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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.

Abstract:

Recently, Bi-doped Cs₂ Ag_0.6 Na_0.4 InCl₆ lead-free double perovskites demonstrating efficient warm-white emission have been reported. To enable the solution processing and enrich the application fields of this promising material, here a colloidal synthesis of Cs₂ Ag_{1- x} Na_x In_{1- y} Bi_y Cl₆ nanocrystals is further developed. Different from its bulk states, the emission color temperatures of the nanocrystal can be tuned from 9759.7 to 4429.2 K by Na⁺ and Bi³⁺ incorporation. Furthermore, the newly developed nanocrystals can break the wavefunction symmetry of the self-trapped excitons by partial replacement of Ag⁺ ions with Na⁺ ions and consequently allow radiative recombination. Assisted with Bi³⁺ ions doping and ligand passivation, the photoluminescence quantum yield of the Cs₂ Ag_0.17 Na_0.83 In_0.88 Bi_0.12 Cl₆ nanocrystals is further promoted to 64%, which is the highest value for lead-free perovskite nanocrystals at present. The new colloidal nanocrystals with tunable color temperature and efficient photoluminescence are expected to greatly advance the research progress of lead-free perovskites in single-emitter-based white emitting materials and devices.