Bilayer Crystals Research Articles

Controllable Synthesis of Large-Area MoSe2 Monolayer Films and Bilayer Crystals

Controllable Synthesis of Large-Area MoSe₂ Monolayer Films and Bilayer Crystals

In-situ formation of polymer-stabilized/-free cholesteric bi-layer photonic crystal

Tunable photonic crystals based on cholesteric liquid crystals (CLCs) have attracted considerable attention due to their tunable optical properties and self-assembly capabilities. Despite the rapid development of various CLC-based devices, the narrow bandwidth of the photonic bandgap in CLCs limits their use in some practical applications. This paper presents a method for forming polymer-stabilized and polymer-free cholesteric bilayer photonic crystals in polymer-stabilized cholesteric liquid crystals (PSCLCs). By tuning the concentration of reactive monomers and controlling the UV polymerization conditions, two different PBGs can be formed within a single PSCLC cell. As the concentration of RM257 increases to 40 % and the intensity of UV light is used at 22 mW/cm2, the distance between the two reflectance bands can reach 200 nm, reflecting green and red light. The dynamic formation process and the tunability of these cholesteric bilayer structures under electric fields and temperature variations are investigated. By controlling the temperature and electric field, the reflectance of the liquid crystal layer can be reduced from 50 % to 15 %, resulting in a single-band reflection. In addition, we have proposed a tunable polarization volume grating based on the cholesteric bi-layer photonic crystal, which can diffract two specific light colors.

Control of Subband Energies via Interlayer Twisting in an Artificially Stacked WSe2 Bilayer.

Tuning the electronic structure of artificially stacked bilayer crystals using their twist angle has attracted a significant amount of interest. In this study, resonant tunneling spectroscopy was performed on trilayer WSe2/h-BN/twisted bilayer (tBL) WSe2 devices with a wide range of twist angles (θBL) of tBL WSe2, from 0° to 34°. We observed two resonant tunneling peaks, identified as the first and second lowest hole subbands at the valence band Γ point of tBL WSe2. The subband separation, which directly measured the interlayer coupling strength, was tuned by ∼0.1 eV as θBL increased toward 6° and remained nearly constant for larger θBL values. The θBL dependence was attributed to the emergence of a stable W/Se (Se/W) stacking domain in the small θBL region, owing to the atomic reconstruction of the moiré lattice in tBL WSe2. Our findings demonstrate that the twist-controlled subband energies in tBL WSe2 are predominantly determined by local atomic reconstruction.

Bilayer Crystals of Trapped Ions for Quantum Information Processing

Trapped-ion systems are a leading platform for quantum information processing, but they are currently limited to 1D and 2D arrays, which imposes restrictions on both their scalability and their range of applications. Here, we propose a path to overcome this limitation by demonstrating that Penning traps can be used to realize remarkably clean bilayer crystals, wherein hundreds of ions self-organize into two well-defined layers. These bilayer crystals are made possible by the inclusion of an anharmonic trapping potential, which is readily implementable with current technology. We study the normal modes of this system and discover salient differences compared to the modes of single-plane crystals. The bilayer geometry and the unique properties of the normal modes open new opportunities—in particular, in quantum sensing and quantum simulation—that are not straightforward in single-plane crystals. Furthermore, we illustrate that it may be possible to extend the ideas presented here to realize multilayer crystals with more than two layers. Our work increases the dimensionality of trapped-ion systems by efficiently utilizing all three spatial dimensions, and it lays the foundation for a new generation of quantum information processing experiments with multilayer 3D crystals of trapped ions. Published by the American Physical Society 2024

Phonon spectra split in vertically aligned bilayer crystal of binary complex plasma

Structural and dynamical properties of a bilayer binary strongly coupled dusty plasma system in a sheath of an rf discharge are experimentally investigated. Microparticles of two different sizes are aligned into vertical pairs due to ion focusing (plasma wakes) downstream from the upper particles in the ion flow toward the bottom electrode. The pairs are ordered into a 2D hexagonal crystalline structure. The collective mode dispersion relations are measured and analyzed. Splitting of the modes in the bilayer lattice is observed and theoretically described. The relative intensities of the mode branches reflect non-reciprocal features of the wake-mediated interaction between the microparticles. The conditions of stability of vertically aligned bilayer structure are discussed, and relevant plasma parameters are estimated.

Low-loss plasmonic resonance using surface Bloch waves in photoplasmonic metamaterials

We present a method for the suppression of the radiative loss of plasmonic resonant modes by efficiently coupling them with the nonradiative Bloch surface waves in photoplasmonic metamaterials, comprised of a 2D array of plasmonic resonators deposited on the low-index termination layer of a 1D photonic crystal. The number of photonic crystal bilayers plays a crucial role in the plasmonic radiative loss, with Q-values increasing with incrementing photonic crystal bilayers reaching values of ∼580 in the UV-Vis regime. We also show that the fundamental plasmonic mode of the metamaterial split into different energy levels corresponding to surface Bloch waves associated with each bilayer of the photonic crystal.

Non-reciprocal selective frequency transmission with nonlinear bi-layer cylinder chains

Recent advancements in wave physics have led to the development of systems that break the principle of wave transmission reciprocity. In this study, we present selective frequency transmission with asymmetry in bi-layer phononic crystals, which are composed of two layers of cylinder contact chains. We demonstrate significant non-reciprocal harmonic transmission effects, as well as self-demodulated displacement amplification under excitation from different sides. These effects are achieved through a combination of contact nonlinearity and cascaded bandgaps formed by adjusting the chain lengths in both layers. We find that the evanescent waves generated through nonlinear frequency conversion in the stopband are converted into propagating waves at the interface, subsequently leading to the transmission. Our findings have implications for programmable asymmetric acoustic devices, providing a novel framework for energy mitigation, conversion, and harvesting.

Imaging lattice reconstruction in homobilayers and heterobilayers of transition metal dichalcogenides

Moiré interference effects influence profoundly the optoelectronic properties of vertical van der Waals structures. Here we systematically establish secondary electron imaging in a scanning electron microscope as a powerful technique for visualizing reconstruction of moiré lattices into registry-contrasting domains in vertical homobilayers and heteorbilayers of transition metal dichalcogenides (TMDs) with parallel and antiparallel alignment. With optimal parameters for contrast-maximizing imaging of high-symmetry registries, we identify distinct crystal realizations of WSe2 homobilayers and MoSe2–WSe2 heterostructures synthesized by chemical vapor deposition. In particular, we find evidence for a mutually exclusive competition between and registries, manifesting in complete reconstruction of bilayer crystals into one distinct registry or alternating large-area domains in and stacking. Our results have immediate implications for the optical properties of registry-specific excitons in layered stacks of TMDs, and demonstrate the general potential of secondary electron imaging for van der Waals twistronics.

Revealing the Hidden Spin-Polarized Bands in a Superconducting Tl Bilayer Crystal.

The interplay of spin-orbit coupling and crystal symmetry can generate spin-polarized bands in materials only a few atomic layers thick, potentially leading to unprecedented physical properties. In the case of bilayer materials with global inversion symmetry, locally broken inversion symmetry can generate degenerate spin-polarized bands, in which the spins in each layer are oppositely polarized. Here, we demonstrate that the hidden spins in a Tl bilayer crystal are revealed by growing it on Ag(111) of sizable lattice mismatch, together with the appearance of a remarkable phenomenon unique to centrosymmetric hidden-spin bilayer crystals: a novel band splitting in both spin and space. The key to success in observing this novel splitting is that the interaction at the interface has just the right strength: it does not destroy the original wave functions of the Tl bilayer but is strong enough to induce an energy separation.

Interlayer Sliding Phonon Drives Phase Transition in the Ph-BTBT-10 Organic Semiconductor.

In the field of organic electronics, the semiconductor 7-decyl-2-phenyl[1]benzothieno[3,2-b][1]benzothiophene (Ph-BTBT-10) has become a benchmark due to its high charge mobility and chemical stability in thin film devices. Its phase diagram is characterized by a crystal phase with a bilayer structure that at high temperature transforms into a Smectic E liquid crystal with monolayer structure. As the charge transport properties appear to depend on the phase present in the thin film, the transition has been the subject of structural and computational studies. Here such a process has been investigated by polarized low frequency Raman spectroscopy, selectively probing the intermolecular dynamics of the two phases. The spectroscopic observations demonstrate the key role played by a displacive component of the transition, with the interpenetration of the crystal bilayers driven by lattice phonon mode softening followed by the intralayer rearrangement of the molecule rigid cores into the herringbone motif of the liquid crystal. The mechanism can be related to the effectiveness of thermal annealing to restore the crystal phase in films.

2D Hemiporphyrazine: A new nanoporous material

Crystalline microporous materials are solids formed by interconnected pores of less than 2 nm in size. Typically, they possess large surface areas desirable for versatile applications such as catalysis, gas adsorption, and energy storage. In the present work, we propose a new porphyrin-based 2D nanoporous crystal, named 2D Porphyrazine (2DP), which is formed by topological assembling H$_{5}$C$_{13}$N$_{4}$ porphyrins. We have considered its monolayer, bi-layer, and molecular crystal (bulk) arrangements. We carried out DFT calculations to investigate 2DP structural and electronic properties. Results show that 2DP is a very stable structure with a direct bandgap of 0.65 eV and significant optical absorption in the visible range. 2DP exhibited satisfactory affinity to lithium atoms. Simulations also showed the existence of proton transfer between nitrogen atoms. It is the first report on the site-specific hydrogen exchange process in 2D crystals.

Exploring the effect of dielectric screening on neutral and charged-exciton properties in monolayer and bilayer MoTe2

Dielectric engineering of heterostructures made from two-dimensional van der Waals semiconductors is a unique and powerful tool to tailor the electric and optical band gaps solely via the dielectric environment and the crystal thickness modulation. Here, we utilize high quality MoTe2 monolayer and bilayer crystals as a candidate for near-infrared photonic applications. The crystals are exfoliated on various technologically relevant carrier substrates: silicon/silicon dioxide, poly(methyl methacrylate), hexagonal boron nitride, silicon carbide, and silicon nitride. These substrates provide a large range of high frequency dielectric constants from 2.1 to 7.0 for MoTe2-containing heterostructures. We assess the relationship between the environmental dielectric function and Coulomb screening by combining detailed spectroscopic measurements, utilizing low-temperature and high-spatially resolved photoluminescence and contrast reflectivity, with microscopic many-body modeling, to explore the potential of this less-recognized material platform for applications in optoelectronics at photon wavelengths above 1 μm. We observe a redshift of the optical gap emission energy from the monolayer to bilayer regime on the order of 30 meV. Furthermore, the thickness controlled shift is slightly larger than the one induced by the local dielectric environment, which ranges on the order of 20 meV for the MoTe2 monolayers and on the order of 8 meV for the MoTe2 bilayers. We also show that the local dielectric screening barely affects the trion binding energy, which is captured by our microscopic model, accounting for the screened Coulomb potential for the heterostructures.

Crystallization of Bi-substituted iron garnet bi-layers

Magneto-optical (MO) structures are widely used for different application in the fields of magnetoplasmonics, magneto-optics, photonics e.t.c. Bi-substituted iron garnet (Bi:IG) is high-performance MO material. Integration of Bi:IG films to silicon semiconductor technology gives new opportunities to create nanoscale hight performance MO devices. Vacuum sputtering deposition allows to fabricate Bi:IG structures on different substrate types. Authors investigate crystallization process of Bi:IG bi-layers in a different process parameter (different layers composition and its thickness, temperature and time of annealing) using gadolinium gallium garnet GGG and fused quartz SiO2 substrates to determine dependences which impact on crystallization.

Symmetry and control of spin-scattering processes in two-dimensional transition metal dichalcogenides

Transition metal dichalcogenides (TMDs) combine interesting optical and spintronic properties in an atomically thin material, where the light polarization can be used to control the spin and valley degrees of freedom for the development of novel optospintronic devices. These promising properties emerge due to their large spin-orbit coupling in combination with their crystal symmetries. Here, we provide simple symmetry arguments in a group-theory approach to unveil the symmetry-allowed spin-scattering mechanisms, and indicate how one can use these concepts towards an external control of the spin lifetime. We perform this analysis for both monolayer (inversion asymmetric) and bilayer (inversion symmetric) crystals, indicating the different mechanisms that play a role in these systems. We show that in monolayer TMDs, electrons and holes transform fundamentally differently----leading to distinct spin-scattering processes. We find that one of the electronic states in the conduction band is partially protected by time-reversal symmetry, indicating a longer spin lifetime for that state. In bilayer and bulk TMDs, a hidden spin polarization can exist within each layer despite the presence of global inversion symmetry. We show that this feature enables control of the interlayer spin-flipping scattering processes via an out-of-plane electric field, providing a mechanism for electrical control of the spin lifetime.

Surface roughening, premelting and melting of monolayer and bilayer crystals.

Dimensionality often strongly affects material properties and phase transition behaviors, but its effects on crystal surfaces, such as roughening and premelting, have been poorly studied. Our simulation revealed that these surface behaviors are distinct in monolayer and multilayer Lennard-Jones (LJ) crystals. Solid surfaces fluctuate as capillary waves during the roughening process, but complete roughening is preempted by premelting. As the melting temperature is approached, the thickness of the premelted liquid layer approaches a constant (i.e., blocked premelting) for monolayer crystals, but diverges as a power law (i.e., complete premelting) for bilayer and trilayer crystals. The surface liquids of monolayer crystals contain crystalline patches and exhibits rough liquid-vapour and liquid-crystal interfaces, in contrast to the normal surface liquids of bilayer and trilayer crystals. Monolayer crystals melt heterogeneously from the surface without forming a hexatic phase and produce many vacancies.

The flexibility of long chain substituents influences spin-crossover in isomorphous lipid bilayer crystals.

[Fe(bpp)2][BF4]2 (bpp = 2,6-di{pyrazol-1-yl}pyridine) derivatives with a bent geometry of hexadec-1-ynyl or hexadecyl pyrazole substituents are isomorphous, and high-spin at room temperature. However, only the latter compound undergoes an abrupt, stepwise spin-transition on cooling. This may reflect the different conformational flexibilities of their long chain substituents.

Higher harmonic generation from bilayer nanostructures assisted by electron backscattering

In the framework of time-dependent density functional theory, we obtain high-order harmonics of photon energies up to 10 Up from bilayer crystals with an interlayer spacing d = 70 {\AA}. At grazing incidence, a clear double-plateau structure is observed in the harmonic spectrum. The photon energy of the second plateau far beyond atomic-like harmonics can be well explained by the inclusion of backscattering of ionized electrons. Ab initio simulations reveal that the cutoff of the second plateau is continuously extended with an increasing d. Our classical calculations predict that the maximum electronic kinetic energy is linearly dependent on d over a wide range. Moreover, the harmonic yield in the second plateau is significantly enhanced by increases in the wavelength of the driving laser. Owing to the confined spreading of the electronic wave packet, a beneficial wavelength scaling of {\lambda}2.85 is obtained. This study therefore establishes a novel and efficient way of producing high-energy light source based on layered nanostructures.

Biaxial strain engineering of CVD and exfoliated single- and bi-layer MoS2 crystals

Single- and bi-layer MoS2 are two-dimensional semiconductors able to withstand very large deformations before failure, standing out as suitable templates for strain engineering applications and flexible electronics. It is imperative, for the proper integration of this material in practical applications, that the relationship between material property and strain is well understood. Two dimensional MoS2 crystals fabricated by chemical vapor deposition or micromechanical exfoliation are transferred onto flexible substrates and subjected to biaxial tension on a carefully designed and assessed loading stage with high accuracy and control. The successful stress transfer from substrate to the overlying 2D crystal is identified by in-situ monitoring of the strain-induced phonon frequency and photoluminescence peak shifts. Reliable values for the mode Grüneisen parameters and exciton deformation potentials were obtained by studying a significant number of crystals. The experimental results are backed by density functional theory calculations and are in good agreement with the experiments. This work highlights the potential of these materials in strain engineering applications and gives accurate values for single- and bi-layer MoS2 thermomechanical parameters.

Heterostructured CoOx-TiO2 Mesoporous/Photonic Crystal Bilayer Films for Enhanced Visible-Light Harvesting and Photocatalysis.

Heterostructured bilayer films, consisting of co-assembled TiO2 photonic crystals as the bottom layer and a highly performing mesoporous P25 titania as the top layer decorated with CoOx nanoclusters, are demonstrated as highly efficient visible-light photocatalysts. Broadband visible-light activation of the bilayer films was implemented by the surface modification of both titania layers with nanoscale clusters of Co oxides relying on the chemisorption of Co acetylacetonate complexes on TiO2, followed by post-calcination. Tuning the slow photon regions of the inverse opal supporting layer to the visible-light absorption of surface CoOx oxides resulted in significant amplification of salicylic-acid photodegradation under visible and ultraviolet (UV)–visible light (Vis), outperforming benchmark P25 films of higher titania loading. This enhancement was related to the spatially separated contributions of slow photon propagation in the inverse opal support layer assisted by Bragg reflection toward the CoOx-modified mesoporous P25 top layer. This effect indicates that photonic crystals may be highly effective as both photocatalytically active and backscattering layers in multilayer photocatalytic films.

Exciton g-factors in monolayer and bilayer WSe2 from experiment and theory

The optical properties of monolayer and bilayer transition metal dichalcogenide semiconductors are governed by excitons in different spin and valley configurations, providing versatile aspects for van der Waals heterostructures and devices. Here, we present experimental and theoretical studies of exciton energy splittings in external magnetic field in neutral and charged WSe2 monolayer and bilayer crystals embedded in a field effect device for active doping control. We develop theoretical methods to calculate the exciton g-factors from first principles for all possible spin-valley configurations of excitons in monolayer and bilayer WSe2 including valley-indirect excitons. Our theoretical and experimental findings shed light on some of the characteristic photoluminescence peaks observed for monolayer and bilayer WSe2. In more general terms, the theoretical aspects of our work provide additional means for the characterization of single and few-layer transition metal dichalcogenides, as well as their heterostructures, in the presence of external magnetic fields.