Unconventional Phase Research Articles

Time-reversal symmetry-breaking superconductivity in epitaxial bismuth/nickel bilayers

Superconductivity that spontaneously breaks time-reversal symmetry (TRS) has been found, so far, only in a handful of three-dimensional (3D) crystals with bulk inversion symmetry. We report an observation of spontaneous TRS breaking in a 2D superconducting system without inversion symmetry: the epitaxial bilayer films of bismuth and nickel. The evidence comes from the onset of the polar Kerr effect at the superconducting transition in the absence of an external magnetic field, detected by the ultrasensitive loop-less fiber-optic Sagnac interferometer. Because of strong spin-orbit interaction and lack of inversion symmetry in a Bi/Ni bilayer, superconducting pairing cannot be classified as singlet or triplet. We propose a theoretical model where magnetic fluctuations in Ni induce the superconducting pairing of the [Formula: see text] orbital symmetry between the electrons in Bi. In this model, the order parameter spontaneously breaks the TRS and has a nonzero phase winding number around the Fermi surface, thus making it a rare example of a 2D topological superconductor.

Nonadiabatic geometric quantum computation in decoherence-free subspaces based on unconventional geometric phases

Nonadiabatic geometric quantum computation in decoherence-free subspaces has received increasing attention due to the merits of its high-speed implementation and robustness against both control errors and decoherence. However, all the previous schemes in this direction have been based on the conventional geometric phases, of which the dynamical phases need to be removed. In this paper, we put forward a scheme of nonadiabatic geometric quantum computation in decoherence-free subspaces based on unconventional geometric phases, of which the dynamical phases do not need to be removed. Specifically, by using three physical qubits undergoing collective dephasing to encode one logical qubit, we realize a universal set of geometric gates nonadiabatically and unconventionally. Our scheme not only maintains all the merits of nonadiabatic geometric quantum computation in decoherence-free subspaces, but also avoids the additional operations required in the conventional schemes to cancel the dynamical phases.

Gas-Phase Synthesis of the Elusive Trisilicontetrahydride Species (Si3H4).

The bimolecular gas-phase reaction of ground-state atomic silicon (Si; 3P) with disilane (Si2H6; 1A1g) was explored under single-collision conditions in a crossed molecular beam machine at a collision energy of 21 kJ mol-1. Combined with electronic structure calculations, the results suggest the formation of Si3H4 isomer(s) along with molecular hydrogen via indirect scattering dynamics through Si3H6 collision complex(es) and intersystem crossing from the triplet to the singlet surface. The nonadiabatic reaction dynamics can synthesize the energetically accessible singlet Si3H4 isomers in overall exoergic reaction(s) (-93 ± 21 kJ mol-1). All reasonable reaction products are either cyclic or hydrogen-bridged suggesting extensive isomerization processes from the reactants via the initially formed collision complex(es) to the fragmenting singlet intermediate(s). The underlying chemical dynamics of the silicon-disilane reaction are quite distinct from the isovalent carbon-ethane system that does not depict any reactivity at all, and open the door for an unconventional gas phase synthesis of hitherto elusive organosilicon molecules under single-collision conditions.

Geometry induced sequence of nanoscale Frank–Kasper and quasicrystal mesophases in giant surfactants

Frank-Kasper (F-K) and quasicrystal phases were originally identified in metal alloys and only sporadically reported in soft materials. These unconventional sphere-packing schemes open up possibilities to design materials with different properties. The challenge in soft materials is how to correlate complex phases built from spheres with the tunable parameters of chemical composition and molecular architecture. Here, we report a complete sequence of various highly ordered mesophases by the self-assembly of specifically designed and synthesized giant surfactants, which are conjugates of hydrophilic polyhedral oligomeric silsesquioxane cages tethered with hydrophobic polystyrene tails. We show that the occurrence of these mesophases results from nanophase separation between the heads and tails and thus is critically dependent on molecular geometry. Variations in molecular geometry achieved by changing the number of tails from one to four not only shift compositional phase boundaries but also stabilize F-K and quasicrystal phases in regions where simple phases of spheroidal micelles are typically observed. These complex self-assembled nanostructures have been identified by combining X-ray scattering techniques and real-space electron microscopy images. Brownian dynamics simulations based on a simplified molecular model confirm the architecture-induced sequence of phases. Our results demonstrate the critical role of molecular architecture in dictating the formation of supramolecular crystals with "soft" spheroidal motifs and provide guidelines to the design of unconventional self-assembled nanostructures.

Decorated defect condensate: A window to unconventional quantum phases in Weyl semimetals

We investigate the unconventional quantum phase transitions in Weyl semimetals. The emergent boson fields, coupling with the Weyl fermion bilinears, contain a Wess-Zumino-Witten term or topological $\Theta$ term inherited from the momentum space monopoles carried by Weyl points. Three types of unconventional quantum critical points will be studied in order: (1) The transition between two distinct symmetry breaking phases whose criticality is beyond Landau's paradigm. (2) The transition between a symmetry breaking state to a topological ordered state. (3) The transition between $3d$ topological order phase to trivial disordered phase whose criticality could be traced back to a $Z_2$ symmetry breaking transition in $4d$. The essence of these unconventional critical points lies in the fact that the topological defect of an order parameter carries either a nontrivial quantum number or a topological term so the condensation of the defects would either break some symmetry or give rise to a topological order phase with nontrivial braiding statistics.

Re-entrant DNA gels.

DNA is acquiring a primary role in material development, self-assembling by design into complex supramolecular aggregates, the building block of a new-materials world. Using DNA nanoconstructs to translate sophisticated theoretical intuitions into experimental realizations by closely matching idealized models of colloidal particles is a much less explored avenue. Here we experimentally show that an appropriate selection of competing interactions enciphered in multiple DNA sequences results into the successful design of a one-pot DNA hydrogel that melts both on heating and on cooling. The relaxation time, measured by light scattering, slows down dramatically in a limited window of temperatures. The phase diagram displays a peculiar re-entrant shape, the hallmark of the competition between different bonding patterns. Our study shows that it is possible to rationally design biocompatible bulk materials with unconventional phase diagrams and tuneable properties by encoding into DNA sequences both the particle shape and the physics of the collective response.

Unusual Multiferroic Phase Transitions in PbTiO3 Nanowires.

Unconventional phases and their transitions in nanoscale systems are recognized as an intriguing avenue for both unique physical properties and novel technological paradigms. Although the multiferroic phase has attracted considerable attention due to the coexistence and cross-coupling of electric and magnetic order parameters, mutually exclusive mechanism between ferroelectricity and ferromagnetism leaves conventional ferroelectrics such as PbTiO3 simply nonmagnetic. Here, we demonstrate from first-principles that ultrathin PbTiO3 nanowires exhibit unconventional multiferroic phases with emerging ferromagnetism and coexisting ferroelectric/ferrotoroidic ordering. Nanometer-scale and nonstoichiometric effects intrinsic to the nanowires bring about nonzero and nontrivial magnetic moments that coexist with the host ferroelectricity. The multiferroic order is susceptible to surface termination and nanowire morphology. Furthermore, calculations suggest that the nanowires undergo size-dependent ferroelectric-multiferroic-ferromagnetic phase transitions. This work therefore provides a route to multiferroic transitions in conventional nonmagnetic ferroelectric oxides.

Liquid Crystal Ordering and Isotropic Gelation in Solutions of Four-Base-Long DNA Oligomers.

Liquid crystal ordering is reported in aqueous solutions of the oligomer 5'-ATTAp-3' and of the oligomer 5'-GCCGp-3'. In both systems, we quantitatively interpret ordering as stemming from the chaining of molecules via a "running-bond" type of pairing, a self-assembly process distinct from the duplex aggregation previously reported for longer oligonucleotides. While concentrated solutions of 5'-ATTAp-3' show only a columnar liquid crystal phase, solutions of 5'-GCCGp-3' display a rich phase diagram, featuring a chiral nematic phase analogous to those observed in solutions of longer oligonucleotides and two unconventional phases, a columnar crystal and, at high concentration, an isotropic amorphous gel. The appearance of these phases, which can be interpreted on the basis of features of 5'-GCCGp-3'molecular structure, suggests distinctive assembly motifs specific to ultrashort oligonucleotides.

Universal optical conductivity of a disordered Weyl semimetal.

Topological Weyl semimetals, besides manifesting chiral anomaly, can also accommodate a disorder-driven unconventional quantum phase transition into a metallic phase. A fundamentally and practically important question in this regard concerns an experimentally measurable quantity that can clearly distinguish these two phases. We show that the optical conductivity while serving this purpose can also play the role of a bonafide order parameter across such disorder-driven semimetal-metal quantum phase transition by virtue of displaying distinct scaling behavior in the semimetallic and metallic phases, as well as inside the quantum critical fan supporting a non-Fermi liquid. We demonstrate that the correction to the dielectric constant and optical conductivity in a dirty Weyl semimetal due to weak disorder is independent of the actual nature of point-like impurity scatterers. Therefore, optical conductivity can be used as an experimentally measurable quantity to study the critical properties and to pin the universality class of the disorder-driven quantum phase transition in Weyl semimetals.

Superconductivity in doped Dirac semimetals

We theoretically study intrinsic superconductivity in doped Dirac semimetals. Dirac semimetals host bulk Dirac points, which are formed by doubly degenerate bands, so the Hamiltonian is described by a $4 \times 4$ matrix and six types of $k$-independent pair potentials are allowed by the Fermi-Dirac statistics. We show that the unique spin-orbit coupling leads to characteristic superconducting gap structures and $d$ vectors on the Fermi surface and the electron-electron interaction between intra and interorbitals gives a novel phase diagram of superconductivity. It is found that when the inter-orbital attraction is dominant, an unconventional superconducting state with point nodes appears. To verify the experimental signature of possible superconducting states, we calculate the temperature dependence of bulk physical properties such as electronic specific heat and spin susceptibility and surface state. In the unconventional superconducting phase, either dispersive or flat Andreev bound states appear between point nodes, which leads to double peaks or single peak in the surface density of states, respectively. As a result, possible superconducting states can be distinguished by combining bulk and surface measurements.

Predicted Quantum Topological Hall Effect and Noncoplanar Antiferromagnetism in K_{0.5}RhO_{2}.

The quantum anomalous Hall (QAH) phase is a two-dimensional bulk ferromagnetic insulator with a nonzero Chern number in the presence of spin-orbit coupling (SOC) but in the 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, 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 the noncoplanar chiral antiferromagnetic state is an unconventional three-dimensional QAH insulator with a large band gap and a Néel temperature of a few tens of Kelvins. Furthermore, this unconventional QAH phase is revealed to be the exotic quantum topological Hall effect caused by nonzero scalar spin chirality due to the topological spin structure in the system and without the need of net magnetization and SOC.

An unconventional phase field modeling of domains formation and evolution in tetragonal ferroelectrics

Based on characteristic functions of variants, we developed an unconventional phase field modeling for investigating domains formation and evolution in tetragonal ferroelectrics. In order to develop this computational approach, we constructed the anisotropy energy of tetragonal variants, which is used instead of Landau-Devonshire potential in the conventional phase field method, resulting in that much fewer parameters are needed for simulations. This approach is advantageous in simulations of emerging ferroelectric materials. We employ it to study the formation and evolution of domains in tetragonal barium titanate single crystal, as well as the nonlinear behaviors under cyclical stress and electric field loading. A multi-rank laminated ferroelectric domain pattern, 90° domain switching accompanied by polarization rotation, and 180° domain switching accompanied by move of domain wall are predicted. It is found that the speed of 90° domain switching is slower than that of 180° domain switching, due to both polarization and transformation strain changed in 90° domain switching. It also suggests that large strain actuation can be generated in single crystal ferroelectrics via combined electromechanical loading inducing 90° domain switching. The good agreement between simulation results and experimental measurements is observed.

Variation of optical conductivity spectra in the course of bandwidth-controlled metal-insulator transitions in pyrochlore iridates

We spectroscopically investigate a series of pyrochlore iridates ${R}_{2}{\mathrm{Ir}}_{2}{\mathrm{O}}_{7}$ ($R$: rare-earth and Y ions) where the metal-insulator transitions are induced by systematic bandwidth control via chemical substitutions of $R$ ions. We establish the phase diagram of ${R}_{2}{\mathrm{Ir}}_{2}{\mathrm{O}}_{7}$, as endorsed by the variation of the optical conductivity spectra, in which the competing phases including paramagnetic insulator (PI), paramagnetic metal (PM), and antiferromagnetic insulator (AFI) show up as a function of bandwidth and temperature. For small $R$-ionic radius ($R=$ Y-Sm), i.e., strongly correlated region, pronounced peaks on the edge of the optical gap are discerned below the magnetic transition temperature ${T}_{\mathrm{N}}$, which is attributable to exciton and magnon sideband absorptions. It turns out that the estimated nearest-neighbor exchange interaction increases as $R$-ionic radius increases, whereas ${T}_{\mathrm{N}}$ monotonically decreases, indicating that the all-in all-out magnetic order arises from the interplay among several exchange interactions inherent to extended $5d$ orbitals on the frustrated lattice. For larger $R$-ionic radius ($R=$ Sm-Pr), i.e., relatively weakly correlated region, the optical conductivity spectra markedly change below 0.3 eV in the course of PM-AFI transition, implying that the magnetic order induces the insulating state. In particular, we have found distinct electrodynamics in the composition of $R=\phantom{\rule{4pt}{0ex}}{\mathrm{Nd}}_{0.5}{\mathrm{Pr}}_{0.5}$ which is located on the boundary of the quantum PM-AFI transition, pointing to the possible emergence of unconventional topological electronic phases related possibly to the correlated Weyl electrons.

Orientational bond and Néel order in the two-dimensional ionic Hubbard model

Unconventional phases often occur where two competing mechanisms compensate. An excellent example is the ionic Hubbard model where the alternating local potential $\ensuremath{\delta}$, favoring a band insulator (BI), competes with the local repulsion $U$, favoring a Mott insulator (MI). By continuous unitary transformations we derive effective models in which we study the softening of various excitons. The softening signals the instability towards new phases that we describe on the mean-field level. On increasing $U$ from the BI in two dimensions, we find a bond-ordered phase breaking orientational symmetry due to a $d$-wave component. Then, antiferromagnetic order appears coexisting with the $d$-wave bond order. Finally, the $d$-wave order vanishes and a N\'eel-type MI persists.

Functional renormalization and mean-field approach to multiband systems with spin-orbit coupling: Application to the Rashba model with attractive interaction

The functional renormalization group (RG) in combination with Fermi surface patching is a well-established method for studying Fermi liquid instabilities of correlated electron systems. In this article, we further develop this method and combine it with mean-field theory to approach multiband systems with spin-orbit coupling, and we apply this to a tight-binding Rashba model with an attractive, local interaction. The spin dependence of the interaction vertex is fully implemented in a RG flow without SU(2) symmetry, and its momentum dependence is approximated in a refined projection scheme. In particular, we discuss the necessity of including in the RG flow contributions from both bands of the model, even if they are not intersected by the Fermi level. As the leading instability of the Rashba model, we find a superconducting phase with a singlet-type interaction between electrons with opposite momenta. While the gap function has a singlet spin structure, the order parameter indicates an unconventional superconducting phase, with the ratio between singlet and triplet amplitudes being plus or minus one on the Fermi lines of the upper or lower band, respectively. We expect our combined functional RG and mean-field approach to be useful for an unbiased theoretical description of the low-temperature properties of spin-based materials.

Conventional and Unconventional Pairing and Condensates in Dilute Nuclear Matter

This contribution will survey recent progress toward an understanding of diverse pairing phenomena in dilute nuclear matter at small and moderate isospin asymmetry, with results of potential relevance to supernova envelopes and proto-neutron stars. Application of ab initio many-body techniques has revealed a rich array of temperature-density phase diagrams, indexed by isospin asymmetry, which feature both conventional and unconventional superfluid phases. At low density there exist a homogeneous translationally invariant BCS phase, a homogeneous LOFF phase violating translational invariance, and an inhomogeneous translationally invariant phase-separated BCS phase. The transition from the BCS to the BEC phases is characterized in terms of the evolution, from weak to strong coupling, of the pairing gap, condensate wave function, and quasiparticle occupation numbers and spectra. Additionally, a schematic formal analysis of pairing in neutron matter at low to moderate densities is presented that establishes conditions for the emergence of both conventional and unconventional pairing solutions and encompasses the possibility of dineutron formation.

Multi-target-qubit unconventional geometric phase gate in a multi-cavity system.

Cavity-based large scale quantum information processing (QIP) may involve multiple cavities and require performing various quantum logic operations on qubits distributed in different cavities. Geometric-phase-based quantum computing has drawn much attention recently, which offers advantages against inaccuracies and local fluctuations. In addition, multiqubit gates are particularly appealing and play important roles in QIP. We here present a simple and efficient scheme for realizing a multi-target-qubit unconventional geometric phase gate in a multi-cavity system. This multiqubit phase gate has a common control qubit but different target qubits distributed in different cavities, which can be achieved using a single-step operation. The gate operation time is independent of the number of qubits and only two levels for each qubit are needed. This multiqubit gate is generic, e.g., by performing single-qubit operations, it can be converted into two types of significant multi-target-qubit phase gates useful in QIP. The proposal is quite general, which can be used to accomplish the same task for a general type of qubits such as atoms, NV centers, quantum dots, and superconducting qubits.

Topological phase transition of a fractal spin system: The relevance of the network complexity

A new type of collective excitations, due to the topology of a complex random network that can be characterized by a fractal dimension DF, is investigated. We show analytically that these excitations generate phase transitions due to the non-periodic topology of the DF > 1 complex network. An Ising system, with long range interactions, is studied in detail to support the claim. The analytic treatment is possible because the evaluation of the partition function can be decomposed into closed factor loops, in spite of the architectural complexity. The removal of the infrared divergences leads to an unconventional phase transition, with spin correlations that are robust against thermal fluctuations.

Cd2Re2O7under high pressure: Pyrochlore lattice distortion-driven metal-to-nonmetal transition

Pyrochlore ${\mathrm{Cd}}_{2}{\mathrm{Re}}_{2}{\mathrm{O}}_{7}$ has been investigated under high pressure by x-ray diffraction, resistivity and, mid-IR reflectance measurements. At $\ensuremath{\sim}14$ GPa, the high-temperature cubic pyrochlore phase [space group (SG): $Fd\overline{3}m$] undergoes a second-order transition to a rhombohedral structure (SG: $R\overline{3}m$) with trigonal distortion in its pyrochlore lattice. Temperature-dependent resistivity $\ensuremath{\rho}(T)$ reveals a large number of exotic electronic phases (including superconducting and unconventional metallic phases) in its $P\text{\ensuremath{-}}T$ phase diagram. At the metal-nonmetal boundary (at 21 GPa) the resistivity displays quadratic power-law behavior over a wide $T$ range with possible formation of heavy mass coherent quasiparticles. In the nonmetallic state $(d\ensuremath{\rho}/dTl0)$, the nondivergent and quadratic power-law resistivity as $T\ensuremath{\rightarrow}0$ reveals the novel character of the ground state. High-pressure optical conductivity measurement evidences electronic correlation playing the vital role in the emergence of the nonmetallic state as the electron-lattice coupling exceeds spin-orbit interaction due to large structural distortion.

Magnetic fluctuations driven insulator-to-metal transition in Ca(Ir(1-x)Rux)O3.

Magnetic fluctuations in transition metal oxides are a subject of intensive research because of the key role they are expected to play in the transition from the Mott insulator to the unconventional metallic phase of these materials, and also as drivers of superconductivity. Despite much effort, a clear link between magnetic fluctuations and the insulator-to-metal transition has not yet been established. Here we report the discovery of a compelling link between magnetic fluctuations and the insulator-to-metal transition in Ca(Ir1−xRux)O3 perovskites as a function of the substitution coefficient x. We show that when the material turns from insulator to metal, at a critical value of x ~ 0.3, magnetic fluctuations tend to change their character from antiferromagnetic, a Mott insulator phase, to ferromagnetic, an itinerant electron state with Hund’s orbital coupling. These results are expected to have wide-ranging implications for our understanding of the unconventional properties of strongly correlated electrons systems.