Colloidal-quantum-dot (CQD) photovoltaic devices are promising candidates for low-cost power sources owing to their low-temperature solution processability and bandgap tunability. A power conversion efficiency (PCE) of >10% is achieved for these devices; however, there are several remaining obstacles to their commercialization, including their high energy loss due to surface trap states and the complexity of the multiple-step CQD-layer-deposition process. Herein, high-efficiency photovoltaic devices prepared with CQD-ink using a phase-transfer-exchange (PTE) method are reported. Using CQD-ink, the fabrication of active layers by single-step coating and the suppression of surface trap states are achieved simultaneously. The CQD-ink photovoltaic devices achieve much higher PCEs (10.15% with a certified PCE of 9.61%) than the control devices (7.85%) owing to improved charge drift and diffusion. Notably, the CQD-ink devices show much lower energy loss than other reported high-efficiency CQD devices. This result reveals that the PTE method is an effective strategy for controlling trap states in CQDs.
While perovskite solar cells (PSCs) have emerged as promising low-cost solar power generators, most reported high-performance PSCs employ electron transport layers (ETLs, mainly TiO2) treated at high temperatures (≥450 °C), which may eventually hinder the development of flexible PSCs. Meanwhile, the development of low-temperature processed PSCs (L-PSCs) possessing performance levels comparable to those of high-temperature processed PSCs has actively been reported. In this study, L-PSCs with improved long-term stability and negligible hysteresis were developed through the effective passivation of shallow and deep traps in organic–inorganic hybrid perovskite (OIHP) crystals and at the ETL/OIHP interface. L-PSCs with alkaline chloride modification achieved state-of-the-art performance among reported L-PSCs (power conversion efficiency (PCE) = 22.6%) with a long-term shelf life. The origin of long-term stability and the efficient passivation of deep traps was revealed by monitoring the trap-state distribution. Moreover, the high PCE of a large-area device (21.3%, 1.12 cm2) was also demonstrated, confirming the uniformity of the modification.
IntroductionColloidal quantum dot (CQD) based photovoltaic devices (CQDPVs) have emerged as promising next-generation solar cells owing to low-cost solution processibility at low temperature, easy bandgap tunability into the near infrared (NIR, λ > 800 nm) regime, and multiple exciton generation. [1,2] The power conversion efficiency (PCE) of CQDPVs has improved High-efficiency solid-state-ligand-exchange (SSE) step-free colloidal quantum dot photovoltaic (CQDPV) devices are developed by employing CQD ink based active layers and organic (Polythieno[3,4-b]-thiophene-co-benzodithiophene (PTB7) and poly(3-hexylthiophene) (P3HT)) based hole transport layers (HTLs). The device using PTB7 as an HTL exhibits superior performance to that using the current leading organic HTL, P3HT, because of favorable energy levels, higher hole mobility, and facilitated interfacial charge transfer. The PTB7 based device achieves power conversion efficiency (PCE) of 9.60%, which is the highest among reported CQDPVs using organic HTLs. This result is also comparable to the PCE of an optimized device based on a thiol-exchanged p-type CQD, the current-state-of-the-art HTL. From the viewpoint of device processing, the fabrication of CQDPVs is achieved by direct single-coating of CQD active layers and organic HTLs at low temperature without SSE steps. The experimental results and device simulation results in this work suggest that further engineering of organic HTL materials can open new doors to improve the performance and processing of CQDPVs.
Organic p‐type materials are potential candidates as solution processable hole transport materials (HTMs) for colloidal quantum dot solar cells (CQDSCs) because of their good hole accepting/electron blocking characteristics and synthetic versatility. However, organic HTMs have still demonstrated inferior performance compared to conventional p‐type CQD HTMs. In this work, organic π‐conjugated polymer (π‐CP) based HTMs, which can achieve performance superior to that of state‐of‐the‐art HTM, p‐type CQDs, are developed. The molecular engineering of the π‐CPs alters their optoelectronic properties, and the charge generation and collection in CQDSCs using them are substantially improved. A device using PBDTTPD‐HT achieves power conversion efficiency (PCE) of 11.53% with decent air‐storage stability. This is the highest reported PCE among CQDSCs using organic HTMs, and even higher than the reported best solid‐state ligand exchange‐free CQDSC using pCQD‐HTM. From the viewpoint of device processing, device fabrication does not require any solid‐state ligand exchange step or layer‐by‐layer deposition process, which is favorable for exploiting commercial processing techniques.
While hole extraction is crucial for the external quantum efficiency of conventional n-i-p colloidal quantum dot (CQD) solar cells (CQDSCs), sulfur-passivated p-type CQDs (pCQDs) have been the best hole-transport material (HTM) thus far. In this work, we developed organic πconjugated polymers (π-CPs) that can achieve substantially improved HTM performance compared with conventional pCQDs. A weakly electron-withdrawing triisopropylsilylethynyl (TIPS) group was employed with a weak donor moiety, benzo[1,2-b:4,5:b']-dithiophene (BDT), in the push-pull structured π-CPs to optimize the optoelectronic properties of the HTM. The CQDSCs using TIPS-containing π-CPs achieved a substantially higher PCE (13.03%) than those previously reported using pCQD (11.33%) or π-CPs (11.25%) owing to the improved charge collection efficiency near the photoactive CQD layer/HTM interface. To the best of our knowledge, our CQDSCs using TIPS-based π-CPs achieved the highest reported PCE among SSE-free CQDSCs.
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