Fate of Optical Excitons in FAPbI3 Nanocube Superlattices.

Understanding the nature of the photoexcitation and ultrafast charge dynamics pathways in organic halide perovskite nanocubes and their aggregation into superlattices is key for potential applications as tunable light emitters, photon-harvesting materials, and light-amplification systems. In this work, we apply two-dimensional coherent electronic spectroscopy (2DES) to track in real time the formation of near-infrared optical excitons and their ultrafast relaxation in CH(NH2)2PbI3 nanocube superlattices. Our results unveil that the coherent ultrafast dynamics is limited by the combination of the inherent short exciton decay time (≃40 fs) and the dephasing due to the coupling with selective optical phonon modes at higher temperatures. On the picosecond time scale, we observe the progressive formation of long-lived localized trap states. The analysis of the temperature dependence of the excitonic intrinsic line width, as extracted by the antidiagonal components of the 2D spectra, unveils a dramatic change of the excitonic coherence time across the cubic to tetragonal structural transition. Our results offer a new way to control and enhance the ultrafast coherent dynamics of photocarrier generation in hybrid halide perovskite synthetic solids.

Halide Perovskite Artificial Solids as a New Platform to Simulate Collective Phenomena in Doped Mott Insulators.

The development of quantum simulators, artificial platforms where the predictions of many-body theories of correlated quantum materials can be tested in a controllable and tunable way, is one of the main challenges of condensed matter physics. Here we introduce artificial lattices made of lead halide perovskite nanocubes as a new platform to simulate and investigate the physics of correlated quantum materials. We demonstrate that optical injection of quantum confined excitons in this system realizes the two main features that ubiquitously pervade the phase diagram of many quantum materials: collective phenomena, in which long-range orders emerge from incoherent fluctuations, and the excitonic Mott transition, which has one-to-one correspondence with the insulator-to-metal transition described by the repulsive Hubbard model in a magnetic field. Our results demonstrate that time-resolved experiments provide a quantum simulator that is able to span a parameter range relevant for a broad class of phenomena, such as superconductivity and charge-density waves.

Ultrafast Electronic Band Gap Control in an Excitonic Insulator.

We report on the nonequilibrium dynamics of the electronic structure of the layered semiconductor Ta_{2}NiSe_{5} investigated by time- and angle-resolved photoelectron spectroscopy. We show that below the critical excitation density of F_{C}=0.2 mJ cm^{-2}, the band gap narrows transiently, while it is enhanced above F_{C}. Hartree-Fock calculations reveal that this effect can be explained by the presence of the low-temperature excitonic insulator phase of Ta_{2}NiSe_{5}, whose order parameter is connected to the gap size. This work demonstrates the ability to manipulate the band gap of Ta_{2}NiSe_{5} with light on the femtosecond time scale.