Low-energy electronic structure in the unconventional charge-ordered state of ScV6Sn6.

Kagome vanadates AV3Sb5 display unusual low-temperature electronic properties including charge density waves (CDW), whose microscopic origin remains unsettled. Recently, CDW order has been discovered in a new material ScV6Sn6, providing an opportunity to explore whether the onset of CDW leads to unusual electronic properties. Here, we study this question using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The ARPES measurements show minimal changes to the electronic structure after the onset of CDW. However, STM quasiparticle interference (QPI) measurements show strong dispersing features related to the CDW ordering vectors. A plausible explanation is the presence of a strong momentum-dependent scattering potential peaked at the CDW wavevector, associated with the existence of competing CDW instabilities. Our STM results further indicate that the bands most affected by the CDW are near vHS, analogous to the case of AV3Sb5 despite very different CDW wavevectors.

First-order antiferromagnetic transitions of SrMn2P2 and CaMn2P2 single crystals containing corrugated-honeycomb Mn sublattices.

SrMn2P2 and CaMn2P2 are insulators that adopt the trigonal CaAl2Si2-type structure containing corrugated Mn honeycomb layers. Magnetic susceptibility χ and heat capacity versus temperature T data reveal a weak first-order antiferromagnetic (AFM) transition at the Néel temperature [Formula: see text] K for SrMn2P2 and a strong first-order AFM transition at [Formula: see text] K for CaMn2P2 Both compounds exhibit isotropic and nearly T-independent [Formula: see text], suggesting magnetic structures in which nearest-neighbor moments are aligned at [Formula: see text] to each other. The 31P NMR measurements confirm the strong first-order transition in CaMn2P2 but show critical slowing down above [Formula: see text] for SrMn2P2, thus also evidencing second-order character. The 31P NMR measurements indicate that the AFM structure of CaMn2P2 is commensurate with the lattice whereas that of SrMn2P2 is incommensurate. These first-order AFM transitions are unique among the class of (Ca, Sr, Ba)Mn2 (P, As, Sb, Bi)2 compounds that otherwise exhibit second-order AFM transitions. This result challenges our understanding of the circumstances under which first-order AFM transitions occur.

Complex magnetic properties associated with competing local and itinerant magnetism in [Formula: see text].

Ternary intermetallic compound [Formula: see text] has been synthesized in single phase and characterized by x-ray diffraction, scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM-EDX) analysis, magnetization, heat capacity, neutron diffraction and muon spin rotation/relaxation ([Formula: see text]SR) measurements. The polycrystalline compound was synthesized in single phase by introducing necessary vacancies in Co/Si sites. Magnetic, heat capacity, and zero-field neutron diffraction studies reveal that the system undergoes magnetic transition below [Formula: see text]4 K. Neutron diffraction measurement further reveals that the magnetic ordering is antiferromagnetic in nature with an weak ordered moment. The high temperature magnetic phase has been attributed to glassy in nature consisting of ferromagnetic clusters of itinerant (3d) Co moments as evident by the development of internal field in zero-field [Formula: see text]SR below 50 K. The density-functional theory (DFT) calculations suggest that the low temperature magnetic transition is associated with antiferromagnetic coupling between Pr 4f and Co 3d spins. Pr moments show spin fluctuation along with unconventional orbital moment quenching due to crystal field. The evolution of the symmetry and the crystalline electric field environment of Pr-ions are also studied and compared theoretically between the elemental Pr and when it is coupled with other elements such as Co. The localized moment of Pr 4f and itinerant moment of Co 3d compete with each other below [Formula: see text]20 K resulting in an unusual temperature dependence of magnetic coercivity in the system.

Short-range ferromagnetic order due to Ir substitutions in single-crystallineBa(Co1-xIrx)2As2(0 ≤ x ≤ 0.25).

The ternary-arsenide compound BaCo2As2was previously proposed to be in proximity to a quantum-critical point where long-range ferromagnetic (FM) order is suppressed by quantum fluctuations. Here we report the effect of Ir substitutions for Co on the magnetic and thermal properties of Ba(Co1-xIrx)2As2(0 ≤ x ≤ 0.25) single crystals. These compositions all crystallize in an uncollapsed body-centered-tetragonal ThCr2Si2structure with space groupI4/mmm. Magnetic susceptibility measurements reveal clear signatures of short-range FM ordering for x ≥ 0.11 below a nearly composition-independent characteristic temperatureTcl≈ 13 K. The small variation ofTclwith x, thermomagnetic irreversibility between zero-field-cooled and field-cooled magnetic susceptibility versusT, the occurrence of hysteresis in magnetization versus field isotherms at low field and temperature, and very small spontaneous and remanent magnetizations < 0.01 µB/f.u. together indicate that the FM response arises from short-range FM ordering of FM spin clusters as previously inferred to occur in Ca(Co1-xIrx)2-yAs2. Heat-capacityCp(T) data do not exhibit any clear feature aroundTcl, consistent with the very small moments of the FM clusters. TheCp(T) in the paramagnetic temperature regime 25-300 K is well described by the sum of a Sommerfeld electronic contribution and Debye and Einstein lattice contributions where the latter lattice contribution suggests the presence of low-frequency optic modes associated with the heavy Ba atoms in the crystals.

Short-range ferromagnetic order due to Ir substitutions in single-crystalline Ba(Co1- x Ir x )2As2 (0 ⩽ x ⩽ 0.25).

The ternary-arsenide compound BaCo2As2 was previously proposed to be in proximity to a quantum-critical point where long-range ferromagnetic (FM) order is suppressed by quantum fluctuations. Here we report the effect of Ir substitutions for Co on the magnetic and thermal properties of Ba[Formula: see text] (0 ⩽ x ⩽ 0.25) single crystals. These compositions all crystallize in an uncollapsed body-centered-tetragonal ThCr2Si2 structure with space group I4/mmm. Magnetic susceptibility measurements reveal clear signatures of short-range FM ordering for x ⩾ 0.11 below a nearly composition-independent characteristic temperature T cl ≈ 13 K. The small variation of T cl with x, thermomagnetic irreversibility between zero-field-cooled and field-cooled magnetic susceptibility versus T, the occurrence of hysteresis in magnetization versus field isotherms at low field and temperature, and very small spontaneous and remanent magnetizations <0.01 µ B/f.u. together indicate that the FM response arises from short-range FM ordering of FM spin clusters as previously inferred to occur in Ca(Co1-x Ir x )2-y As2. Heat-capacity C p(T) data do not exhibit any clear feature around T cl, consistent with the very small moments of the FM clusters. The C p(T) in the paramagnetic temperature regime 25-300 K is well described by the sum of a Sommerfeld electronic contribution and Debye and Einstein lattice contributions where the latter lattice contribution suggests the presence of low-frequency optic modes associated with the heavy Ba atoms in the crystals.

Studies on magnetocaloric effect of Tb2Ni0.90Si2.94 compound.

A comparative study has been carried out on the magnetocaloric properties of as-cast and annealed Tb2Ni0.90Si2.94 intermetallic compound. While the as-cast material exhibits ferromagnetic cluster-glass behaviour below 9.9 K coexisting with antiferromagnetic (AFM) interaction, the annealed system shows AFM ordering below 13.5 K and spin freezing occurs below 4 K. The compound exhibits moderate magnetocaloric performance with maximum isothermal entropy changes (-ΔS M) 8.8 and 10.9 J kg-1 K-1, relative cooling power (RCP) 306 and 365 J kg-1, along with adiabatic temperature change (ΔT ad) 5.5 and 8.15 K for 70 kOe magnetic field change in as-cast and annealed forms, respectively. The estimated magnetic entropy change is found to be larger for annealed sample in comparison to that of as-cast analogue. However, the full width at half maxima (FWHM) of -ΔS M(T) behaviour is larger in as-cast compound due to the presence of inherent structural disorder which reduces with thermal annealing. A positive isothermal entropy change (-ΔS M) and adiabatic temperature change (ΔT ad) is observed for the as-cast compound in the measured field and temperature region. In contrast, the annealed system exhibits inverse magnetocaloric effect in the low field and temperature region where AFM interactions dominate. Magnetocaloric effect (MCE) is used as a tool to establish a subtle correlation between the observed magnetocaloric effect and the reported magnetic properties of the system.

Unusual bidirectional frequency dependence of dynamical susceptibility in hexagonal intermetallic Pr2Ni0.95Si2.95.

In this study, the synthesis of a novel ternary intermetallic compound Pr2Ni0.95Si2.95 forming in single phase only by deliberately introducing vacancies in Ni/Si site is reported. The detailed studies on dc magnetization, heat capacity, ac magnetization & associated dynamical scaling, different types of non-equilibrium dynamical behaviour, viz., magnetic relaxation behaviour as a function of wait time and temperature, aging phenomena, and magnetic memory effect firmly establish that the compound exhibits spin freezing behaviour below 3.3 K (Tf). However, below Tf, temperature dependence of ac susceptibility data exhibit an additional peak that shows reverse frequency dependence to that generally observed in a glassy system. The unusual bidirectional frequency dependence in a single magnetic system is of significant interest and rarely reported in literature. Competing exchange interaction arising from c/a ~ 1 and crystallographic randomness driven magnetic phase separation has been argued to be responsible for such observation. The reverse frequency shift of the low temperature peak has been described on the basis of a simple phenomenological model proposed in this work.

Observation of short range order driven large refrigerant capacity in chemically disordered single phase compound Dy2Ni0.87Si2.95.

In this work, we report the successful synthesis of a new intermetallic compound Dy2Ni0.87Si2.95 forming in single phase only with a chemically disordered structure. The random distribution of Ni/Si and crystal defects create a variation in the local electronic environment between the magnetic Dy ions. In the presence of both disorder and competing exchange interactions driven magnetic frustration, originating due to c/a ∼ 1, the compound undergoes spin freezing behaviour below 5.6 K. In the non-equilibrium state below the spin freezing behaviour, the compound exhibits aging phenomena and magnetic memory effects. In the magnetically short-range ordered region, much above the freezing temperature, an unusual occurrence of considerable magnetic entropy change, -ΔSmaxM ∼ 21 J kg-1 K-1 with large cooling power RCP ∼ 531 J kg-1 and adiabatic temperature change, ΔTad ∼ 10 K for a field change of 70 kOe, is observed for this short range ordered cluster-glass compound without any magnetic hysteresis loss.

Role of random magnetic anisotropy on the valence, magnetocaloric and resistivity properties in a hexagonal Sm2Ni0.87Si2.87 compound.

In this work, we report the effect of random magnetic anisotropy (RMA) on the valence, magnetocaloric and resistivity properties in a glassy intermetallic material Sm2Ni0.87Si2.87. On the basis of detailed studies on the valence band and core level electronic structure, we have established that both the Sm3+ and Sm2+ ions are present in the system, suggesting the compound to be of mixed valence in nature. The significant observation of positive magnetic entropy change in zero-field cooled measurement has been argued due to the presence of RMA that develops due to local electronic environmental variations between the rare-earth ions in the system. The quantum interference effect caused by the elastic electron-electron interaction is responsible for the resistivity upturn at low-temperature for this disordered metallic conductor.

Chemical disorder driven reentrant spin cluster glass state formation and associated magnetocaloric properties of Nd2Ni0.94Si2.94.

In this work, we report the synthesis of a new ternary intermetallic compound, Nd2Ni0.94Si2.94, that forms in single phase only in a defect crystal structure. The compound exhibits an antiferromagnetic transition below 7.2 K (TN) followed by a spin cluster freezing behaviour below 2.85 K (Tf), which makes the compound a reentrant spin cluster glass system. The detailed studies of dc and ac magnetization, heat capacity, non-equilibrium dynamical behaviour, viz., aging effect, temperature and field dependent magnetic relaxation and magnetic memory effect establish the compound to be a cluster-glass material below freezing temperature. The interplay between competing exchange coupling (c/a ≃ 1.04 ⇒ JNN ≃ JNNN) and chemical disorder driven variation in the electronic environment among the Nd ions has been argued to be responsible for such a metastable state formation. A considerable value of MCE parameters (-ΔS ∼ 11.4 J kg-1 K-1, RCP ∼ 160 J kg-1 and ΔTad ∼ 5.2 K for a field change of 70 kOe) is obtained for this magnetically frustrated glassy compound.

Low-field induced large magnetocaloric effect in Tm2Ni0.93Si2.93: influence of short-range magnetic correlation.

In this work, we report the successful synthesis of a new intermetallic compound Tm2 [Formula: see text] [Formula: see text] that forms in single phase only in defect crystal structure. The compound does not show any long range magnetic ordering down to 2 K. The material exhibits a large magnetic entropy change ([Formula: see text] J [Formula: see text] K-1) and adiabatic temperature change ([Formula: see text] K) at 2.2 K for a field change of 20 kOe which can be realized by permanent magnets, thus being very beneficial for application purpose. In the absence of long-range magnetic ordering down to 2 K, the metastable nature of low-temperature spin dynamics and short-range magnetic correlations are considered to be responsible for such a large magnetocaloric effect over a wide temperature region.

Magnetic frustration induced large magnetocaloric effect in the absence of long range magnetic order.

We have synthesized a new intermetallic compound Ho2Ni0.95Si2.95 in a single phase with a defect crystal structure. The magnetic ground state of this material found to be highly frustrated without any long range order or glassy feature as investigated through magnetic, heat capacity and neutron diffraction measurements. The interest in this material stems from the fact that despite the absence of true long range order, large magnetocaloric effect (isothermal magnetic entropy change, -ΔSM ~ 28.65 J/Kg K (~205.78 mJ/cm3 K), relative cooling power, RCP ~ 696 J/Kg (~5 J/cm3) and adiabatic temperature change, ΔT ad ~ 9.32 K for a field change of 70 kOe) has been observed which is rather hard to find in nature.

Role of the stability of charge ordering in exchange bias effect in doped manganites.

In this work we have carried out an elaborate study on the magnetic properties and investigated the exchange bias phenomena of some charge-ordered (CO) manganites. The detailed study of Sm1-x Ca x MnO3 (x = 0.5, 0.55, 0.6, 0.65, 0.7) compounds shows that Sm0.4Ca0.6MnO3, which is the most robust charge ordered material studied here, shows significantly large exchange bias field (HE) as compared to the other compounds. Our experimental results and analysis indicate that TCO, which reflects the stability of the charge-ordered state, is one of the key parameters for the exchange bias effect. Similar behaviour is found in other rare-earth analogues, viz., La1-x Ca x MnO3 and Pr1-x Ca x MnO3 compounds as well. We also found that with increasing stability of CO states in Sm1-x Ca x MnO3 compounds, HE enhances due to increase in number and reduction in size of ferromagnetic clusters.