We study theoretically the exciton Bose-Einstein condensation and exciton vortices in a two-dimensional (2D) perovskite (PEA)2PbI4 monolayer. Combining the first-principles calculations and the Keldysh model, the exciton binding energy of (PEA)2PbI4 in a monolayer can approach hundreds meV, which make it possible to observe the excitonic effect at room temperature. Due to the large exciton binding energy, and hence the high density of excitons, we find that the critical temperature of the exciton condensation could approach the liquid nitrogen regime. In presence of perpendicular electric fields, the dipole-dipole interaction between excitons is found to drive the condensed excitons into patterned vortices, as the evolution time of vortex patterns is comparable to the exciton lifetime.
We theoretically propose a family of structurally stable monolayer halide perovskite A$_3$B$_2$C$_9$ (A=Rb, Cs; B=Pd, Pt; C=Cl, Br) with easy magnetization planes. These materials are all half-metals with large spin gaps over 1~eV accompanying with a single spin Dirac point located at K point. When the spin-orbit coupling is switched on, we further show that Rb$_3$Pt$_2$Cl$_9$, Cs$_3$Pd$_2$Cl$_9$, and Cs$_3$Pt$_2$Cl$_9$ monolayers can open up large band gaps from 63 to 103 meV to harbor quantum anomalous Hall effect with Chern numbers of $\mathcal{C}=\pm1$, whenever the mirror symmetry is brok…
It is highly desirable to search for promising two-dimensional (2D) monolayer materials for deep insight of 2D materials and applications. We use first-principles method to investigate tetragonal perovskite oxide monolayers as 2D materials. We find four stable 2D monolayer materials from SrTiO$_3$, LaAlO$_3$, KTaO$_3$, and BaFeO$_3$, denoting them as STO-ML, LAO-ML, KTO-ML, and BFO-ML. Our further study shows that through overcoming dangling bonds the first three monolayers are 2D wide-gap semiconducotors, and BFO-ML is a 2D isotropic Heisenberg ferromagnetic metal. There is a large electrosta…
Using first-principles density functional theory calculations, we systematically investigate the structural, electronic and vibrational properties of bulk and potential single-layer structures of perovskite-like CsPb2Br5 crystal. It is found that while Cs atoms have no effect on the electronic structure, their presence is essential for the formation of stable CsPb2Br5 crystals. Calculated vibrational spectra of the crystal reveal that not only the bulk form but also the single-layer forms of CsPb2Br5 are dynamically stable. Predicted single-layer forms can exhibit either semiconducting or meta…
Vortex is a universal and significant phenomenon that has been known for centuries. However, creating vortices to the atomic limit has remained elusive because that the characteristic length to support a vortex is usually much larger than the atomic scale. Very recently, it was demonstrated that intervalley scattering induced by the single carbon defect of graphene leads to phase winding over a closed path surrounding the defect. Motivated by this, we demonstrate, in this Letter, that the single carbon defects at A and B sublattices of graphene can be regarded as pseudospin-mediated atomic-sca…
Many-body effect and strong Coulomb interaction in monolayer transition metal dichalcogenides lead to shrink the intrinsic bandgap, originating from the renormalization of electrical/optical bandgap, exciton binding energy, and spin-orbit splitting. This renormalization phenomenon has been commonly observed at low temperature and requires high photon excitation density. Here, we present the augmented bandgap renormalization in monolayer MoS_2 anchored on CsPbBr_3 perovskite quantum dots at room temperature via charge transfer. The amount of electrons significantly transferred from perovskite g…
Tuning exciton emission via ferroelectric polarization at a heterogeneous interface between a monolayer transition metal dichalcogenide and a perovskite oxide membrane
Two-dimensional (2D) layered hybrid perovskites provide an ideal platform for studying the properties of excitons. Here, we report on a strong triplet-exciton and longitudinal-optical (LO) phonon coupling in 2D (C6H5CH2CH2NH3, PEA)2PbBr4 perovskites. The triplet excitons exhibit strong photoluminescence (PL) in thick perovskite microflakes, and the PL is not detectable for monolayer microflakes. The coupling strength of the triplet exciton-LO phonon is approximately two to three times greater than that of the singlet exciton-LO phonon with a LO phonon energy of about 21 meV. This difference mi…
Perovskites have attracted much attention due to their remarkable optical properties. While it is well established that excitons dominate their optical response, the impact of higher excitonic states and formation of phonon sidebands in optical spectra still need to be better understood. Here, we perform a theoretical study on excitonic properties of monolayered hybrid organic perovskites -- supported by temperature-dependent photoluminescence measurements. Solving the Wannier equation, we obtain microscopic access to the Rydberg-like series of excitonic states including their wavefunctions an…
The application of ultrathin two-dimensional (2D) perovskites in near-infrared and visible-range optoelectronics has been limited owing to their inherent wide bandgaps, large excitonic binding energies and low optical absorption at higher wavelengths. Here, we show that by tailoring interfacial band alignments via conjugation with low-dimensional materials like monolayer transition metal dichalcogenides (TMD), the functionalities of 2D perovskites can be extended to diverse, visible-range photophysical applications. Based on the choice of individual constituents in the 2D perovskite/TMD hetero…
Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton-exciton interactions. In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of exciton-exciton interaction, making materials with highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow to overcome this limitatio…
Exciton-polaritons in semiconductor microcavities generate fascinating effects such as long-range spatial coherence and Bose-Einstein Condensation (BEC), which are attractive for their potential use in low threshold lasers, vortices and slowing light, etc. However, currently most of exciton-polariton effects either occur at cryogenic temperature or rely on expensive cavity fabrication procedures. Further exploring new semiconductor microcavities with stronger exciton photon interaction strength is extensively needed. Herein, we demonstrate room temperature photon exciton strong coupling in hyb…
Halide perovskite light absorbers have great advantages for photovoltaics such as efficient solar energy absorption, but charge accumulation and recombination at the interface with an electron transport layer (ETL) remains a major challenge in realizing their full potential. Here we report the experimental realization of a zipper-like interdigitated interface between a Pb-based halide perovskite light absorber and an oxide ETL by the PbO capping of the ETL surface, which produces an atomically thin two-dimensional metallic layer that can significantly enhance the perovskite/ETL charge extracti…
Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西埃茨基大学）；Philipps-Universität Marburg（马尔堡菲利普斯大学）；Wroclaw University of Science and Technology（弗罗茨瓦夫科技大学）；University of Applied Sciences Emden/Leer（埃姆登/莱尔应用科学大学）；Fraunhofer-Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所IOF）；Friedrich Schiller University, Jena（耶拿弗里德里希·席勒大学）；University of Chemistry and Technology Prague（布拉格化学技术大学）；Massachusetts Institute of Technology（麻省理工学院）；Vidyasirimedhi Institute of Science and Technology (VISTEC)（维他西亚米德科学与技术学院(VISTEC)）；Laboratoire National des Champs Magnétiques Intenses, EMFL, CNRS UPR, 3228, University Grenoble Alpes, University Toulouse, University Toulouse 3, INSA-T Grenoble（强磁场国家实验室，EMFL，CNRS UPR 3228，格勒诺布尔阿尔卑斯大学，图卢兹大学，图卢兹第三大学，INSA-T格勒诺布尔）
Huazhong University of Science and Technology（华中科技大学）；Tsinghua University（清华大学）；Nanyang Technological University（南洋理工大学）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）
Noncollinear spin textures in low-dimensional magnetic systems have been studied for decades because of their extraordinary properties and promising applications derived from the chirality and topological nature. However, material realizations of topological spin states are still limited. Employing first-principles and Monte Carlo simulations, we propose that monolayer chromium trichloride (CrCl3) can be a promising candidate for observing the vortex/antivortex type of topological defects, so-called merons. The numbers of vortices and antivortices are found to be the same, maintaining an overa…
Trion polaron problem in bulk and two-dimensional materials
MIPT（莫斯科物理技术学院）；University of Iceland（冰岛大学）；Vanderbilt University（范德堡大学）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Universidad del País Vasco（巴斯克大学）；IKERBASQUE, Basque Foundation for Science（伊克尔巴斯基克科学基金会）
Quantum Griffiths singularity (QGS) reveals the profound influence of quenched disorder on the quantum phase transitions, characterized by the divergence of the dynamical critical exponent at the boundary of the vortex glass-like phase, named as quantum Griffiths phase. However, in the absence of vortices, whether the QGS can exist under parallel magnetic field remains a puzzle. Here we study the magnetic field induced superconductor-metal transition in ultrathin crystalline PdTe2 films grown by molecular beam epitaxy. Remarkably, the QGS emerges under both perpendicular and parallel magnetic …
