All-inorganic perovskite CsPbX (X = Cl, Br, I) and related materials are promising candidates for potential solar cells, light emitting diodes, and photodetectors. Here, a novel architecture made of CsPbX /ZnS quantum dot heterodimers synthesized via a facile solution-phase process is reported. Microscopic measurements show that CsPbX /ZnS heterodimer has high crystalline quality with enhanced chemical stability, as also evidenced by systematic density functional theory based first-principles calculations. Remarkably, depending on the interface structure, ZnS induces either n-type or p-type doping in CsPbX and both type-I and type-II heterojunctions can be achieved, leading to rich electronic properties. Photoluminescence measurement results show a strong blue-shift and decrease of recombination lifetime with increasing sulfurization, which is beneficial for charge diffusion in solar cells and photovoltaic applications. These findings are expected to shed light on further understanding and design of novel perovskite heterostructures for stable, tunable optoelectronic devices.
The further practical applications of halide perovskite quantum dots (QDs) are blocked by problems of instability and nonradiative Auger recombination manifested as photoluminescence blinking. Here, single core/shell structured perovskite semiconductor QDs are successfully fabricated by capping CsPbBr3 QD core with CdS shell. It is demonstrated that CsPbBr3/CdS core/shell QDs exhibit ultrahigh chemical stability and nonblinking photoluminescence with high quantum yield due to the reduced electronic traps within the core/shell structure. Efficiency of amplified spontaneous emission exhibits obvious enhancement compared to that of pure CsPbBr3 QDs, originating from the mitigated competition between stimulated emission and suppressed nonradiative biexciton Auger recombination. Furthermore, low‐threshold whispering‐gallery‐mode lasing with a high‐quality factor is achieved by incorporating CsPbBr3/CdS QDs into microtubule resonators. Density functional theory (DFT)‐based first‐principles calculations are also performed to reveal the atomic interface structure, which supports the existence of CsPbBr3/CdS structure. An interesting feature of spatially separated charge density at CsPbBr3/CdS interface is found, which may greatly contribute to the suppressed Auger recombination. The results provide a practical approach to improve the stability and suppress the blinking of halide perovskite QDs, which may pave the way for future applications for various optoelectronic devices.
Recent years have witnessed a surge of research in all-inorganic perovskite nanomaterials for solar cells and light emitting diodes due to their higher chemical stability compared to their hybrid organic-inorganic counterparts. Herein, by combining material synthesis, characterization, optical measurement, and density functional theory based first principles calculation, a type of all-inorganic perovskite CsPb 2 Br 5 microplate with superior crystallinity, enhanced stability, and tunable optical properties is reported. With a robust band gap of ≈2.44 eV, CsPb 2 Br 5 microplate exhibits low-threshold amplified spontaneous emission under both one-and two-photon excitation, which is related to its unique spatially distinguished valence/conduction band edge states originating from the intrinsic sandwiched structure. These results are expected to shed new light on future design and development of novel perovskite nanomaterials for optoelectronic devices.
Recent years have witnessed a surge of research in two-dimensional (2D) nanostructures for development of new rechargeable Li/Na-ion battery systems. Herein, via first-principles calculations we demonstrate strain-engineered Li/Na adsorption and storage in 2D MoS2 as anode material, aiming to enhance the operating performance of Li/Na-ion batteries. Our results show that tensile strain greatly increases the adsorption of Li/Na atoms on MoS2, and a modest strain of 6% increases Li (Na) adsorption energy by over 70%, which originates from the strain-induced upshift of Mo d states towards Fermi level that interact strongly with Li/Na s states, in analogy with the d-band model in metal catalyst. Significant narrowing of the n-doped semiconducting gap of MoS2 suggests the improved electric conductivity that may benefit charge carrier transport. By mapping out the potential energy surfaces, we show shallow energy barriers of ion diffusion with ~0.2 eV for Li and 0.1 eV for Na. Furthermore, the strain-steered competition between chemical bonding and coulomb repulsion results in high Li/Na storage capability and relatively low average operating voltage. We believe that the fundamental principle underlying the use of strain to enhance performance of renewable ion battery is applicable to other stretchable low-dimensional nanomaterials.
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