Chiral States Research Articles

Quantum description of Fermi arcs in Weyl semimetals in a magnetic field

For a Weyl semimetal (WSM) in a magnetic field, a semiclassical description of the Fermi-arc surface state dynamics is usually employed for explaining various unconventional magnetotransport phenomena, e.g., Weyl orbits, the three-dimensional quantum Hall effect, and the high transmission through twisted WSM interfaces. For a half-space geometry, we determine the low-energy quantum eigenstates for a four-band model of a WSM in a magnetic field perpendicular to the surface. The eigenstates correspond to in- and out-going chiral Landau level (LL) states, propagating (anti)parallel to the field direction near different Weyl nodes, which are coupled by evanescent surface-state contributions generated by all other LLs. These replace the Fermi arc in a magnetic field. Computing the phase shift accumulated between in- and out-going chiral LL states, we compare our quantum-mechanical results to semiclassical predictions. We find quantitative agreement between both approaches. Published by the American Physical Society 2024

Quantum Valley Hall Effect without Berry Curvature.

The quantum valley Hall effect (QVHE) is characterized by the valley Chern number (VCN) in a way that one-dimensional (1D) chiral metallic states are guaranteed to appear at the domain walls (DW) between two domains with opposite VCN for a given valley. Although in the case of QVHE, the total Berry curvature (BC) of the system is zero, the BC distributed locally around each valley makes the VCN well defined as long as intervalley scattering is negligible. Here, we propose a new type of valley-dependent topological phenomenon that occurs when the BC is strictly zero at each momentum. Such zero Berry curvature (ZBC) QVHE is characterized by the valley Euler number (VEN) which is computed by integrating the Euler curvature around a given valley in two-dimensional (2D) systems with space-time inversion symmetry. 1D helical metallic states can be topologically protected at the DW between two domains with the opposite VENs when the DW configuration preserves either the mirror symmetry with respect to the DW or the combination of the DW space-time inversion and chiral symmetries. We establish the fundamental origin of ZBC QVHE. Also, by combining tight-binding model study and first-principles calculations, we propose stacked hexagonal bilayer lattices including h-BX (X=As, P) and large-angle twisted bilayer graphenes as candidate systems with robust helical DW states protected by VEN.

Phonon-Induced Geometric Chirality.

Chiral properties have seen increasing use in recent years, leading to the emerging fields of chiral quantum optics, plasmonics, and phononics. While these fields have achieved manipulation of the chirality of light and lattice vibrations, controlling the chirality of materials on demand has yet remained elusive. Here, we demonstrate that linearly polarized phonons can be used to induce geometric chirality in achiral crystals when excited with an ultrashort laser pulse. We show that nonlinear phonon coupling quasistatically displaces the crystal structure along phonon modes that reduce the symmetry of the lattice to that of a chiral point group corresponding to a chiral crystal. By reorienting the polarization of the laser pulse, the two enantiomers can be induced selectively. Therefore, geometric chiral phonons enable the light-induced creation of chiral crystal structures and therefore the engineering of chiral electronic states and optical properties.

Chiral quasi-bound states in the continuum for refractive-index sensing in metasurfaces

Chiral quasi-bound states in the continuum for refractive-index sensing in metasurfaces

Steering high-Q intrinsic chiral quasi-bound states in the continuum via engineered 2.5D phase-change metasurfaces.

High-Q intrinsic quasi-bound states in the continuum (QBICs) require three-dimensional (3D) geometries with both in-plane and out-of-plane mirror symmetry breakings, hindering practical implementations due to the complex architectures. Here we demonstrate that high-Q intrinsic QBICs can be flexibly controlled by using the engineered 2.5D phase-change metasurfaces of Ge2Sb2Te5 (GST). By introducing the additional out-of-plane perturbations of slant angle θ and azimuthal angle φ, highly efficient and high-Q intrinsic circular dichroism (CD) for both reflection and transmission can be realized. The spinning-selected magnetic dipole (MD) is responsible for the high-Q intrinsic chirality. The high-Q intrinsic CD is robust to the variation of structural parameters, and its Q-factor and resonance location can be tuned through the phase transition of GST.

Tilted-chiral-state-induced topological Hall effect in chiral magnetic soliton host Cr1/3TaS2

Chromium-intercalated Cr1/3TaS2 is well known for hosting a nontrivial chiral magnetic soliton lattice (CSL) with the reported highest Curie temperature (TC∼151 K) and strongest spin–orbit coupling, which has significant applications in gigahertz and high-speed spintronic devices. Herein, we thoroughly investigate the magneto-electrical transport properties of Cr1/3TaS2 single crystals. For H//ab, our magnetoresistance (MR) measurements reveal distinctive step-like behaviors, which are attributed to the formation and annihilation of chiral magnetic solitons. When under an oblique field, similar but weaker MR behaviors are observed compared to H//ab, indicating the appearance of an inclination-field-induced tilted-CSL. A topological Hall effect is observed under an oblique field, which is suggested to be induced by a nonzero topological charge density resulting from the tilted chiral states. The Cr1/3TaS2 offers an intriguing platform for studying the impact of chiral magnetic structures on magneto-electrical properties, which holds promise for both future spintronic device applications and fundamental investigation.

Chirality and Solvent Coassist the Structural Evolution of Hybrid Manganese Chlorides with Second-Harmonic-Generation Response.

Chiral hybrid metal halides have shown great potential in optoelectronics, including for spin splitting, circularly polarized luminescence, and nonlinear-optical properties. However, despite their inherent inversion symmetry breaking, studies on second harmonic generation (SHG) of chiral hybrid manganese(II) halides remain relatively rare. Here, we report a series of structurally diverse hybrid manganese(II) chlorides: (Rac-MBA)2[MnCl4(H2O)2] (1), (S-MBA)2[MnCl4(H2O)2] (2), (S-MBA)2[Mn2Cl6(H2O)4] (3), and (S-MBA)[MnCl3(MeOH)] (4), where MBA = α-methylbenzylammonium, providing tunability of the coordination environment and structural dimensionality via fine control of the MBA cation chiral state and crystal preparation process, thereby enabling modulation of the SHG effects. Specifically, as the amount of methanol increases during the crystal preparation process, the structures of the chiral compounds vary from a 0D structure consisting of isolated octahedra to a 0D structure composed of octahedra dimers and to 1D chains of edge-sharing Mn-centered octahedra. In contrast, the structure of the racemic compound remains unchanged, independent of the crystal preparation pathway. The structural details, including the coordination environment, H-bonding, dimensionality, and lattice distortion, are described. The SHG response of the racemic compound derives only from the inorganic lattice, while the responses of the chiral compounds are attributed to the synergetic effect of the chiral cations and inorganic moieties.

Magnetisation control of the nematicity direction and nodal points in a superconducting doped topological insulator

We study the effects of magnetisation on the properties of the doped topological insulator of the $\text{Bi}_2\text{Se}_3$ family with nematic superconductivity. We found that the direction of the in-plane magnetisation fixes the direction of the nematicity in the system. The chiral state is more favourable than the nematic state for large values of out-of-plane magnetisation. Overall, the critical temperature of the nematic superconductivity is robust against magnetisation. We explore in detail the spectrum of the system with the pinned direction of the nematic order parameter $\Delta_{y}$. Without magnetisation, there is a full gap in the spectrum because of finite hexagonal warping. At an out-of-plane $m_z$ or orthogonal in-plane $m_x$ magnetisation that is strong enough, the spectrum is closed at the nodal points that are split by the magnetisation. Flat Majorana surface states connect such split bulk nodal points. Parallel magnetisation $m_y$ lifts the nodal points and opens a full gap in the spectrum. We discuss relevant experiments and propose experimental verifications of our theory.

Strong coupling between excitons and chiral quasibound states in the continuum of the bulk WS2 metasurface.

In the fields of optics and photonics, the topic of light-matter interactions, particularly strong coupling effects, is a developing area of research. Exciton polariton, a hybridized state brought about by strong coupling, is a hot topic, especially from the standpoint of chiral optics. Under the incidence of right circularly polarized light and left circularly polarized (RCP and LCP) light, we investigate the strong coupling between excitons and quasibound states in the continuum (Q-BICs) resonance in a bulk WS2 metasurface. It is discovered that the Q-BICs are affected obviously on center frequencies and linewidth by structure parameters; while the exciton peaks are impacted insignificantly. Furtherly Q-BIC shows chiral enhancing features. When we take into account both Q-BIC and excitons of the metasurface simultaneously, there is a strong coupling as evidenced by the Rabi splitting up to 182 meV and the clear anti-crossing behavior in the transmittance and reflectance spectra of left and right circularly polarized light, respectively. Notably, a quasi-induced transparency window forms in the circular dichroism (CD) spectrum around the exciton band due to the non-chirality of exciton peaks. This enables the removal of excitons that are not involved in the strong coupling. The bulk WS2 chiral metasurface as a strong coupling system not only provides a way to understand the strong Light-matter interaction, but also generate a potential possibility for realizing the application of chiral optics. Additionally, it can realize the strong chiral coupling with a single self-hybridized element in the structure. Our results have potential implications in the chiral optical field and provide a chiral perspective on the study of strong photon-exciton coupling.

Organocatalysis for Enantioselective Decarboxylative Nucleophilic Addition Reactions

AbstractThe catalytic decarboxylation of malonic acid half oxy‐ and thioesters, β‐ketocarboxylic acids, and their related compounds is a straightforward, powerful, and atom‐economical strategy for the in‐situ formation of enolates, which are important and well‐studied synthons for various functional materials and natural products. This strategy, inspired by the biosynthesis of polyketides and fatty acids, is an attractive method for synthesizing enols from carboxyl compounds with less reactive α‐hydrogen atoms under mild conditions. In addition, these reactions are environmentally friendly and are of great interest to chemists because the use of a stoichiometric amount of base can be avoided, and the only byproduct is CO2. Thus far, remarkable progress has been made, especially in the field of organocatalytic enantioselective decarboxylation reactions, allowing for the stereocontrolled formation of new C−H, C−C, C−heteroatom, and C−X bonds. This review provides a comprehensive overview of organocatalytic enantioselective decarboxylation reactions and highlights the significant progress made since 2020. In particular, it focuses on chiral catalyst systems and transition states as key parameters for decarboxylation reactions.

Tailoring directional chiral emission from molecules coupled to extrinsic chiral quasi-bound states in the continuum

Tailoring directional chiral emission from molecules coupled to extrinsic chiral quasi-bound states in the continuum

Chiral Bell-State Transfer via Dissipative Liouvillian Dynamics.

Chiral state transfer along closed loops in the vicinity of an exceptional point is one of the many counterintuitive observations in non-Hermitian physics. The application of this property beyond proof-of-principle in quantum physics, is an open question. In this work, we demonstrate chiral state conversion between singlet and triplet Bell states through fully quantum Liouvillian dynamics. Crucially, we demonstrate that this property can be used for the chiral production of Bell states from separable states with a high fidelity and for a large range of parameters. Additionally, we show that the removal of quantum jumps from the dynamics through postselection can result in near-perfect Bell states from initially separable states. Our work presents the first application of chiral state transfer in quantum information processing and demonstrates a novel way to control entangled states by means of dissipation engineering.

Design of tunable selective light-absorbing metasurfaces driven by intrinsically chiral quasi-bound states in the continuum.

Chiral metasurfaces with high quality factors (Q-factors) and strong circular dichroism (CD) are excellent platforms for studying chiral optical response. Here, a design is proposed of an intrinsic chiral silicon metasurface driven by bound states in the continuum (BIC), with ultra-high Q-factor (Q = 3722) and chirality response close to the unit CD (CD > 0.99). By breaking the in-plane and out-of-plane symmetry of the structure, the intrinsic chirality based on BIC can be precisely controlled. In addition to studying intrinsic chirality, we have also achieved extrinsic chirality by obliquely incident circularly polarized light without introducing out-of-plane asymmetry. Moreover, we introduce graphene into the intrinsically chiral metasurface to form a graphene-Si hybridized metasurface. Selective absorption of intensity-controlled right-handed/left-handed circularly polarized light (RCP/LCP) was achieved by actively tuning the Fermi level and out-of-plane tilt angle of the graphene structure based on coupled-mode theory. Our research provides another insight into the application of intrinsic optical chirality, which is expected to be widely used in the fields of optical filters, polarization detectors, and chiral imaging.

Multiple Chirality Switching of a Dye‐Grafted Helical Polymer Film Driven by Acid & Base

AbstractA stimuli‐responsive multiple chirality switching material, which can regulate opposed chiral absorption characteristics, has great application value in the fields of optical modulation, information storage and encryption, etc. However, due to the rareness of effective functional systems and the complexity of material structures, developing this type of material remains an insurmountable challenge. Herein, a smart polymer film with multiple chirality inversion properties was fabricated efficiently based on a newly‐designed acid & base‐sensitive dye‐grafted helical polymer. Benefited from the cooperative effects of various weak interactions (hydrogen bonds, electrostatic interaction, etc.) under the aggregated state, this polymer film exhibited a promising acid & base‐driven multiple chirality inversion property containing record switchable chiral states (up to five while the solution showed three‐state switching) and good reversibility. The creative exploration of such a multiple chirality switching material can not only promote the application progress of current chiroptical regulation technology, but also provide a significant guidance for the design and synthesis of future smart chiroptical switching materials and devices.

Magnetic order in the computational 2D materials database (C2DB) from high throughput spin spiral calculations

We report high throughput computational screening for magnetic ground state order in 2D materials. The workflow is based on spin spiral calculations and yields the magnetic order in terms of a two-dimensional ordering vector Q. We then include spin-orbit coupling to extract the easy and hard axes for collinear structures and the orientation of spiral planes in non-collinear structures. Finally, for all predicted ferromagnets we compute the Dzyaloshinskii-Moriya interactions and determine whether or not these are strong enough to overcome the magnetic anisotropy and stabilise a chiral spin spiral ground state. We find 58 ferromagnets, 21 collinear anti-ferromagnets, and 85 non-collinear ground states of which 15 are chiral spin spirals driven by Dzyaloshinskii-Moriya interactions. The results show that non-collinear order is in fact as common as collinear order in these materials and emphasise the need for detailed investigation of the magnetic ground state when reporting magnetic properties of new materials.

Multiple Chirality Switching of a Dye-Grafted Helical Polymer Film Driven by Acid & Base.

A stimuli-responsive multiple chirality switching material, which can regulate opposed chiral absorption characteristics, has great application value in the fields of optical modulation, information storage and encryption, etc. However, due to the rareness of effective functional systems and the complexity of material structures, developing this type of material remains an insurmountable challenge. Herein, a smart polymer film with multiple chirality inversion properties was fabricated efficiently based on a newly-designed acid & base-sensitive dye-grafted helical polymer. Benefited from the cooperative effects of various weak interactions (hydrogen bonds, electrostatic interaction, etc.) under the aggregated state, this polymer film exhibited a promising acid & base-driven multiple chirality inversion property containing record switchable chiral states (up to five while the solution showed three-state switching) and good reversibility. The creative exploration of such a multiple chirality switching material can not only promote the application progress of current chiroptical regulation technology, but also provide a significant guidance for the design and synthesis of future smart chiroptical switching materials and devices.

Proximity-encirclement of exceptional points in a multimode optomechanical system

Dynamic encirclement of second-order exceptional points (EPs) exhibits chiral state transfer; however, investigations into the dynamics involving multiple and higher-order EPs remain sparse. Here, we study the proximity-encirclement of EPs within a multimode optomechanical system to elucidate the closed-path evolution in high-order non-Hermitian systems. Our optomechanical framework presents three distinct EP scenarios: absence of EPs, presence of a pair of second-order EPs, and the existence of a third-order EP. We meticulously analyze the system’s dynamic behavior, considering variables such as initial state, loop orientation and velocity, loop starting point variance, and the number and order of encircled EPs during state transfer processes. The findings reveal that chiral or non-reciprocal state transfer can be achieved when a loop encircles a second-order EP with varying radii. Encircling two second-order EPs results exclusively in chiral state transfer. Furthermore, both chiral and non-reciprocal state transfers are observed within a single loop encircling a third-order EP. These phenomena in the context of multimode optomechanical systems provide a new approach for manipulating state transfer in higher-order non-Hermitian systems.

Time-Dependent Extension of Grimme's Continuous Chirality Measure for Electronic Chirality Flips in Femto- and Attosecond Time Domains.

Grimme's Continuous Chirality Measure ( ) was developed for comparisons of the chirality of the electronic wave functions of molecules, typically in their ground states. For example, , and for alanine, hydrogen-peroxide, and for achiral molecules, respectively. Well-designed laser pulses can excite achiral molecules from the electronic ground state to time-dependent chiral superposition states, with chirality flips in the femto- or even attosecond (fs or as) time domains. Here we provide a time-dependent extension of Grimme's for trailing the electronic chirality flips. As examples, we consider two laser driven electronic wavefunctions which represent flips between opposite electronic enantiomers of oriented NaK within and . The corresponding vary respectively from or from to , and back.

Chemical Trends of the Bulk and Surface Termination-Dependent Electronic Structure of Metal-Intercalated Transition Metal Dichalcogenides.

The addition of metal intercalants into the van der Waals gaps of transition metal dichalcogenides has shown great promise as a method for controlling their functional properties. For example, chiral helimagnetic states, current-induced magnetization switching, and a giant valley-Zeeman effect have all been demonstrated, generating significant renewed interest in this materials family. Here, we present a combined photoemission and density-functional theory study of three such compounds: , , and , to investigate chemical trends of the intercalant species on their bulk and surface electronic structure. Our resonant photoemission measurements indicate increased hybridization with the itinerant NbS2-derived conduction states with increasing atomic number of the intercalant, leading to pronounced mixing of the nominally localized intercalant states at the Fermi level. Using spatially and angle-resolved photoemission spectroscopy, we show how this impacts surface-termination-dependent charge transfers and leads to the formation of new dispersive states of mixed intercalant-Nb character at the Fermi level for the intercalant-terminated surfaces. This provides an explanation for the origin of anomalous states previously reported in this family of compounds and paves the way for tuning the nature of the magnetic interactions in these systems via control of the hybridization of the magnetic ions with the itinerant states.

Direct flipping dynamics and quantized enrichment of chirality at single-molecule resolution.

Chirality is an important aspect of nature, and numerous macroscopic methods have been developed to understand and control chirality. For the chiral tertiary amines, their flexible flipping process makes it possible to achieve high chiral controllability without bond formation and breaking. Here, we present a type of stable chiral single-molecule devices formed by tertiary amines, using graphene-molecule-graphene single-molecule junctions. These single-molecule devices allow real-time, in situ, and long-time measurements of the flipping process of an individual chiral nitrogen center with high temporal resolution. Temperature- and bias voltage-dependent experiments, along with theoretical investigations, revealed diverse chiral intermediates, indicating the regulation of the flipping dynamics by energy-related factors. Angle-dependent measurements further demonstrated efficient enrichment of chiral states using linearly polarized light by a symmetry-related factor. This approach offers a reliable means for understanding the chirality's origin, elucidating microscopic chirality regulation mechanisms, and aiding in the design of effective drugs.