Mike Pols

We use symmetry arguments combined with density functional theory to demonstrate that all surfaces of crystalline materials host surface phonons that are chiral. As model system, we study slabs of highly symmetric AB rocksalt compounds, and find surface-localized phonons whose atomic displacements exhibit chiral motion. We further show that these chiral surface phonons generate sheets of in-plane magnetism at the surface. Our results reveal that chiral phonons can emerge in all crystalline materials as a result of reduced symmetry at surfaces or interfaces. These findings establish surfaces as a previously overlooked source of chiral phonons and their associated magnetic moments, which could play a role in a broad range of surface-sensitive measurements.

Ferrons are a type of quasiparticle corresponding to elementary excitations of the ferroelectric order. Analogously to how magnons modulate and transport magnetization, ferrons modulate and transport electric polarization. Here, we introduce multiferrons as elementary excitations with both electric and magnetic character. Multiferrons lead to a tilt and elliptical precession of the polarization and at the same time create a magnetization through the mechanism of dynamical multiferroicity. Using first-principles calculations for LiNbO\(_{3}\), we show that the electric polarization of multiferrons is perpendicular to the equilibrium ferroelectric polarization, whereas the magnetization is parallel to it. Our calculations further demonstrate that multiferrons carry net electric and magnetic quadrupole and octupole moments, which we term multipolons. These multipolons could couple to internal multipolar degrees of freedom, for example in altermagnets, or to external probes such as neutrons, leading to potentially experimentally observable phenomena following coherent or thermal excitation of multiferrons.

Chiral two-dimensional (2D) halide perovskites are formed by embedding chiral organic cations in a perovskite crystal structure. The chirality arises from distortions of the 2D metal halide layers induced by the packing of these organic cations. Sn-based octahedra spontaneously distort, but it remains unclear whether this intrinsic structural instability enhances the chirality. We investigate the effect of the metal cation on structural and phonon chirality in MBA\(_{2}\)Sn\(_{x}\)Pb\(_{1-x}\)⁢I\(_{4}\) (x = 0, 1/2, and 1). Incorporating Sn does distort the metal halide octehedra, yet it only has a minor impact on the structural chirality. In contrast, the phonons in MBA\(_{2}\)SnI\(_{4}\) are substantially more chiral than in MBA\(_{2}\)SnI\(_{4}\), especially the in-plane acoustic modes. However, this enhanced phonon chirality does not lead to a generation of a larger angular momentum under a temperature gradient, because the contributions of different chiral phonons tend to compensate one another.

Phonons in chiral crystal structures can be circularly polarized, making them chiral. Chiral phonons carry angular momentum, which is observable in heat currents, and, via coupling to electron spin, in spin currents. Two-dimensional (2D) halide perovskites, versatile direct band gap semiconductors, can easily form chiral structures by incorporating chiral organic cations. As a result, they exhibit phenomena such as chirality-induced spin selectivity (CISS) and the spin Seebeck effect, although the underlying mechanisms remain unclear. Using on-the-fly machine-learning force fields trained against density functional theory calculations, we confirm the presence of chiral phonons, a potential key factor for these effects. Our analysis reveals that low-energy phonons, originating from the inorganic framework, primarily exhibit chirality. Under a temperature gradient, these chiral phonons generate substantial angular momentum, leading to experimentally observable effects. These findings position chiral 2D perovskites as a promising platform for exploring the interplay among phononic, electronic, spintronic, and thermal properties.

With the use of chiral organic cations in two-dimensional metal halide perovskites, chirality can be induced in the metal halide layers, which results in semiconductors with intriguing chiral optical and spin-selective transport properties. The chiral properties strongly depend upon the temperature, despite the basic crystal symmetry not changing fundamentally. We identify a set of descriptors that characterize the chirality of metal halide perovskites, such as MBA\(_{2}\)PbI\(_{4}\), and study their temperature dependence using molecular dynamics simulations with on-the-fly machine-learning force fields obtained from density functional theory calculations. We find that, whereas the arrangement of organic cations remains chiral upon increasing the temperature, the inorganic framework loses this property more rapidly. We ascribe this to the breaking of hydrogen bonds that link the organic with the inorganic substructures, which leads to a loss of chirality transfer.

The migration of defects plays an important role in the stability of halide perovskites. It is challenging to study defect migration with experiments or conventional computer simulations. The former lacks an atomic-scale resolution and the latter suffers from short simulation times or a lack of accuracy. Here, we demonstrate that machine-learned force fields, trained with an on-the-fly active learning scheme against accurate density functional theory calculations, allow us to probe the differences in the dynamical behaviour of halide interstitials and halide vacancies in two closely related compositions CsPbI\(_{3}\) and CsPbBr\(_{3}\). We find that interstitials migrate faster than vacancies, due to the shorter migration paths of interstitials. Both types of defects migrate faster in CsPbI\(_{3}\) than in CsPbBr\(_{3}\). We attribute this to the less compact packing of the ions in CsPbI\(_{3}\), which results in a larger motion of the ions and thus more frequent defect migration jumps.