Excitons and their complexes govern optical-related behaviors in semiconductors. Here, using angle-resolved photoemission spectroscopy (ARPES), we have elucidated the light-matter interaction mediated by quasi-steady excitonic complexes within a monolayer of the prototypical two-dimensional (2D) semiconductor WSe2. Under continuous incident light, we have observed the generation of quasi-steady excitons and their complexes, encompassing ground and excited state excitons, trions, as well as their intricate interplay. We further show spectral evidence of electronic excitation states within the background of quasi-steady excitonic complexes, characterized by valence band (VB) effective mass renormalization, the enhanced spin-orbit coupling (SOC), the formation of an excitonic gap near the Fermi level (EF ) of the conduction band (CB), and intervalley excitonic band folding. Our findings not only unveil a quasi-steady excitonic complex background for the creation of diverse electronic excitations in 2D semiconductors but also offer new insights into the role of excitons in the charge density wave (CDW) formation mechanism and facilitate the advancement of correlated electronic state engineering based on the coupling between electrons and excitonic complexes in a quasi-equilibrium state.
Excitonic insulators conduct neither electrons nor holes but bound electron-hole pairs, excitons. Unfortunately, it is not possible to inject and detect the electron and hole currents independently within a single semiconducting layer. However, interlayer excitonic insulators provide a spatial separation of electrons and holes enabling exciton current measurements. The problem is that the spatial separation weakens electron-hole pairing and may lead to interlayer exciton disassociation. Here we develop an explicitly solvable model to determine an interlayer separation that is strong enough to …
The excitonic insulator is an elusive electronic phase exhibiting a correlated excitonic ground state. Materials with such a phase are expected to have intriguing properties such as excitonic high-temperature superconductivity. However, compelling evidence on the experimental realization is still missing. Here, we theoretically propose hybrids of two-dimensional semiconductors functionalized by organic molecules as prototypes of excitonic insulators, with the exemplary candidate WS$_2$-F6TCNNQ. This material system exhibits an excitonic insulating phase at room temperature with a ground state …
Excitons in two-dimensional semiconductors provide a novel platform for fundamental studies of many-body interactions. In particular, dipolar interactions between spatially indirect excitons may give rise to strongly correlated phases of matter that so far have been out of reach of experiments. Here, we show that excitonic few-body systems in atomically thin transition-metal dichalcogenides undergo a crossover from a Tonks-Girardeau to a charge-density-wave regime. To this end, we take into account realistic system parameters and predict the effective exciton-exciton interaction potential. We …
Spontaneously formed excitonic density wave with vortex-antivortex lattice in twisted semiconductor bilayers
National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University（南京大学固体微结构物理国家重点实验室和物理系）；Department of Physics, University of Massachusetts（马萨诸塞大学物理系）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）；Jiangsu Physical Science Research Center, Nanjing University（南京大学江苏物理科学研究中心）；Hefei National Laboratory（合肥国家实验室）
Three-dimensional gapless semiconductors with quadratic band touching, such as HgTe, $α$-Sn, or Pr$_2$Ir$_2$O$_7$ are believed to display a non-Fermi-liquid ground state due to long-range electron-electron interaction. We argue that this state is inherently unstable towards spontaneous formation of a (topological) excitonic insulator. The instability can be parameterized by a critical fermion number $N_c$. For $N < N_c$ the rotational symmetry is spontaneously broken, the system develops a gap in the spectrum, and features a finite nematic order parameter. To leading order in the 1/N expansion…
We study the time evolution of excitonic states after photo-excitation in the one-dimensional spin-less extended Falicov-Kimball model. Several numerical methods are employed and benchmarked against each other: time-dependent mean-field simulations, the second-Born approximation (2BA) within the Kadanoff-Baym formalism, the generalized Kadanoff-Baym Ansatz (GKBA) implemented with the 2BA and the infinite time-evolving block decimation (iTEBD) method. It is found that the GKBA gives the best agreement with iTEBD and captures the relevant physics. We find that excitations to the particle-hole co…
In this paper, the effects of the external transverse magnetic field $B$ (perpendicular to the surface of the layers) on the electronic and excitonic properties are studied in the AA-stacked bilayer graphene (BLG). The effects of the Coulomb interactions and excitonic pairing have been taken into account and analyzed in detail within the bilayer Hubbard model. Both half-filling and partial filling regimes have been taken into account and the magnetic field dependence of a series of physical parameters was found. It is shown that the difference between the average electron concentrations in the…
Many-body Effects on Excitonic Optical Properties of Photoexcited Semiconductor Quantum Wire Structures
通过求解动态屏蔽的Bethe-Salpeter方程，研究了载流子相互作用引起的多体效应对高度光激发的一维半导体量子线系统激子光学性质的影响.包括电子/空穴自能和电子-空穴相互作用顶点函数中的动态屏蔽效应，我们发现对于大范围的光激发密度（$n= 0-6\times 10^5$ cm $^{-1}$），激子吸收基本上在恒定能量处达到峰值，高于该峰值吸收峰消失而没有明显的增益，即，观察到\textit{no}激子到自由电子-空穴等离子体的Mott跃迁，与以前的理论结果相反，但与最近的实验结果一致。这种增益的缺乏（或莫特跃迁的不存在）源于一维等离子体激元或电荷密度激发的强非弹性散射，与一维系统的非费米液体性质密切相关。我们的理论工作证明了一维光激发电子-空穴系统从低密度区（$n<10^5$ cm $^{-1}$）的非相互作用激子稀气体的有效费米液体行为到高密度区（$n>10^5$ cm $^{-1}$）的非费米液体行为的转变或交叉.对该问题进行了常规的准静态近似，并与全动力学结果进行了比较。激子结合能和吸收光谱的数值结果作为载流子密度和温度的函数。
Motivated by the remarkable discovery of superconductivity in elemental Bismuth, we study its normal state in detail using a combination of tight-binding (TB) and-structural supplemented by dynamical mean-field theory (DMFT). We show that a two-fluid model composed of preformed and dynamically fluctuating excitons coupled to a tiny number of carriers provides a unified rationalization of a range of ill-understood normal state spectral and transport data. Based on these, we propose that resonant scattering involving a very low density of renormalized carriers and the excitonic liquid drives log…
The coupling of excitons with atomic vibrations plays a pivotal role on the nonequilibrium optical properties of layered semiconductors. However, addressing the dynamical interaction between excitons and phonons represents a hard task both experimentally and theoretically. By means of time-resolved broadband optical reflectivity combined with state-of-the-art ab-initio calculations of a bismuth triiodide single crystal, we unravel the universal spectral fingerprints of exciton--phonon coupling in layered semiconductors. Furthermore, we microscopically relate a photoinduced coherent energy modu…
We study the orbital diamagnetic susceptibility in excitonic condensation phase using the meanfield approximation for a two-band model defined on a square lattice. We find that, in semiconductors, the excitonic condensation acquires a finite diamagnetic susceptibility due to spontaneous hybridization between the valence and the conduction bands, whereas in semimetals, the diamagnetic susceptibility in the normal phase is suppressed by the excitonic condensation. We also study the orbital diamagnetic and Pauli paramagnetic susceptibilities of Ta2NiSe5 using a two-dimensional three-band model an…
Excitonic insulators are insulating states formed by the coherent condensation of electron and hole pairs into BCS-like states. Isotropic spatial wave functions are commonly considered for excitonic condensates since the attractive interaction among the electrons and the holes in semiconductors usually leads to $s$-wave excitons. Here, we propose a new type of excitonic insulator that exhibits order parameter with $p+ip$ symmetry and is characterized by a chiral Chern number $C_\textrm{c}=1/2$. This state displays the parity anomaly, which results in two novel topological properties: fractiona…
Excitonic insulator is a coherent electronic phase that results from the formation of a macroscopic population of bound particle-hole pairs - excitons. With only a few candidate materials known, the collective excitonic behavior is challenging to observe, being obscured by crystalline lattice effects. Here we use polarization-resolved Raman spectroscopy to reveal the quadrupolar excitonic mode in the candidate zero-gap semiconductor Ta$_2$NiSe$_5$ disentangling it from the lattice phonons. The excitonic mode pronouncedly softens close to the phase transition, showing its electronic character, …
