Dr Shunran Li

Abstract:

Two-dimensional organic semiconductor-incorporated perovskites are a promising family of hybrid materials for optoelectronic applications, owing in part to their inherent quantum well architecture. Tuning their structures and properties for specific properties, however, has remained challenging. Here we report a general method to tune the dimensionality of phase-pure organic semiconductor-incorporated perovskite single crystals during their synthesis, by judicious choice of solvent. The length of the conjugated semiconducting organic cations and the dimensionality (n value) of the inorganic layers can be manipulated at the same time. The energy band offsets and exciton dynamics at the organic-inorganic interfaces can therefore be precisely controlled. Furthermore, we show that longer and more planar π-conjugated organic cations induce a more rigid inorganic crystal lattice, which leads to suppressed exciton-phonon interactions and better optoelectronic properties as compared to conventional two-dimensional perovskites. As a demonstration, optically driven lasing behaviour with substantially lower lasing thresholds was realized.

Abstract:

The layer stacking order in 2D materials strongly affects functional properties and holds promise for next-generation electronic devices. In bulk, octahedral MoTe₂ possesses two stacking arrangements, the ferroelectric Weyl semimetal T_d phase and the higher-order topological insulator 1T' phase. However, in thin flakes of MoTe₂, it is unclear if the layer stacking follows the T_d, 1T', or an alternative stacking sequence. Here, we use atomic-resolution scanning transmission electron microscopy to directly visualize the MoTe₂ layer stacking. In thin flakes, we observe highly disordered stacking, with nanoscale 1T' and T_d domains, as well as alternative stacking arrangements not found in the bulk. We attribute these findings to intrinsic confinement effects on the MoTe₂ stacking-dependent free energy. Our results are important for the understanding of exotic physics displayed in MoTe₂ flakes. More broadly, this work suggests c-axis confinement as a method to influence layer stacking in other 2D materials.

Abstract:

Two key interfaces in flexible perovskite solar cells (f-PSCs) are mechanically reinforced simultaneously: one between the electron-transport layer (ETL) and the 3D metal-halide perovskite (MHP) thin film using self-assembled monolayer (SAM), and the other between the 3D-MHP thin film and the hole-transport layer (HTL) using an in situ grown low-dimensional (LD) MHP capping layer. The interfacial mechanical properties are measured and modeled. This rational interface engineering results in the enhancement of not only the mechanical properties of both interfaces but also their optoelectronic properties holistically. As a result, the new class of dual-interface-reinforced f-PSCs has an unprecedented combination of the following three important performance parameters: high power-conversion efficiency (PCE) of 21.03% (with reduced hysteresis), improved operational stability of 1000 h T₉₀ (duration at 90% initial PCE retained), and enhanced mechanical reliability of 10 000 cycles n₈₈ (number of bending cycles at 88% initial PCE retained). The scientific underpinnings of these synergistic enhancements are elucidated.

Abstract:

Understanding thermal transport at the microscale to the nanoscale is crucially important for a wide range of technologies ranging from device thermal management and protection systems to thermal-energy regulation and harvesting. In the past decades, non-contact optical methods, such as time-domain and frequency-domain thermoreflectance, have emerged as extremely powerful and versatile thermal metrological techniques for the measurement of material thermal conductivities. Here, we report the measurement of thermal conductivity of thin films of CH₃NH₃PbI₃ (MAPbI₃), a prototypical metal-halide perovskite, by developing a time-resolved optical technique called vibrational-pump visible-probe (VPVP) spectroscopy. The VPVP technique relies on the direct thermal excitation of MAPbI₃ by femtosecond mid-infrared optical pump pulses that are wavelength-tuned to a vibrational mode of the material, after which the time dependent optical transmittance across the visible range is probed in the ns to the μs time window using a broadband pulsed laser. Using the VPVP method, we determine the thermal conductivities of MAPbI₃ thin films deposited on different substrates. The transducer-free VPVP method reported here is expected to permit spectrally resolving and spatiotemporally imaging of the dynamic lattice temperature variations in organic, polymeric, and hybrid organic-inorganic semiconductors.