Simulations of Trions and Biexcitons in Layered Hybrid Organic-Inorganic Lead Halide Perovskites
arXiv:2010.10542 · doi:10.1103/PhysRevLett.126.216402
Abstract
Behaving like atomically-precise two-dimensional quantum wells with non-negligible dielectric contrast, the layered HOIPs have strong electronic interactions leading to tightly bound excitons with binding energies on the order of 500 meV. These strong interactions suggest the possibility of larger excitonic complexes like trions and biexcitons, which are hard to study numerically due to the complexity of the layered HOIPs. Here, we propose and parameterize a model Hamiltonian for excitonic complexes in layered HOIPs and we study the correlated eigenfunctions of trions and biexcitons using a combination of diffusion Monte Carlo and very large variational calculations with explicitly correlated Gaussian basis functions. Binding energies and spatial structures of these complexes are presented as a function of the layer thickness. The trion and biexciton of the thinnest layered HOIP have binding energies of 35 meV and 44 meV, respectively, whereas a single exfoliated layer is predicted to have trions and biexcitons with equal binding enegies of 48 meV. We compare our findings to available experimental data and to that of other quasi-two-dimensional materials.
arXiv commentmain text: 6 pages, 4 figures, 1 table; supplement: 7 pages, 2 figures
References in corpus (26)
- Observation of tightly bound trions in monolayer MoS2
- Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
- Observation of giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
- Tightly bound excitons in monolayer WSe2
- Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
- Local polar fluctuations in lead halide perovskite crystals
- Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
- Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites
- Many-Body Theory of Trion Absorption Features in Two-Dimensional Semiconductors
- Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder
- How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites
- Environmentally-Sensitive Theory of Electronic and Optical Transitions in Atomically-Thin Semiconductors
- Diffusion quantum Monte Carlo study of excitonic complexes in two-dimensional transition-metal dichalcogenides
- Density matrix quantum Monte Carlo
- Binding energies of trions and biexcitons in two-dimensional semiconductors from diffusion quantum Monte Carlo calculations
- Binding energies and spatial structures of small carrier complexes in monolayer transition metal dichalcogenides via diffusion Monte Carlo
- Three-particle Complexes in Two-Dimensional Semiconductors
- Exciton complexes in low dimensional transition metal dichalcogenides
- Photoinduced phase separation in the lead halides is a polaronic effect
- Effective mass theory for the anisotropic exciton in 2D crystals: Application to phosphorene
- Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach
- Theoretical investigation of electron-hole complexes in anisotropic two-dimensional materials
- Electrostatics of electron-hole interactions in van der Waals heterostructures
- Preconditioning and perturbative estimators in full configuration interaction quantum Monte Carlo
- Fast randomized iteration: diffusion Monte Carlo through the lens of numerical linear algebra
- Thermal dissociation of dipositronium: path integral Monte Carlo approach