Extremely Large Magnetic Entropy Changes, Quantum Phases, Transitions and Diagram in Gd(OH)3 Single Crystal Nanowires - Quasi-1D Large Spin (S = -7/2) Chain Antiferromagnet
R. Zeng, C. F. Zhang, J. C. Debnath, P. Shamba, J. L. Wang, Z. X. Chen, Z. P. Guo, S. X. Dou
Systematically magnetic and magnetothermal measurements at temperatures down to 2 K and magnetic fields up to 13.5 Tesla for Gd(OH)3 Single Crystal Nanowires - Quasi-1D Large Spin (S = -7/2) Chain Antiferromagnet have been conducted. We find that, (1) magnetic field enhances the thermal and local spin fluctuations which suppress long-range spin ordering (LRO) within the measured temperature range, and close to 0 K at the quantum critical point (QCP); (2) possible field-induced exotic local spin-liquid-like, aligned-spin, and spin-flip exotic paramagnetic phases, and transitions in the low temperature and high field range have been observed, allowing us to identify a possible quantum critical point; (3) there is extremely large, fully reversible MCE (magnetic entropy change (-ΔSM) = 27.8, 66, and 88 J / kg K, adiabatic temperature change (ΔTad) = 6.7, 17.6, and 36.4 K at 2.55 K for field changes of 2, 5, and 11 T, respectively in the continuum of quantum phase transitions in this system; (4) moreover, careful experiments and analysis may allow experimental determination and set up a quantum phase diagram of this system. The magnetic-entropy change monotonically increases with decreasing temperature, and it exceeds the magnetocaloric effect (MCE) in any other known low temperature reversible MCE material by at least a factor of 3. The extremely large magnetic entropy change may be attributed to the large amount of weakly interacting spins that can be easily aligned at low-lying energy in the quantum critical regime of our nanosized materials, since there is large MCE in the local spin-liquid-like (low energy excitation and even gapless state) range. These indicate that the material is a promising MCE candidate for low temperature application, and possibly could make ultra-low temperatures easily achievable for most laboratories and for space application as well.
We present a Monte Carlo study of the magnetic properties of thin cylindrical nanowires composed of a ferromagnetic core and an antiferromagnetic shell implementing a classical spin Hamiltonian. We address systematically the impact of interface exchange coupling on the loop characteristics and the magnetization reversal mechanism. We study the effect of shell polycrystallinity on the characteristic fields of the isothermal hysteresis loop (coercivity, exchange-bias). We demonstrate that coupling to a polycrystalline antiferromagnetic shell increases the critical core diameter for transition fr…
Magnetic nanowires supporting field- and current-driven domain wall motion are envisioned for new methods of information storage and processing. A major obstacle for their practical use is the domainwall velocity, which is traditionally limited due to the Walker breakdown occurring when the forcing field or current reaches a critical threshold value. We show through numerical and analytical modeling that the Walker breakdown limit can be extended or completely eliminated in antiferromagnetically coupled magnetic nanowires. These coupled nanowires allow for giant domain-wall velocities driven b…
The magnetic properties of Co (<D>=15 nm, <L>=130nm) nanowires are reported. In oxidized wires, we measure large exchange bias fields of the order of 0.1 T below T ~ 100 K. The onset of the exchange bias, between the ferromagnetic core and the anti-ferromagnetic CoO shell, is accompanied by a coercivity drop of 0.2 T which leads to a minimum in coercivity at $\sim100$ K. Magnetization relaxation measurements show a temperature dependence of the magnetic viscosity S which is consistent with a volume distribution of the CoO grains at the surface. We propose that the superparamagnetic fluctuation…
Time-dependent drift of resistance and threshold voltage in phase change memory (PCM) devices is of concern as it leads to data loss. Electrical drift in amorphous chalcogenides has been argued to be either due to electronic or stress relaxation mechanisms. Here we show that drift in amorphized Ge2Sb2Te5 nanowires with exposed surfaces is extremely low in comparison to thin-film devices. However, drift in stressed nanowires embedded under dielectric films is comparable to thin-films. Our results shows that drift in PCM is due to stress relaxation and will help in understanding and controlling …
Antiferromagnets (AFMs) are widely believed to be superior than ferromagnets in spintronics because of their high stability due to the vanishingly small stray field. It is thus expected that the order parameter of AFM should always align along the easy-axis of the crystalline anisotropy. In contrast to this conventional wisdom, we find that the AFM order parameter switches away from the easy-axis below a critical anisotropy strength when an AFM is properly tailored into a nano-structure. The switching time first decreases and then increases with the damping. Above the critical anisotropy, the …
An emerging branch of electronics, the optospintronics, would be highly boosted if the control of magnetic order by light is implemented in magnetic semiconductors nanostructures being compatible with the actual technology. Here we show that the ferromagnetic magnetization of low Fe-doped ZnO nanowires prepared by carbothermal process is enhanced under illumination up to temperatures slightly below room temperature. This enhancement is related to the existence of an oxygen vacancy V$_{\rm O}$ in the neighbouring of an antiferromagnetic superexchange Fe$^{3+}$-Fe$^{3+}$ pair. Under illumination…
Theoretical studies have shown that Majorana bound states can be induced at the ends of a one dimensional wire, a phenomenon possible due to the interplay between s-wave superconductivity, spin-orbit coupling, and an external magnetic field. These states have been observed in superconductor-semiconductor hybrid nanostructures in the presence of a Zeeman field, and in the limit of a low density of particles. In this paper, we demonstrate and discuss the possibility of the emergence of Majorana bound states in a superconducting Rashba nanowire deposited on an antiferromagnetically ordered surfac…
Growth of GaAs and InGaAs nanowires by the group-III assisted Molecular Beam Epitaxy growth method is studied in dependence of growth temperature, with the objective of maximizing the indium incorporation. Nanowire growth was achieved for growth temperatures as low as 550°C. The incorporation of indium was studied by low temperature micro-photoluminescence spectroscopy, Raman spectroscopy and electron energy loss spectroscopy. The results show that the incorporation of indium lowering the growth temperature does not have an effect in increasing the indium concentration in the bulk of the nanow…
Using Landau-Ginzburg-Devonshire theory we study the complex interplay between structural antiferrodistortive order parameter (oxygen octahedron rotations), polarization and magnetization in EuxSr1-xTiO3 nanotubes and nanowires. We calculated EuxSr1-xTiO3 bulk and nanosystem phase diagrams, which include the antiferrodistortive, ferroelectric, ferromagnetic and antiferromagnetic phases. Our calculation shows the presence of "triple" antiferrodistortive-ferroelectric-ferromagnetic phases for EuxSr1-xTiO3 nanowires and nanotubes. presents interest for fundamental study and can be important for t…
Incorporating relativistic physics into quantum tunneling can lead to exotic behavior such as perfect transmission via Klein tunneling. Here, we probe the tunneling properties of spin-momentum locked relativistic fermions by designing and implementing a tunneling geometry that utilizes nanowires of the topological Kondo insulator candidate, SmB6. The nanowires are attached to the end of scanning tunneling microscope tips, and used to image the bicollinear stripe spin-order in the antiferromagnet Fe1.03Te with a Neel temperature of ~50 K. The antiferromagnetic stripes become invisible above 10 …
We predicted the ferroelectric-ferromagnetic multiferroic properties of EuTiO3 nanowires and generated the phase diagrams in coordinates of temperature and wire radii. The calculations were performed within the Landau-Ginzburg-Devonshire theory with phenomenological parameters extracted from tabulated experimental data and first principles calculations. Since bulk EuTiO3 is antiferromagnetic at temperatures lower than 5.5 K and paraelectric at all temperatures, our goal was to investigate the possibility of inducing the ferroelectric and ferromagnetic properties of EuTiO3 by reducing the bulk …
The combination of x-ray spectroscopy methods complemented with theoretical analysis unravels the coexistence of paramagnetic and antiferromagnetic phases in the Zn_0.9Mn_0.1O shell deposited onto array of wurtzite ZnO nanowires. The shell is crystalline with orientation toward the ZnO growth axis, as demonstrated by X-ray linear dichroism. EXAFS analysis confirmed that more than 90% of Mn atoms substituted Zn in the shell while fraction of secondary phases was below 10%. The value of manganese spin magnetic moment was estimated from the Mn Kβ X-ray emission spectroscopy to be 4.3μB which is c…
A cylindrical magnetic nanowire system composed of ferromagnetic core and shell layers has been investigated by using effective field theory with correlations. Both ferromagnetic and antiferromagnetic exchange couplings at the core-shell interface have been considered. Main attention has been focused on the effects of the quenched disordered shell bonds, as well as interface bonds on the magnetic properties of the system. A complete picture of the phase diagrams and magnetization profiles has been represented. It has been shown that for the antiferromagnetic nanowire system, the magnetization …
By means of first-principles density functional theory calculations, we find that hydrogen-passivated ultrathin silicon nanowires (SiNWs) along [100] direction with symmetrical multiple surface dangling bonds (SDBs) and boron doping can have a half-metallic ground state with 100% spin polarization, where the half-metallicity is shown quite robust against external electric fields. Under the circumstances with various SDBs, the H-passivated SiNWs can also be ferromagnetic or antiferromagnetic semiconductors. The present study not only offers a possible route to engineer half-metallic SiNWs witho…
By means of the effective-field theory (EFT) with correlations, the thermodynamic and magnetic quantities such as magnetization, susceptibility, internal energy, free energy, hysteresis curves and compensation behaviors of the spin-1/2 hexagonal Ising nanowire (HIN) system with core/shell structure have been presented. The hysteresis curves are obtained for different values of the system parameters on both ferromagnetic and antiferromagnetic case. It has been shown that the system only undergoes a second-order phase transition. Moreover, from the thermal variations of the total magnetization, …
A low temperature hydrothermal route has been developed, and pure phase Ba$_2$Ni$_3$F$_{10}$ nanowires have been successfully prepared under the optimized conditions. Under the 325 nm excitation, the Ba$_2$Ni$_3$F$_{10}$ nanowires exhibit three emission bands with peak positions locating at 360 nm, 530 nm, and 700 nm, respectively. Combined with the first-principles calculations, the photoluminescence property can be explained by the electron transitions between the t2g and eg orbitals. Clear hysteresis loops observed below the temperature of 60 K demonstrates the weak ferromagnetism in Ba$_2$…
We present a study of magnetic properties of single-crystal Co3O4 nanowires with diameter about 7 nm. The nanowires expose (111) planes composed of plenty of Co3+ cations and exhibit two Néel temperatures at 56 K (TN of wire cores) and 73 K (TN of wire shells), which are far above TN = 40 K of bulk Co3O4. This novel bahavior is attributed to symmetry breaking of surface Co3+ cations and magnetic proximity effect. The nanowire shells show macroscopic residual magnetic moments. Cooling in a magnetic field, a fraction of the residual moments are tightly pinned to the antiferromagnetic lattice, wh…
Porous materials provide a large surface to volume ratio, thereby providing a knob to alter fundamental properties in unprecedented ways. In thermal transport, porous nanomaterials can reduce thermal conductivity by not only enhancing phonon scattering from the boundaries of the pores and therefore decreasing the phonon mean free path, but also by reducing the phonon group velocity. Here we establish a structure-property relationship by measuring the porosity and thermal conductivity of individual electrolessly etched single crystalline silicon nanowires using a novel electron beam heating tec…
Electron spin relaxation in nanowire-based quantum dots induced by confined phonons is investigated theoretically. Due to the one-dimensional nature of the confined phonons, the van Hove singularities of the confined phonons and the zero of the form factor of the electron-phonon coupling can lead to unique features of the spin relaxation rate. Extremely strong spin relaxation can be obtained at the van Hove singularity. Meanwhile the spin relaxation rate can also be greatly suppressed at the zero of the form factor. This unique feature indicates the flexibility of nanowire-based quantum dots i…
Quasi one-dimensional (1D) vanadium tetrasulfide ($VS_4$) nanowires (NWs) are synthetic semiconductors which combine with each other through Van der Waals interactions to form bulk phases. However, the properties of these individual nanowires remain unknown. Nevertheless, our calculations of their stability indicate that $VS_4$) NWs can be separated from their bulk structures. Accordingly, we theoretically investigated the geometrical, electronic, and magnetic properties of bulk phase and isolated $VS_4$ NWs. Our results indicate that both bulk phase and isolated $VS_4$ NWs are semiconductors …
The development of molecular nanostructures plays a major role in emerging organic electronic applications, as it leads to improved performance and is compatible with our increasing need for miniaturisation. In particular, nanowires have been obtained from solution or vapour phase and have displayed high conductivity, or large interfacial areas in solar cells. In all cases however, the crystal structure remains as in films or bulk, and the exploitation of wires requires extensive post-growth manipulation as their orientations are random. Here we report copper phthalocyanine (CuPc) nanowires wi…
The structural and optical properties of 3 different kinds of GaAs nanowires with 100% zinc-blende structure and with an average of 30% and 70% wurtzite are presented. A variety of shorter and longer segments of zinc-blende or wurtzite crystal phases are observed by transmission electron microscopy in the nanowires. Sharp photoluminescence lines are observed with emission energies tuned from 1.515 eV down to 1.43 eV when the percentage of wurtzite is increased. The downward shift of the emission peaks can be understood by carrier confinement at the interfaces, in quantum wells and in random sh…
The virtual (i.e., fundamental many body quantum theory-based, computational) synthesis method is used to establish electronic templates of about 30 non-stoichiometric nanosystems composed of nickel and oxygen atoms and ranging from about 6 Å to 6 nm in linear dimensions. Flexible and stretchable Ni-O bond in such structures accommodates various ratios of Ni to O atoms, and both antiferromagnetic and ferromagnetic spin alignments. Depending on synthesis conditions, smaller Ni-O quantum dots (QDs) composed of up to 14 atoms or so may have both types of spin alignments, while quantum-confined, q…
We have studied the effect of thermal effects on the structural and transport response of Ag atomic-size nanowires generated by mechanical elongation. Our study involves both time-resolved atomic resolution transmission electron microscopy imaging and quantum conductance measurement using an ultra-high-vacuum mechanically controllable break junction. We have observed drastic changes in conductance and structural properties of Ag nanowires generated at different temperatures (150 and 300 K). By combining electron microscopy images, electronic transport measurements and quantum transport calcula…
As the conventional silicon metal-oxide-semiconductor field-effect transistor (MOSFET) approaches its scaling limits; many novel device structures are being extensively explored. Among them, the silicon nanowire transistor (SNWT) has attracted broad attention. To understand device physics in depth and to assess the performance limits of SNWTs, simulation is becoming increasingly important. The objectives of this work are: 1) to theoretically explore the essential physics of SNWTs (e.g., electrostatics, transport and band structure) by performing computer-based simulations, and 2) to assess the…
The demonstration of the generation and control of a pure spin current (without net charge flow) by electric fields and/or temperature gradient has been an essential leap in the quest for low-power consumption electronics. The key issue of whether and how such a current can be utilized to drive and control information stored in magnetic domain walls (DWs) is still outstanding and is addressed here. We demonstrate that pure spin current acts on DWs in a magnetic stripe with an effective spin-transfer torque resulting in a mutual DWs separation dynamics and picosecond magnetization reversal. In …
Intersubband optoelectronic devices rely on transitions between quantum-confined electron levels in semiconductor heterostructures, which enables infrared (IR) photodetection in the 1-30 $μ$m wavelength window with picosecond response times. Incorporating nanowires as active media could enable an independent control over the electrical cross-section of the device and the optical absorption cross-section. Furthermore, the three-dimensional carrier confinement in nanowire heterostructures opens new possibilities to tune the carrier relaxation time. However, the generation of structural defects a…
We investigate the magnetic interactions in triangular rare-earth delafossites materials NaYbO$_2$ and NaYbS$_2$ via first-principles calculations. The calculated Curie-Weiss temperatures are in good agreement with experiments. We perform classical Monte Carlo simulations of the two compounds using the extracted exchange parameters. We find that if only the nearest neighbor interactions are considered, the magnetic ground states of NaYbO$_2$ and NaYbS$_2$ are a stripe and a planar 120\degree~ Néel state, respectively. The simulated transition temperatures are much higher than the lowest experi…
Reduced dimensionality leads to emergent phenomena in quantum materials and there is a need for accelerated materials discovery of nanoscale quantum materials in reduced dimensions. Thermomechanical nanomolding is a rapid synthesis method that produces high quality single-crystalline quantum nanowires with controlled dimensions over wafer-scale sizes. Herein, we apply nanomolding to fabricate nanowires from bulk feedstock of MoP, a triple-point topological metal with extremely high conductivity that is promising for low-resistance interconnects. Surprisingly, we obtained single-crystalline Mo$…
A major challenge in spintronics is to find an efficient means to manipulate antiferromagnet (AFM) states, which are inert relative to a uniform magnetic field, due to the vanishingly-small net magnetization. The question is, how does an AFM response to an inhomogeneous field? Here we address the problem through a complete classification of the magnetic forces on an AFM domain wall (DW), revealing the following physical properties: (i) the tiny net magnetization still responses to the field gradient. (ii) the Néel order is sensitive to the field difference between two sublattices. (iii) DW ene…
Iron phthalocyanine (FePc) is a molecular semiconductor whose building blocks are one-dimensional ferromagnetic chains. We show that its optical and magnetic properties are controlled by the growth strategy, obtaining extremely high coercivities of over 1 T and modulating the exchange constant between 15 and 29 K through tuning the crystal phase by switching from organic molecular beam deposition, producing continuous thin films of nanocrystals with controlled orientations, to organic vapour phase deposition, producing ultralong nanowires. Magnetisation measurements are analysed using a suite …
By comparing femtosecond laser pulse induced ferro- and antiferromagnetic dynamics in one and the same material - metallic dysprosium - we show both to behave fundamentally different. Antiferromagnetic order is considerably faster and much more efficiently manipulated by optical excitation than its ferromagnetic counterpart. We assign the fast and extremely efficient process in the antiferromagnet to an interatomic transfer of angular momentum within the spin system. Our findings do not only reveal this angular momentum transfer channel effective in antiferromagnets and other magnetic structur…
Magnetotransport investigation of a half-Heusler antiferromagnet DyPdBi revealed hallmark features of Weyl semimetal: huge negative longitudinal magnetoresistance and planar Hall effect. Both effects have recently been linked to chiral magnetic anomaly - axial charge pumping between Weyl nodes. Magnetoresistance (MR) of single crystals of DyPdBi is very pronounced. In magnetic field longitudinal to electrical current direction it reaches -80% and its relative difference with respect to that measured in transverse field (expressed as anisotropic magnetoresistance) is extremely strong: -60% at 1…
Wireless technology relies on the conversion of alternating electromagnetic fields to direct currents, a process known as rectification. While rectifiers are normally based on semiconductor diodes, quantum mechanical non-reciprocal transport effects that enable highly controllable rectification have recently been discovered. One such effect is magnetochiral anisotropy (MCA), where the resistance of a material or a device depends on both the direction of current flow and an applied magnetic field. However, the size of rectification possible due to MCA is usually extremely small, because MCA rel…
We report the electronic and magnetic behaviour of the frustrated triangular metallic antiferromagnet 2H-AgNiO2 in high magnetic fields (54 T) using thermodynamic and transport measurements. Here localized d electrons are arranged on an antiferromagnetic triangular lattice nested inside a honeycomb lattice with itinerant d electrons. When the magnetic field is along the easy axis we observe a cascade of field-induced transitions, attributed to the competition between easy-axis anisotropy, geometrical frustration and coupling of the localized and itinerant system. The quantum oscillations data …
The electron spin resonance (ESR) spectroscopy was employed to investigate the spin dynamics in triangular lattice antiferromagnets CuCr$_{1-x}$Mg$_{x}$O$_2$ with $x =$ 0 and 0.02. All spectra can be well fitted by a single Lorentzian lineshape. The analysis of the $g$ factor, the linewidth $\bigtriangleup H$, and the ESR intensity $I$ as a function of temperature suggests the development of significant antiferromagnetic (AFM) spin fluctuations at temperature well above $T_N$ in both samples. However, the evolution of the AFM spin fluctuations is different for each sample. For undoped sample t…
Searching for a high anomalous Nernst effect (ANE) is crucial for thermoelectric energy conversion applications because the associated unique transverse geometry facilitates module fabrication. Topological ferromagnets with large Berry curvatures show high ANEs; however, they face drawbacks such as strong magnetic disturbances and low mobility due to high magnetization. Herein, we demonstrate that YbMnBi2, a canted antiferromagnet, has a large ANE conductivity of ~10 Am-1K-1 that surpasses the common high values (i.e. 3-5 Am-1K-1) observed so far in ferromagnets. The canted spin structure of M…
Single crystals of $R$Cd$_{0.67}$As$_2$ ($R$ = La and Ce) have been synthesized by high temperature ternary melt and their physical properties have been explored by means of magnetization, specific heat, electrical resistivity, Hall coefficient, and thermoelectric power measurements. $R$Cd$_{0.67}$As$_2$ compounds indicate a (structural) phase transition at high temperatures, accompanied by a remarkable increase of the electrical resistivity with an extremely low carrier concentration. CeCd$_{0.67}$As$_2$ exhibits a large magnetic anisotropy and an antiferromagnetic (AFM) order below $T_{N} = …
Quantum anomalous Hall (QAH) phase is a two-dimensional bulk ferromagnetic insulator with a nonzero Chern number in presence of spin-orbit coupling (SOC) but absence of applied magnetic fields. Associated metallic chiral edge states host dissipationless current transport in electronic devices. This intriguing QAH phase has recently been observed in magnetic impurity-doped topological insulators, {\it albeit}, at extremely low temperatures. Based on first-principles density functional calculations, here we predict that layered rhodium oxide K$_{0.5}$RhO$_2$ in noncoplanar chiral antiferromagnet…
For the innovation of spintronic technologies, Dirac materials, in which the low-energy excitation is described as relativistic Dirac fermions, are one of the most promising systems, because of the fascinating magnetotransport associated with the extremely high mobility. To incorporate Dirac fermions into spintronic applications, their quantum transport phenomena are desired to be manipulated to a large extent by magnetic order in a solid. We here report a bulk half-integer quantum Hall effect in a layered antiferromagnet EuMnBi$_2$, in which field-controllable Eu magnetic order significantly …
Spin superfluid is a novel emerging quantum matter arising from the Bose-Einstein condensate (BEC) of spin-1 bosons. We demonstrate the spin superfluid ground state in canted antiferromagnetic Cr2O3 thin film at low temperatures via nonlocal spin transport. A large enhancement of the nonlocal spin signal is observed below ~ 20 K, and it saturates from ~ 5 K down to 2 K. We show that the spins can propagate over very long distances (~ 20 micro meters) in such spin superfluid ground state and the nonlocal spin signal decreases very slowly as the spacing increases with an inverse relationship, wh…
As a collective quasiparticle excitation of the magnetic order in magnetic materials, spin wave, or magnon when quantized, can propagate in both conducting and insulating materials. Like the manipulation of its optical counterpart, the ability to manipulate spin wave polarization is not only important but also fundamental for magnonics. With only one type of magnetic lattice, ferromagnets can only accommodate the right-handed circularly polarized spin wave modes, which leaves no freedom for polarization manipulation. In contrast, antiferromagnets, with two opposite magnetic sublattices, have b…
We show that the antiferromagnetic structure in the quantum spin trimer system ${{\rm Ca_{3}CuNi_2(PO_4)_4}}$ is based on both arms of propagation vector $\vec{k}$ star $\{[{1\over2},{1\over2},0],[-{1\over2},{1\over2},0]\}$ of the paramagnetic space group $C2/c$. The structure is generated by a symmetric direction of the order parameter of two dimensional irreducible representation of $C2/c$ with one active magnetic mode and corresponds to the Shubnikov magnetic space group $C_a2/c$. We reveal the relation between representation analysis in the propagation vector formalism and Shubnikov symmet…
