The rhombohedral (r) polytypes of transition metal dichalcogenides (TMDs) constitute a novel class of two-dimensional ferroelectric materials, where lateral shifts between parallel layers induce reversible out-of-plane polarization. This emerging field, known as SlideTronics, holds significant potential for next-generation electronic and optoelectronic applications. While extensive studies have investigated the effects of electrical and chemical doping on excitonic signatures in 2H-TMDs, as well as the influence of dielectric environments on their optical properties, the impact of intrinsic polarization in asymmetric environments remains largely unexplored. Here, we demonstrate a striking polarization-dependent photoluminescence (PL) contrast of up to 400\% between ferroelectric domains in bilayer and trilayer rhombohedral molybdenum disulfide (r-MoS2). This pronounced contrast arises from an asymmetric dielectric environment, which induces polarization-dependent shifts in the Fermi energy, leading to a modulation of the exciton-trion population balance. A detailed temperature-dependent line shape analysis of the PL, conducted from 4K to room temperature, reveals domain-specific trends that further reinforce the connection between polarization states and excitonic properties. The persistence of these distinct optical signatures at room temperature establishes PL as a robust and non-invasive probe for ferroelectric domain characterization, particularly in fully encapsulated device architectures where conventional techniques, such as Kelvin probe force microscopy, become impractical.
The excitonic radiative recombination of intercalated Cl2 molecules for two different polytypes 2H-MoS2 and 3R-MoS2 layered crystals are presented. The structure of the excitonic emission is unique and provides a robust experimental signature of crystal polytype investigated. This result is confirmed by X-ray diffraction analysis and DFT electronic band structure calculations. Thus, the bound exciton emission provides a nondestructive fingerprint for the reliable identification of the polytype of MoS2 layered crystals.
We report our first-principles investigations on three polytypes of BaTiO3 (BTO): a paraelectric phase with cubic Pm-3m structure and two ferroelectric (FE) phases with tetragonal P4mm and rhombohedral R3m structures. We compared the structural and the electrical properties of BTO obtained by using various approaches: e.g., the Hartree-Fock (HF) theory, the density functional theory (DFT) with the local density approximation (LDA) or with the two generalized gradient approximations (two GGAs: PWGGA and PBE), and three hybrid functionals of the HF and the DFT (B3LYP, B3PW, and PBE0). For the P4…
Atomically thin two-dimensional molybdenum disulfide (MoS2) sheets have attracted much attention due to their potential for future electronic applications. They not only present the best planar electrostatic control in a device, but also lend themselves readily for dielectric engineering. In this work, we experimentally investigated the dielectric effect on the Raman and photoluminescence (PL) spectra of monolayer MoS2 by comparing samples with and without HfO2 on top by atomic layer deposition (ALD). Based on considerations of the thermal, doping, strain and dielectric screening influences, i…
We quantitatively study the Raman and photoluminescence (PL) emission from single layer molybdenum disulfide (MoS2) on dielectric (SiO2, hexagonal boron nitride, mica and the polymeric dielectric Gel-Film) and conducting substrates (Au and few-layer graphene). We find that the substrate can affect the Raman and PL emission in a twofold manner. First, the absorption and emission intensities are strongly modulated by the constructive/destructive interference within the different substrates. Second, the position of the A1g Raman mode peak and the spectral weight between neutral and charged excito…
Optical properties of semiconductors can exhibit strong polarization dependence due to crystalline anisotropy. A number of recent experiments have shown that the photoluminescence intensity in free standing nanowires is polarization dependent. One contribution to this effect is the anisotropy of the dielectric function due to the fact that most nanowires crystalize in the wurtzite form. While little is known experimentally about the band structures wurtzite phase III-V semiconductors, we have previously predicted the bulk band structure of nine III-V semiconductors in wurtzite phase.Here, we p…
Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. …
Atomically thin semiconductors such as monolayer MoS2 and WS2 exhibit nonlinear exciton-exciton annihilation at notably low excitation densities (below ~10 excitons/um2 in MoS2). Here, we show that the density threshold at which annihilation occurs can be tuned by changing the underlying substrate. When the supporting substrate is changed from SiO2 to Al2O3 or SrTiO3, the rate constant for second-order exciton-exciton annihilation, k_XX [cm2/s], is reduced by one or two orders of magnitude, respectively. Using transient photoluminescence microscopy, we measure the effective room-temperature ex…
Spectral ellipsometry studies of the optical functions, first observation of photoluminescence and low frequency dielectric permittivity investigations were performed in ferroelectric - multiferroic TbMnO3 single crystals. The main attention was paid to electronic band structure, nature of the main optical transitions and unusual behavior of the dielectric permittivity in the region of the sharp narrow temperature maximum, associated with ferroelectric phase transition. It was found that magnitude of the permittivity maximum decreases strongly with frequency, whereas position of maximum is fre…
Ferroelectric Control of Interlayer Excitons in 3R-MoS$_{2}$ / MoSe$_{2}$ Heterostructures
University of Rostock（罗斯托克大学）；Technical University of Munich（慕尼黑工业大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Saha Institute of Nuclear Physics（萨哈核物理研究所）；Homi Bhabha National Institute（霍米·巴巴国立学院）；NIMS（日本材料研究所）
Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance of surface interactions and charging effects requiring new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping o…
Hexagonal YMnO$_3$ is well known for the co-occurrence of ferroelectricity and antiferromagnetism at low temperatures. Using temperature-dependent spectroscopic ellipsometry at an $a$-plane oriented single crystal, we show how the dielectric function is affected by the magnetic order transition at the Néel temperature. We focus especially on the pronounced charge transfer transitions around (1.6-1.7)eV which are strongly connected to Mn 3$d$ electrons. If described with a Bose-Einstein model, the temperature dependency of their energy and broadening is characterized by effective phonon energie…
Zero dimensional graphene quantum dots (GQDs) exhibit interesting physical and chemical properties due to the edge effect and quantum confinement. As the number of carbon atoms in edge is more than on basal plane, GQDs are more reactive. Room temperature XRD pattern confirms the formation of the GQDs. UV-Visible spectra confirm that GQDs show optical absorption in the visible region. The emission peaks in the photoluminescence spectra are red shifted with the increase of excitation wavelength. Dynamic light scattering (DLS) analysis shows that the average size of the particles is found to be 6…
Nanoscopy of Excitons in Atomically Thin In-Plane Heterostructures with Nanointerfaces
University of Georgia（佐治亚大学）；Syracuse University（雪城大学）；The Pennsylvania State University（宾夕法尼亚州立大学）；University of Extremadura（埃斯特雷马杜拉大学）；University of Vigo（维戈大学）；Rice University（莱斯大学）
Multiferroic bismuth ferrite Bi_2Fe_4O_9 (BFO) ceramic was synthesized by conventional solid state reaction route. X-ray diffraction and Rietveld refinement show formation of single phase ceramic with orthorhombic crystal structure (space group Pbam). The morphological study depicted a well-defined grain of size $\simeq$2μm. The optical studies were carried out by using UV-Vis spectrophotometer which shows a band gap of 1.53 eV and a green emission spectrum at 537 is observed in the Photoluminescence study. The frequency dependent dielectric study at various temperature revealed that the diele…
Machine Learning Assisted Reconstruction of Local Electronic Structure of Non-Uniformly Strained MoS2
Indian Institute of Science Education and Research Thiruvananthapuram（印度科学教育与研究特里凡得琅研究所）；J. Heyrovsky Institute of Physical Chemistry, Czech Academy of Sciences（捷克科学院J.赫罗斯夫斯基物理化学研究所）
Unidirectional in-plane structural anisotropy in Rhenium-based transition metal dichalcogenides (TMDs) introduces a new class of 2-D materials, exhibiting anisotropic optical properties. In this work, we perform temperature dependent, polarization-resolved photoluminescence and reflectance measurements on several-layer ReS$_{2}$. We discover two additional excitonic resonances (X$_{3}$ and X$_{4}$), which can be attributed to splitting of spin degenerate states. Strong in-plane oscillator strength of exciton species X$_{1}$ and X$_{2}$ are accompanied by weaker counterparts X$_{3}$ and X$_{4}$…
