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Nanoscale spatial mapping of charge carrier dynamics in perovskite solar cells
摘要： Charge carrier dynamics and behaviors are key parameters and need to be mapped at the nanoscale in order to search for correct materials for high-performance solar cells. Unfortunately, currently, there are no existing tools or capabilities that can simultaneously map charge carrier dynamics at nanometer range in solar cells. Here we use a Transient Photo-response AFM (TP-AFM) to map for the first time apparent carrier recombination lifetime (τr), transport time (τt) and diffusion length (LD) in hybrid perovskites solar cells. These spatially resolved parameters reveal substantial variations at grain boundaries (GBs) τr, τt and LD at GBs broaden the performance of these state-of-the-art mixed cation perovskites. Detail analysis of these parameters allow us to conclude that reduced density of trap states and recombination in mixed cation perovskites at GBs and its surrounding locations (extending to several nanometers into the grain interior) implies less ion migration. This first of its kind experimental realization of nanoscale mapping of charge carrier dynamics in photovoltaic materials can be used for applications in other optoelectronic devices.
关键词： Perovskites,Nanoscale mapping and ion migration,Grain boundary,Charge carrier dynamics
更新于2025-09-23 15:21:01
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Effect of indium alloying on the charge carrier dynamics of thick-shell InP/ZnSe quantum dots
摘要： Thick-shell InP/ZnSe III–V/II–VI quantum dots (QDs) were synthesized with two distinct interfaces between the InP core and ZnSe shell: alloy and core/shell. Despite sharing similar optical properties in the spectral domain, these two QD systems have differing amounts of indium incorporation in the shell as determined by high-resolution energy-dispersive x-ray spectroscopy scanning transmission electron microscopy. Ultrafast fluorescence upconversion spectroscopy was used to probe the charge carrier dynamics of these two systems and shows substantial charge carrier trapping in both systems that prevents radiative recombination and reduces the photoluminescence quantum yield. The alloy and core/shell QDs show slight differences in the extent of charge carrier localization with more extensive trapping observed in the alloy nanocrystals. Despite the ability to grow a thick shell, structural defects caused by III–V/II–VI charge carrier imbalances still need to be mitigated to further improve InP QDs.
关键词： indium alloying,InP/ZnSe,charge carrier dynamics,photoluminescence quantum yield,quantum dots
更新于2025-09-23 15:21:01
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How the Mixed Cations (Guanidium, Formamidinium, and Phenylethylamine) in Tin Iodide Perovskites Affect Their Charge Carrier Dynamics and Solar Cell Characteristics
摘要： Despite recent interest in lead-free Sn iodide perovskite (ASnI3) solar cells, the role of mixed A-site cations is yet to be fully understood. Here, we report the effect of the ternary mixing of organic A-site cations (guanidium, GA; formamidinium, FA; and phenylethylamine, PEA) on the solar cell performance and charge carrier dynamics that are evaluated using time-resolved microwave conductivity (TRMC). (GAxFA1?x)0.9PEA0.1SnI3 exhibits the maximum power conversion efficiency (PCE) of 7.90% at x = 0.15 and a drastic decrease with increasing GA content. Notably, our TRMC measurements of ASnI3 with/without a hole transport layer reveal the same trend with the devices. From the analyses, we suggest that a variation of electron mobility affected by the location of the GA cation in the grains significantly impacts the PCE. Our work sheds light on the role of mixed A-site cations and directs a route toward the further development of Sn perovskite solar cells.
关键词： time-resolved microwave conductivity,mixed A-site cations,solar cell performance,Sn iodide perovskite,charge carrier dynamics,lead-free
更新于2025-09-23 15:21:01
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Gradient Formation and Charge Carrier Dynamics of CuBiI4 based Perovskite-like Solar Cells
摘要： Designing lead-free inorganic perovskite or perovskite-like structure materials and researching the corresponding photoinduced charge carrier dynamics are always promising due to both the environment and power conversion efficiency considerations. In this work, we intelligently employ bilayer metal Bi/Cu thin film with different atomic ratios as precursor to in-situ fabricate CuBiI4 perovskite-like film with controlled Bi gradient at room temperature. This structure can significantly affect the photoinduced charge carrier dynamic of the resulting products. Next, a series of transient surface photovoltage (TSPV) measurements have been carried out to investigate the photoinduced charge carrier dynamics of such CuBiI4 and CuBiI4: organic hybrid thin films. It reveals that the gradually decreased Bi content from ITO to CuBiI4 can help the photoinduced charge carrier transportation. Finally, a champion PCE of 1.10% has been obtained from an ITO/ CuBiI4: polythieno[3,4-b]-thiophene-co-benzodithiophene (PTB7)/ Au solar cell device. In particular, we find an exact negative correlation of the defined parameter L (the defined value for evaluating the photoinduced charge carrier dynamic in TSPV measurements) with the corresponding PCE of various devices for the first time, which may pave a new way for evaluating the potential photoelectric and photovoltaic performances of new materials without assembly of solar cell devices.
关键词： CuBiI4,solar cell,photoinduced charge carrier dynamics,lead-free inorganic perovskite,transient surface photovoltage
更新于2025-09-23 15:19:57
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Grain Boundaries Limit the Charge Carrier Transport in Pulsed Laser Deposited ?±-SnWO <sub/>4</sub> Thin Film Photoabsorbers
摘要： Recently, α-SnWO4 attracted attention as a material to be used as a top absorber in a tandem device for photoelectrochemical water splitting due to its nearly optimum bandgap of ~1.9?eV and an early photocurrent onset potential of ~0 V vs. RHE. However, the mismatch between the charge carrier diffusion length and light penetration depth—which is typical for metal oxide semiconductors—currently hinders the realization of high photoconversion efficiencies. In this work, the pulsed laser deposition process and annealing treatment of α-SnWO4 thin films are elucidated in order to optimize their charge carrier transport properties. A high temperature treatment is found to enhance the photoconductivity of α-SnWO4 by more than one order of magnitude, as measured with time-resolved microwave conductivity (TRMC). A complimentary analysis by time-resolved terahertz spectroscopy (TRTS) shows that this improvement can be assigned to an increase of the grain size in the heat-treated films. In addition, TRTS reveals electron-hole charge carrier mobilities of up to 0.13 cm2 V-1s-1 in α-SnWO4. This is comparable to values found for BiVO4, which is one of the best performing metal oxide photoanode materials to date. These findings show that there is a significant potential for further improving the properties of α-SnWO4 photoanodes.
关键词： α-SnWO4,metal oxide photoelectrodes,grain boundaries,charge carrier dynamics,pulsed laser deposition
更新于2025-09-23 15:19:57
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Investigating ultrafast carrier dynamics in perovskite solar cells with an extended ??-conjugated polymeric diketopyrrolopyrrole layer for hole transportation
摘要： Here, we show a new diketopyrrole based polymeric hole-transport material (PBDTP-DTDPP, (poly[[2,5-bis(2-hexyldecyl)-2,3,5,6-tetrahydro-3,6-dioxopyrrolo[3,4-c]pyrrole-1,4-diyl]-alt-[[2,20-(4,8-bis(4-ethylhexyl-1-phenyl)-benzo[1,2-b:4,5-b0]dithiophene)bis-thieno[3,2-b]thiophen]-5,50-diyl]])) in perovskite solar cells. The material performance was tested in a solar cell with an optimized configuration, FTO/SnO2/perovskite/PBDTP-DTDPP/Au, and the device showed a power conversion efficiency of 14.78%. The device charge carrier dynamics were investigated using transient absorption spectroscopy. The charge separation and recombination kinetics were determined in a device with PBDTP-DTDPP and the obtained results were compared to a reference device. We find that PBDTP-DTDPP enables similar charge separation time (<4.8 ps) to the spiro-OMeTAD but the amount of nongeminate recombination is different. Specifically, we find that the polymeric PBDTP-DTDPP hole-transport layer (HTL) slows-down the second-order recombination much less than spiro-OMeTAD. This effect is of particular importance in studying the charge transportation in optimized solar cell devices with diketopyrrole based HTL materials.
关键词： perovskite solar cells,transient absorption spectroscopy,PBDTP-DTDPP,charge carrier dynamics,hole-transport material
更新于2025-09-23 15:19:57
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Ultrafast THz photophysics of solvent engineered triple-cation halide perovskites
摘要： Solution processed thin film organic-inorganic perovskites are key to the large scale manufacturing of next generation wafer scale solar cell devices. The high efficiency of the hybrid perovskite solar cells is derived mainly from the large carrier mobility and the charge dynamics of films, which heavily depend on the type of solvent used for the material preparation. Here, we investigate the nature of conduction and charge carrier dynamics of mixed organic-inorganic cations [methylammonium (MA), formamidinium (FA), and cesium (Cs)] along with the mixed halides [iodine (I) and bromine (Br)] perovskite material [Cs0.05(MA0.17FA0.83)0.95Pb(I0.83Br0.17)3] synthesized in different solvents using optical pump terahertz probe (OPTP) spectroscopy. Our findings reveal that carrier mobilities and diffusion lengths strongly depend on the type of solvent used for the preparation of the mixed cation perovskite film. The mixed cation perovskite film prepared using dimethylformamide/dimethylsulfoxide solvent shows greater mobility and diffusion length compared to γ-butyrolactone solvent. Our findings provide valuable insights to improve the charge carrier transport in mixed cation perovskites through solvent engineering.
关键词： charge carrier dynamics,OPTP spectroscopy,diffusion length,perovskites,carrier mobility,solvent engineering
更新于2025-09-09 09:28:46
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Electronic Traps and Phase Segregation in Lead Mixed-Halide Perovskite
摘要： An understanding of the factors driving halide segregation in lead mixed-halide perovskites is required for their implementation in tandem solar cells with existing silicon technology. Here we report that the halide segregation dynamics observed in the photoluminescence from CH3NH3Pb(Br0.5I0.5)3 is strongly influenced by the atmospheric environment, and that encapsulation of films with a layer of poly(methyl methacrylate) allows for halide segregation dynamics to be fully reversible and repeatable. We further establish an empirical model directly linking the amount of halide segregation observed in the photoluminescence to the fraction of charge-carriers recombining through trap-mediated channels, and the photon flux absorbed. From such quantitative analysis we show that under pulsed illumination, the frequency of the modulation alone has no influence on the segregation dynamics. Additionally, we extrapolate that working CH3NH3Pb(Br0.5I0.5)3 perovskite cells would require a reduction of the trap-related charge-carrier recombination rate to (cid:46) 105 s?1 in order for halide segregation to be sufficiently suppressed.
关键词： photoluminescence,lead mixed-halide perovskites,halide segregation,charge-carrier dynamics,trap-mediated recombination
更新于2025-09-09 09:28:46