quânticas. O fato de não se observar alteração de forma de linha espectral em 30 T nos permitiu concluir que a estrutura magnética incomensurável do CeRhIn5 não é drasticamente alterada através da transição o que corrobora com o cenário de um ponto crítico itinerante em torno de 50 T para CeRhIn5. Esta tese demonstra a relevância da técnica de Ressonância Magnética (NMR e ESR) na investigação das propriedades físicas de sistemas com elétrons fortemente correlacionadosAbstract: The present work aimed the investigation of strongly correlated electron systems via nuclear (NMR) and electronic (ESR) magnetic resonance. The following systems were investigated: i) Er3+ doped SmB6 Kondo insulator (via ESR), ii) FeAs-based superconducting compounds, from the BaFe2As2 family (via NMR) and, iii) CeRhIn5 heavy fermion compound (via ultra-high magnetic field NMR). The study on the SmB6 via Er3+ ESR (9.5 GHz) revealed a set of four resonance transitions at low temperature which show an anisotropy that does not correspond to the expected for transitions of pure cubic crystal field levels. We have shown that the dynamic Jahn-Teller (JT) effect associated to anharmonic rattling vibrations of Er3+ ions at the interstitial of the B-octahedron in the SmB6 lattice explains the anisotropy of the narrow lines at low temperature and agrees with the thermal behavior of the intensity of these resonance lines. As a result of this work, we proposed a new interpretation of the results under the light of a anharmonic rattling of the Er3+ ions in the SmB6 lattice. No topological insulator effect was evidenced by our ESR experiments. For the BaFe2As2 undoped and slightly substituted (~ 0.5%) of Mn, Co and Cu compounds we have performed a detailed study of the evolution of the high temperature transitions, structural and magnetic, which occur in the phase diagram of this superconductor family. Combining 75As high field NMR, high resolution X-ray diffraction and specific heat experiments we have shown that the orthorhombic phase is stabilized by magnetic fluctuations via magneto-elastic coupling and that the tuning of the angle of the As-Fe-As bounds is the most relevant parameter to the suppression of the structural and magnetic transition temperatures. Thus, this structural tuning leads to a rearrangement of the occupancy of the Fe-3d orbitals increasing the occupancy of the planar orbital (3dxy), which is a fundamental condition to the formation of the superconducting phase in these materials. Finally, for the CeRhIn5 compound we have investigated the magnetic field-induced quantum transition which occurs around ~ 30 T (~ 1 K) in this material via 115In ultra-high magnetic field NMR. We observed a knight-shift alteration for the In(1), which is sited in the CeIn3 planes. There is a net knight-shift of 2.3% across the transition at Bc ~ 30 T. Although lineshape effects have not been detected, it demonstrates an effective change in the density of states at the Fermi level consistent with a Fermi surface reconstruction around 30 T previously reported by quantum oscillation measurements. We did not observe a change in the spectral lineshape across 30 T and it leads us to the conclusion that the CeRhIn5 incommensurate magnetic structure is not drastically altered across the transition which is consistent with the scenario of an itinerant quantum critical point at 50 T for CeRhIn5. This thesis demonstrates the relevance of the magnetic resonance (NMR and ESR) techniques in the investigation of physical properties of strongly correlated electron systemsDoutoradoFísicaDoutor em Ciências140837/2013-2CNP

Impact of nematicity on the relationship between antiferromagnetic fluctuations and superconductivity in FeSe0.91S0.09 under pressure

The sulfur-substituted FeSe system, FeSe1−xSx, provides a versatile platform for studying the relationship among nematicity, antiferromagnetism, and superconductivity. Here, by nuclear magnetic resonance (NMR) and resistivity measurements up to 4.73 GPa on FeSe0.91S0.09, we established the pressure- (p-) temperature (T) phase diagram in which the nematic state is suppressed with pressure showing a nematic quantum phase transition (QPT) around p=0.5GPa, two superconductivity (SC) regions separated by the QPT appear, and antiferromagnetic (AFM) phase emerges above ∼3.3GPa. From the NMR results up to 2.1 GPa, AFM fluctuations are revealed to be characterized by the stripe-type wave vector which remains the same for the two SC regions. Furthermore, the electronic state is found to change in character from non-Fermi liquid to Fermi liquid around the nematic QPT and persists up to ∼2.1GPa. In addition, although the AFM fluctuations correlate with Tc in both SC states, demonstrating the importance of the AFM fluctuations for the appearance of SC in the system, we found that, when nematic order is absent, Tc is strongly correlated with the AFM fluctuations whereas Tc weakly depends on the AFM fluctuations when nematic order is present. Our findings on FeSe0.91S0.09 were shown to be applied to the whole FeSe1−xSx system and provide an insight into the relationship between AFM fluctuations and SC in Fe-based superconductors.</p

Pseudoelasticity of SrNi2P2 Micropillar via Double Lattice Collapse and Expansion

The maximum recoverable strain of most crystalline solids is less than 1% because plastic deformation or fracture usually occurs at a small strain. In this work, we show that a SrNi2P2 micropillar exhibits pseudoelasticity with a large maximum recoverable strain of ∼14% under uniaxial compression via unique reversible structural transformation, double lattice collapse–expansion that is repeatable under cyclic loading. Its high yield strength (∼3.8 ± 0.5 GPa) and large maximum recoverable strain bring out the ultrahigh modulus of resilience (∼146 ± 19 MJ/m3), a few orders of magnitude higher than that of most engineering materials. The double lattice collapse–expansion mechanism shows stress–strain behaviors similar to that of conventional shape-memory alloys, such as hysteresis and thermo-mechanical actuation, even though the structural changes involved are completely different. Our work suggests that the discovery of a new class of high-performance ThCr2Si2-structured materials will open new research opportunities in the field of pseudoelasticity.This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Nano Letters, copyright © 2022 American Chemical Society after peer review. To access the final edited and published work see DOI: 10.1021/acs.nanolett.1c01750. DOE Contract Number(s): AC02-07CH11358. Posted with permission

Pseudoelasticity of SrNi2P2 micropillar via double lattice collapse and expansion

The maximum recoverable strain of most crystalline solids is less than 1% because plastic deformation or fracture usually occurs at a small strain. In this work, we show that a SrNi2P2 micropillar exhibits pseudoelasticity with a large maximum recoverable strain of ~14% under uniaxial compression via unique reversible structural transformation, double lattice collapse-expansion that is repeatable under cyclic loading. Its high yield strength (~3.8±0.5 GPa) and large maximum recoverable strain bring out the ultrahigh modulus of resilience (~146±19MJ/m3) a few orders of magnitude higher than that of most engineering materials. The double lattice collapse-expansion mechanism shows stress-strain behaviors similar with that of conventional shape memory alloys, such as hysteresis and thermo-mechanical actuation, even though the structural changes involved are completely different. Our work suggests that the discovery of a new class of high performance ThCr2Si2-structured materials will open new research opportunities in the field of pseudoelasticit