Two-dimensional (2D) van-der-Waals (vdW) layered ferroelectric semiconductors are highly desired for in-memory computing and ferroelectric photovoltaics or detectors. Beneficial from the weak interlayer vdW-force, controlling the structure by interlayer twist/translation or doping is an effective strategy to manipulate the fundamental properties of 2D-vdW semiconductors, which has contributed to the newly-emerging sliding ferroelectricity. Here, we report unconventional room-temperature ferroelectricity, both out-of-plane and in-plane, in vdW-layered γ-InSe semiconductor triggered by yttrium-doping (InSe:Y). We determine an effective piezoelectric constant of ∼7.5 pm/V for InSe:Y flakes with thickness of ∼50 nm, about one order of magnitude larger than earlier reports. We directly visualize the enhanced sliding switchable polarization originating from the fantastic microstructure modifications including the stacking-faults elimination and a subtle rhombohedral distortion due to the intralayer compression and continuous interlayer pre-sliding. Our investigations provide new freedom degrees of structure manipulation for intrinsic properties in 2D-vdW-layered semiconductors to expand ferroelectric candidates for next-generation nanoelectronics. 

/pdf/sliding-ferroelectricity-in-van-der-waals-layered-g-inse-2wjngr4i.pdf

Sliding ferroelectricity in van der Waals layered γ-InSe semiconductor

Most nonferroelectric two-dimensional materials can be endowed with so-called sliding ferroelectricity via nonequivalent homobilayer stacking, which is not applicable to monoelement systems like pure graphene bilayer with inversion symmetry at any sliding vector. Herein, we show first-principles evidence that multilayer graphene with N>3 can all be ferroelectric, where the polarizations of polar states stem from the symmetry breaking in stacking configurations of across layer instead of adjacent layer, which are electrically switchable via interlayer sliding. The nonpolar states can also be electrically driven to polar states via sliding, and more diverse states with distinct polarizations will emerge in more layers. In contrast to the ferroelectric moiré domains with opposite polarization directions in twisted bilayers reported previously, the moiré pattern in some multilayer graphene systems (e.g., twisted monolayer-trilayer graphene) possess nonzero net polarizations with domains of the same direction separated by nonpolar regions, which can be electrically reversed upon interlayer sliding. The distinct moiré bands of two polar states should facilitate electrical detection of such sliding moiré ferroelectricity during switching.Received 10 April 2023Accepted 21 July 2023DOI:https://doi.org/10.1103/PhysRevLett.131.096801© 2023 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasFerroelectricityFirst-principles calculationsTwistronicsPhysical SystemsGrapheneCondensed Matter, Materials & Applied Physics 

Atypical Sliding and Moiré Ferroelectricity in Pure Multilayer Graphene

Circularly polarized light (CPL) with the end of optical vector traveling along circumferential trajectory, shows left- and right-handedness, which transmits chiral information to materials via complicated CPL-matter interactions. Materials with circular dichroism respond to CPL illumination selectively with differential outputs that can be used to design novel photodetectors. Racemic or achiral compounds under CPL go through photodestruction, photoresolution and asymmetric synthesis pathways to generate enantiomeric bias and optical activity. By this strategy, helical polymers and chiral inorganic plasmonic nanostructures are synthesized directly, and their intramolecular folding and subsequent self-assembly are photo-modulable as well. In the aggregated state of self-assembly and liquid crystal phase, helical sense of the dynamic molecular packing is sensitive to enantiomeric bias brought by CPL, enabling the chiral amplification to supramolecular scale. In this review, we aim to systematically summarize and discuss the application-guided design strategies of CPL-responsive materials. Asymmetric synthesis, resolution and property-modulation of small organic compounds, polymers, inorganic nanoparticles, supramolecular assemblies and liquid crystals are highlighted based on the important developments during the last decades. Besides, applications of light-matter interactions including CPL detection and biomedical applications are also referred. This article is protected by copyright. All rights reserved.

Circularly Polarized Light Responsive Materials: Design Strategies and Applications.

Due to the pronounced anisotropic response to circularly polarized light, chiral hybrid organic-inorganic metal halides have been regarded as promising candidates for the application in nonlinear chiroptics, especially for the second-harmonic generation circular dichroism (SHG-CD) effect. However, designing novel lead-free chiral hybrid metal halides with large anisotropy factors and high laser-induced damage thresholds (LDT) of SHG-CD remains challenging. Herein, we develop the first chiral hybrid germanium halide, (R/S-NEA)3 Ge2 I7 ⋅H2 O (R/S-NGI), and systematically investigated its linear and nonlinear chiroptical properties. S-NGI and R-NGI exhibit large anisotropy factors (gSHG-CD ) of 0.45 and 0.48, respectively, along with a high LDT of 38.46 GW/cm2 ; these anisotropy factors were the highest values among the reported lead-free chiral hybrid metal halides. Moreover, the effective second-order nonlinear optical coefficient of S-NGI could reach up to 0.86 pm/V, which was 2.9 times higher than that of commercial Y-cut quartz. Our findings facilitate a new avenue toward lead-free chiral hybrid metal halides, and their implementation in nonlinear chiroptical applications. 

Chiral Hybrid Germanium(II) Halide with Strong Nonlinear Chiroptical Properties.

Controlling molecular chirality by external stimuli is of great significance in both fundamental research and technological applications. Herein, we report a high-temperature (384 K) molecular ferroelectric of a Cu(II) complex whose spontaneous polarization can be switched associated with flipping of molecular chirality. In this two-dimensional perovskite structure, the inorganic layer is separated by (NH3(CH2)2SS(CH2)2NH3)2+ organic cations skewed in a chiral conformation (P- or M-helicity in an individual crystal). As the stereodynamic disulfide bridge determines the molecular dipole moment along the polar axis, the chiral organic cation can be converted to its enantiomer as a consequence of an electric field-induced shift of the S-S moiety relative to its screw axis during the ferroelectric switching. The variation of the molecular chirality is examined with single-crystal X-ray diffraction and circular dichroism spectra. The simultaneous switching of molecular chirality and spontaneous polarization in this perovskite ferroelectric may lead to novel chiral electronic phenomena.

Inversion of Molecular Chirality Associated with Ferroelectric Switching in a High-Temperature Two-Dimensional Perovskite Ferroelectric.

Sliding ferroelectricity is a recently observed polarity existing in two-dimensional materials. However, due to their weak polarization and poor electrical insulation in these materials, all available experimental evidence till now are indirect, with most based on transport properties in the nanoscale or piezoresponse force microscopy. We report the direct observation of sliding ferroelectricity, using a high-quality amphidynamic single crystal, (15-Crown-5)Cd$_3$Cl$_6$, which possesses a large band-gap and so allows direct measurement of P-E hysteresis. This coordination polymer is a van der Waals material, which is composed of inorganic stators and organic rotators as measured using XRD and NMR characterisation. From DFT calculations, we find that after the freezing of rotators an electric dipole is generated in each layer driven by the geometric mechanism, meanwhile a comparable ferroelectric polarization originates from the interlayer sliding. The net polarization of these two components can be directly measured and manipulated. Our finding provides insight into low-dimensional ferroelectrics, especially the controlling of synchronous dynamics of rotating molecules and sliding layers in solids. 

/pdf/direct-observation-of-geometric-and-sliding-ferroelectricity-2qsf8uyl.pdf

Direct observation of geometric and sliding ferroelectricity in an amphidynamic crystal

Direct detection of circularly polarized light (CPL) is a challenging task due to limited materials and ambiguous structure–property relationships that lead to low distinguishability of the light helicities. Perovskite ferroelectric semiconductors incorporating chirality provide new opportunities in dealing with this issue. Herein, a pair of 2D chiral perovskite ferroelectrics is reported, which have enhanced CPL detection performance due to interplays among lattice, photon, charge, spin, and orbit. The chirality‐transfer‐induced chiral&polar ferroelectric phase enhances the asymmetric nature of the photoactive sublattice and achieves a switchable self‐powered detection via the bulk photovoltaic effect. The single‐crystal‐based device exhibits a CPL‐sensitive detection performance under 430 nm with an asymmetric factor of 0.20 for left‐ and right‐CPL differentiation, about two times that of the pure chiral counterparts. The enhanced CPL detection performance is ascribed to the Rashba–Dresselhaus effect that originates from the bulk inversion asymmetry and strong spin–orbit coupling, shown with a large Rashba coefficient, which is demonstrated by density functional theory calculation and circularly polarized light excited photoluminescence measurement. These results provide new perspectives on chiral Rashba ferroelectric semiconductors for direct CPL detection and ferroelectrics‐based chiroptics and spintronics.

Chiral Rashba Ferroelectrics for Circularly Polarized Light Detection

Fast switching feature of spontaneous polarization (Ps) are one of the basis for ferroelectrics application in the field of data storage. However, most of molecular ferroelectrics behave low operating performance...

Fast Switching of Spontaneous Polarization in a Microporous Molecular Rotor Ferroelectric

Above room-temperature dielectric switching in a new Zn-halide hybrid crystal based on pyrrolidine-derivative†

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Direct observation of geometric and sliding ferroelectricity in an amphidynamic crystal

Chiral Rashba Ferroelectrics for Circularly Polarized Light Detection

Fast Switching of Spontaneous Polarization in a Microporous Molecular Rotor Ferroelectric

Above room-temperature dielectric switching in a new Zn-halide hybrid crystal based on pyrrolidine-derivative†