Interlayer excitons are observed coexisting with intralayer excitons in bi-layer, few-layer, and bulk MoSe2 single crystals by confocal reflection contrast spectroscopy. Quantitative analysis using the Dirac-Bloch-Equations provides unambiguous state assignment of all the measured resonances. The interlayer excitons in bilayer MoSe2 have a large binding energy of 153 meV, narrow linewidth of 20 meV, and their spectral weight is comparable to the commonly studied higher-order intralayer excitons. At the same time, the interlayer excitons are characterized by distinct transition energies and permanent dipole moments providing a promising high temperature and optically accessible platform for dipolar exciton physics.
Impact of an electron Wigner crystal on exciton propagation
Philipps-Universität Marburg（马尔堡菲利普斯大学）；mar.quest—Marburg Center for Quantum Materials and Sustainable Technologies（mar.quest—马尔堡量子材料与可持续技术中心）；Institute of Applied Physics and Würzburg-Dresden Cluster of Excellence ct.qmat, TU Dresden（德累斯顿工业大学应用物理研究所与维尔茨堡-德累斯顿卓越集群ct.qmat）
Excitons are bound electron-hole pairs that dominate the optical response of semiconductors and insulators, especially in materials where the Coulomb interaction is weakly screened. Light absorption (including excitonic effects) has been studied extensively using first-principles calculations, but methods for computing radiative recombination and light emission are still being developed. Here we show a unified ab initio approach to compute exciton radiative recombination in materials ranging from bulk crystals to nanostructures and molecules. We derive the rate of exciton radiative recombinati…
Two-dimensional (2D) perovskite materials have recently re-attracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. In this report, the band-edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA)2PbI4 are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2x10^3cm/s and an intrinsic lifetime of 185…
We investigate analytically the anisotropic dielectric properties of single crystal α-SnS near the fundamental absorption edge by considering atomic orbitals. Most striking is the excitonic feature in the armchair- (b-) axis direction, which is particularly prominent at low temperatures. To determine the origin of this anisotropy, we perform first-principles calculations using the GW0 Bethe-Salpeter equation (BSE) including the electron-hole interaction. The results show that the anisotropic dielectric characteristics are a direct result of the natural anisotropy of p orbitals. In particular, …
Spin-dependent Raman and Brillouin light scattering on excitons in CsPbBr$_3$ perovskite crystals
Ioffe Institute, Russian Academy of Sciences（俄罗斯科学院约费研究所）；Technische Universität Dortmund（多特蒙德工业大学）；Research Center FEMS, Technische Universität Dortmund（多特蒙德工业大学FEMS研究中心）
When Cubic Is Not Isotropic: Phonon-Exciton Decoupling in CuInSnS$_4$ Single Crystals
Helmholtz-Zentrum Berlin für Materialien und Energie（柏林赫尔姆霍兹中心）；University of Manchester（曼彻斯特大学）；University of Zurich（苏黎世大学）；University of Basel（巴塞尔大学）；University of Cambridge（剑桥大学）；Freie Universität Berlin（柏林自由大学）
Dimensional Control of Excitonic Interactions in Exfoliated 2D Molecular Crystals
Pohang University of Science and Technology (POSTECH)（浦项科技大学）；Hanyang University（汉阳大学）；Research Institute of Natural Science, Hanyang University（汉阳大学自然科学研究院）；Yonsei University（延世大学）；National Institute for Materials Science（物质材料研究机构）；Queens College, City University of New York（纽约市立大学皇后学院）；Graduate Center, City University of New York（纽约市立大学研究生院）
We demonstrate the successive appearance of the exciton, biexciton, and P band of the exciton-exciton scattering with increasing excitation power in the photoluminescence of indium selenide layered crystals. The strict energy and momentum conservation rules of the P band are used to reexamine the exciton binding energy. The new value $\geq 20$ meV is markedly higher than the currently accepted 14 meV, being however well consistent with the robustness of excitons up to room temperature. A peak controlled by the Sommerfeld factor is found near the bandgap ($\sim 1.36$ eV), which puts the questio…
Elucidating the underlying principles behind band gap engineering is paramount for the successful implementation of semiconductors in photonic and optoelectronic devices. Recently it has been shown that the band gap of a wide and direct band gap semiconductor, such as ZnO, can be modified upon co-crystallization with amino acids, with the role of the biomolecules remaining unclear. Here, by probing and modeling the light emitting properties of ZnO-amino acid co-crystals, we identify the amino acids role on this band gap modulation and demonstrate their effective chirality transfer to the inter…
Suppressed excitonic effects enable high mobility, high-yield photoconductivity in a two-dimensional polymer crystal with axial pyridine coordination
Technische Universität Dresden（德累斯顿工业大学）；Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）；Beijing Institute of Technology（北京理工大学）；Helmholtz-Zentrum Dresden-Rossendorf（亥姆霍兹中心德累斯顿-罗斯托克）；Center for Advanced Systems Understanding（高级系统理解中心）；Yonsei University（延世大学）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微结构物理研究所）
Linear and non-linear spectroscopies are powerful tools used to investigate the energetics and dynamics of electronic excited states of both molecules and crystals. While highly accurate \emph{ab initio} calculations of molecular spectra can be performed relatively routinely, extending these calculations to periodic systems is challenging. Here, we present calculations of the linear absorption spectrum and pump-probe two-photon photoemission spectra of the naphthalene crystal using equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). Molecular acene crystals…
The spatial extent of excitons in molecular systems underpins their photophysics and utility for optoelectronic applications. Phonons are reported to lead to both exciton localization and delocalization. However, a microscopic understanding of phonon-induced (de)localization is lacking, in particular how localized states form, the role of specific vibrations, and the relative importance of quantum and thermal nuclear fluctuations. Here we present a first-principles study of these phenomena in solid pentacene, a prototypical molecular crystal, capturing the formation of bound excitons, exciton-…
We develop a consistent theory of the interlayer exciton-polaron formed in atomically-thin bilayers. Coulomb attraction between an electron and a hole situated in the different layers results in their flexural deformation and provides an efficient mechanism of the exciton coupling with flexural phonons. We study the effect of layers tension on the polaron binding energy and effective mass leading to suppression of polaron formation by the tension both in the weak and strong coupling regimes. We also consider the role of the nonlinearity related to the interaction between the out- and in-plane …
Lead halide perovskites show remarkable performance when used in photovoltaic and optoelectronic devices. However, the peculiarities of light-matter interactions in these materials in general are far from being fully explored experimentally and theoretically. Here we specifically address the energy level order of optical transitions and demonstrate photon echos in a methylammonium lead triiodide single crystal, thereby determining the optical coherence times $T_2$ for excitons and biexcitons at cryogenic temperature to be 0.79 ps and 0.67 ps, respectively. Most importantly, we have developed a…
Singlet exciton fission (SEF) is a key process in the development of efficient opto-electronic devices. An aspect that is rarely probed directly, and yet has a tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction. The data reveal coherent atomic motions at 1 THz, incoherent motions, and an anisotropic lattice distortion representing the polaronic character of the triplet excitons. Combining molecular dynami…
Organic semiconductors exhibit properties of individual molecules and extended crystals simultaneously. The strongly bound excitons they host are typically described in the molecular limit, but excitons can delocalize over many molecules, raising the question of how important the extended crystalline nature is. Using accurate Green's function based methods for the electronic structure and non-perturbative finite difference methods for exciton-vibration coupling, we describe exciton interactions with molecular and crystal degrees of freedom concurrently. We find that the degree of exciton deloc…
Twisted van der Waals heterostructures and the corresponding superlattices, moire superlattices, are remarkable new material platforms, in which electron interactions and excited-state properties can be engineered. Particularly, the band offsets between adjacent layers can separate excited electrons and holes, forming interlayer excitons that exhibit unique optical properties. In this work, we employ the first-principles GW-Bethe-Salpeter Equation (BSE) method to calculate quasiparticle band gaps, interlayer excitons, and their modulated excited-state properties in twisted MoSe2/WSe2 bilayers …
Spin dynamics of excitons and carriers in mixed-cation MA$_{x}$FA$_{1-x}$PbI$_{3}$ perovskite crystals: alloy fluctuations probed by optical orientation
University of Southern California（南加州大学）；Tamkang University（淡江大学）；The University of British Columbia（不列颠哥伦比亚大学）；The University of Texas at Austin（德克萨斯大学奥斯汀分校）；University of Washington（华盛顿大学）；University of California at Berkeley（加利福尼亚大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）
The emergence of two-dimensional crystals has revolutionized modern solid-state physics. From a fundamental point of view, the enhancement of charge carrier correlations has sparked enormous research activities in the transport- and quantum optics communities. One of the most intriguing effects, in this regard, is the bosonic condensation and spontaneous coherence of many-particle complexes. Here, we find compelling evidence of bosonic condensation of exciton-polaritons emerging from an atomically thin crystal of MoSe2 embedded in a dielectric microcavity under optical pumping. The formation o…
Exciton Valley Hall effect is the spatial separation of the valley-tagged excitons in the presence of a drag force. Usually, the effect is associated with the anomalous velocity acquired by the particles due to the Berry curvature of the Bloch bands. Here we show that the anomalous velocity plays no role in the exciton valley Hall effect, which is governed by the side-jump and skew scattering mechanisms. We develop microscopic theory of the exciton valley Hall effect in the presence of synthetic electric field and phonon drag and calculate all relevant contributions to the valley Hall current …
Optical absorption is one of fundamental light-matter interactions. In most materials, optical absorption is a weak perturbation to the light. In this regime, absorption and emission are irreversible, incoherent processes due to strong damping. Excitons in monolayer transition metal dichalcogenides, however, interact strongly with light, leading to optical absorption in the non-perturbative regime where coherent re-emission of the light has to be considered. Between the incoherent and coherent limits, we show that a robust critical coupling condition exists, leading to perfect optical absorpti…
Hybrid organic-inorganic perovskites have emerged as very promising materials for photonic applications, thanks to the great synthetic versatility that allows to tune their optical properties. In the two-dimensional (2D) crystalline form, these materials behave as multiple quantum-well heterostructures with stable excitonic resonances up to room temperature. In this work strong light-matter coupling in 2D perovskite single-crystal flakes is observed, and the polarization-dependent exciton-polariton response is used to disclose new excitonic features. For the first time, an out-of-plane compone…
