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An array of nanoscale polar domains with varying conductance and that are electrically insulated by domain walls can be induced by the interplay of strain and defects in oxide thin films. Local perturbations in complex oxides, such as domain walls 1 , 2 , strain 3 , 4 and defects 5 , 6 , are of interest because they can modify the conduction or the dielectric and magnetic response, and can even promote phase transitions. Here, we show that the interaction between different types of local perturbations in oxide thin films is an additional source of functionality. Taking SrMnO 3 as a model system, we use nonlinear optics to verify the theoretical prediction that strain induces a polar phase, and apply density functional theory to show that strain simultaneously increases the concentration of oxygen vacancies. These vacancies couple to the polar domain walls, where they establish an electrostatic barrier to electron migration. The result is a state with locally structured room-temperature conductivity consisting of conducting nanosized polar domains encased by insulating domain boundaries, which we resolve using scanning probe microscopy. Our ‘nanocapacitor’ domains can be individually charged, suggesting stable capacitance nanobits with a potential for information storage technology.

SignificanceUnderstanding the relationship between entangled degrees of freedom (DOF) is a central problem in correlated materials and the possibility to influence their balance is promising toward realizing novel functionalities. In Sr2IrO4, the interaction between spin–orbit coupling and electron correlations induces an exotic ground state with magnetotransport properties promising for antiferromagnetic spintronics applications. Moreover, the coupling between orbital and spin DOF renders the magnetic structure sensitive to the Ir–O bond environment. To date, a detailed understanding of the microscopic spin-lattice and electron–phonon interactions is still lacking. Here, we use strain engineering to perturb the local lattice environment and, by tracking the response of the low-energy elementary excitations, we unveil the response of the microscopic spin and charge interactions. In the high spin–orbit-coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir–O bond geometry in Sr2IrO4 and perform momentum-dependent resonant inelastic X-ray scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low-energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven cross-over from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron–hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information toward the control of the ground state of complex oxides in the presence of high spin–orbit coupling.

Charge mediated magnetoelectric coupling mechanism in artificial multiferroics originates from interfacial charge modulation or ionic movement at a magnetic/dielectric interface. Despite the existence of several dielectric/ferroelectric systems that can be used in charge mediated artificial multiferroic systems, producing suitable systems with fast time responses still remains a challenge. Here we characterize the frequency response of stoichiometric and non-stoichiometric (low strain) Si3N4 thin film membranes, which can potentially be used as the dielectric layer in magnetoelectric devices, to determine the impact of depletion layers, charge traps and defect mobility on the high frequency (up to 100 MHz) interfacial charge modulation via screening. We find that the dielectric/magnetoelectric properties are largely dominated by extrinsic doping due to point defects. In particular, we find that non-stoichiometric Si3N4 has a dielectric behaviour that is dominated by charge traps and/or mobile ions. However, stoichiometric Si3N4 membranes show a reversible response to the applied bias electric field consistent with a doped semiconductor behaviour; at high frequencies, the intrinsic dielectric behaviour is reached, indicating that it may be suitable for high frequency magnetoelectric device applications. Our results show that minimising the impact of defects on the dielectric properties of magnetoelectric heterostructures is an important prerequisite for obtaining a high frequency magnetoelectric response.

Understanding the relationship between entangled degrees of freedom (DOF) is a central problem in correlated materials and the possibility to influence their balance is promising toward realizing novel functionalities. In Sr 2 IrO 4 , the interaction between spin–orbit coupling and electron correlations induces an exotic ground state with magnetotransport properties promising for antiferromagnetic spintronics applications. Moreover, the coupling between orbital and spin DOF renders the magnetic structure sensitive to the Ir–O bond environment. To date, a detailed understanding of the microscopic spin-lattice and electron–phonon interactions is still lacking. Here, we use strain engineering to perturb the local lattice environment and, by tracking the response of the low-energy elementary excitations, we unveil the response of the microscopic spin and charge interactions. In the high spin–orbit-coupled Sr 2 IrO 4 , the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir–O bond geometry in Sr 2 IrO 4 and perform momentum-dependent resonant inelastic X-ray scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low-energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr 2 IrO 4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven cross-over from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron–hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr 2 IrO 4 , originating from the modified hopping elements between the t 2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr 2 IrO 4 and provides valuable information toward the control of the ground state of complex oxides in the presence of high spin–orbit coupling.

In the high spin–orbit-coupled Sr₂IrO₄, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir–O bond geometry in Sr₂IrO₄ and perform momentum-dependent resonant inelastic X-ray scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low-energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr₂IrO₄ films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven cross-over from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron–hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr₂IrO₄, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr₂IrO₄ and provides valuable information toward the control of the ground state of complex oxides in the presence of high spin–orbit coupling.

Local perturbations in complex oxides, such as domain walls, strain and defects, are of interest because they can modify the conduction or the dielectric and magnetic response, and can even promote phase transitions. Here, we show that the interaction between different types of local perturbations in oxide thin films is an additional source of functionality. Taking SrMnO sub(3) as a model system, we use nonlinear optics to verify the theoretical prediction that strain induces a polar phase, and apply density functional theory to show that strain simultaneously increases the concentration of oxygen vacancies. These vacancies couple to the polar domain walls, where they establish an electrostatic barrier to electron migration. The result is a state with locally structured room-temperature conductivity consisting of conducting nanosized polar domains encased by insulating domain boundaries, which we resolve using scanning probe microscopy. Our 'nanocapacitor' domains can be individually charged, suggesting stable capacitance nanobits with a potential for information storage technology.

In the high spin-orbit coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir-O bond geometry in Sr2IrO4 and perform momentum-dependent Resonant Inelastic X-ray Scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven crossover from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron-hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information towards the control of the ground state of complex oxides in the presence of high spin-orbit coupling.

Ultrafast electron delocalization induced by a fs laser pulse is a well-known process and is the initial step for important applications such as fragmentation of molecules or laser ablation in solids. It is well understood that an intense fs laser pulse can remove several electrons from an atom within its pulse duration. [1] However, the speed of electron localization out of an electron gas, the capture of an electron by ion, is unknown. Here, we demonstrate that electronic localization out of the conduction band can occur within only a few hundred femtoseconds. This ultrafast electron localization into 4f states has been directly quantified by transient x-ray absorption spectroscopy following photo-excitation of a Eu based correlated metal with a fs laser pulse. Our x-ray experiments show that the driving force for this process is either an ultrafast reduction of the energy of the 4f states, a change of their bandwidth or an increase of the hybridization between the 4f and the 3d states. The observed ultrafast electron localization process raises further basic questions for our understanding of electron correlations and their coupling to the lattice.

A fundamental problem in origins of life research is how the first polymers with the properties of nucleic acids were synthesized and incorporated into living systems on the prebiotic Earth. Here, we show that RNA-like polymers can be synthesized non-enzymatically from 5′-phosphate mononucleosides in salty environments. The polymers were identified and analyzed by gel electrophoresis, nanopore analysis, UV spectra, and action of RNases. The synthesis of phosphodiester bonds is driven by the chemical potential made available in the fluctuating hydrated and anhydrous conditions of hydrothermal fields associated with volcanic land masses.

1. Ornamental horticulture is the primary pathway for invasive alien plant introductions. We critically appraise published evidence on the effectiveness of four policy instruments that tackle invasions along the horticulture supply chain: pre-border import restrictions, post-border bans, industry codes of conduct and consumer education. 2. Effective pre-border interventions rely on rigorous risk assessment and high industry compliance. Post-border sales bans become progressively less effective when alien species become widespread in a region. 3. A lack of independent performance evaluation and of public disclosure, limits the uptake and effectiveness of voluntary codes of conduct and discourages shifts in consumer preference away from invasive alien species. 4. Policy implications. Closing the plant invasion pathway associated with ornamental horticulture requires government-industry agreements to fund effective pre- and post-border weed risk assessments that can be subsequently supported by widely adopted, as well as verifiable, industry codes of conduct. This will ensure producers and consumers make informed choices in the face of better targeted public education addressing plant invasions.