Ferroelectric ordering in liquids is a fundamental question of physics. Here, we show that ferroelectric ordering of the molecules causes the formation of recently reported splay nematic liquid-crystalline phase. As shown by dielectric spectroscopy, the transition between the uniaxial and the splay nematic phase has the characteristics of a ferroelectric phase transition, which drives an orientational ferroelastic transition via flexoelectric coupling. The polarity of the splay phase was proven by second harmonic generation imaging, which additionally allowed for determination of the splay modulation period to be of the order of 5–10 microns, also confirmed by polarized optical microscopy. The observations can be quantitatively described by a Landau–de Gennes type of macroscopic theory.

Recent experimental realization of ferroelectric nematic liquid crystalline phases stimulated material development and numerous experimental studies of these phases, guided by their fundamental and applicative interest. In this Perspective, we give an overview of this emerging field by linking history and theoretical predictions to a general outlook of the development and properties of the materials exhibiting ferroelectric nematic phases. We will highlight the most relevant observations to date, e.g., giant dielectric permittivity values, polarization values an order of magnitude larger than in classical ferroelectric liquid crystals, and nonlinear optical coefficients comparable with several ferroelectric solid materials. Key observations of anchoring and electro-optic behavior will also be examined. The collected contributions lead to a final discussion on open challenges in materials development, theoretical description, experimental explorations, and possible applications of the ferroelectric phases.

Different liquid crystalline phases with long-range orientational but not positional order, so-called nematic phases, are scarce. New nematic phases are rarely discovered, and such an event inevitably generates much interest. Here, we describe a transition from a uniaxial to a novel nematic phase characterized by a periodic splay modulation of the director. In this new nematic phase, defect structures not present in the uniaxial nematic phase are observed, which indicates that the new phase has lower symmetry than the ordinary nematic phase. The phase transition is weakly first order, with a significant pretransitional behavior, which manifests as strong splay fluctuations. When approaching the phase transition, the splay nematic constant is unusually low and goes towards zero. Analogously to the transition from the uniaxial nematic to the twist-bend nematic phase, this transition is driven by instability towards splay orientational deformation, resulting in a periodically splayed structure. And, similarly, a Landau-de Gennes type of phenomenological theory can be used to describe the phase transition. The modulated splay phase is biaxial and antiferroelectric.

Nematic liquid crystals have been known for more than a century, but it was not until the 60s–70s that, with the development of room temperature nematics, they became widely used in applications. Polar nematic phases have been long-time predicted, but have only been experimentally realized recently. Synthesis of materials with nematic polar ordering at room temperature is certainly challenging and requires a deep understanding of its formation mechanisms, presently lacking. Here, we compare two materials of similar chemical structure and demonstrate that just a subtle change in the molecular structure enables denser packing of the molecules when they exhibit polar order, which shows that reduction of excluded volume is in the origin of the polar nematic phase. Additionally, we propose that molecular dynamics simulations are potent tools for molecular design in order to predict, identify and design materials showing the polar nematic phase and its precursor nematic phases.

The recent discovery of the ferroelectric nematic phase has opened the door to experimental investigation of one of the most searched liquid crystal phases in decades, with high expectations for future applications. However, at this moment, there are more questions than answers. In this work, we examine the formation and structure of large polar nematic domains of the ferroelectric nematic material RM734 in planar liquid crystals cells with different aligning agents and specifications. We observe that confining surfaces have a strong influence over the formation of different types of domains, resulting in various twisted structures of the nematic director. For those cells predominantly showing mm-scale domains, we investigate the optical and second harmonic generation switching behaviour under applications of electric fields with a special focus on in-plane fields perpendicular to the confinement media rubbing direction. In order to characterise the underlying structure, the polar optical switching behaviour is reproduced using a simplified model together with Berreman calculations. Graphical abstract

Liquid crystals, with their ability to self-assemble, strong response to an electric field and integrability into complex systems, are key materials in light-beam manipulation¹. The recently discovered ferroelectric nematic liquid crystals^2,3 also have considerable second-order optical nonlinearity, making them a potential material for nonlinear optics^4,5. Their use as sources of quantum light could considerably extend the boundaries of photonic quantum technologies⁶. However, spontaneous parametric down-conversion, the basic source of entangled photons⁷, heralded single photons⁸ and squeezed light⁹, has so far not been observed in liquid crystals—or in any liquids or organic materials. Here we implement spontaneous parametric down-conversion in a ferroelectric nematic liquid crystal and demonstrate electric-field tunable broadband generation of entangled photons, with an efficiency comparable to that of the best nonlinear crystals. The emission rate and polarization state of photon pairs is markedly varied by applying a few volts or twisting the molecular orientation along the sample. A liquid-crystal source enables a special type of quasi-phase matching¹⁰, which is based on the molecular twist structure and is therefore reconfigurable for the desired spectral and polarization properties of photon pairs. Such sources promise to outperform standard nonlinear optical materials in terms of functionality, brightness and the tunability of the generated quantum state. The concepts developed here can be extended to complex topological structures, macroscopic devices and multi-pixel tunable quantum light sources.