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An Insight into the Interface through Excited-State Carrier Dynamics for Promising Enhancement of Power Conversion Efficiency in a Mn-Doped CdZnSSe Gradient Alloy

机译:通过激励状态载波动态对界面的洞察,以便在MN掺杂Cdznsse梯度合金中提高功率转换效率的提高

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To explore the significance of impurity doping in power conversion efficiency, quaternary gradient CdZnSSe alloy nanocrystals (NCs) and its Mn-doped analogues were synthesized by high-temperature pyrolysis. The undoped and Mn-doped CdZnSSe alloy NCs have been characterized by employing high-resolution TEM, X-ray diffraction, energydispersive X-ray spectroscopy, and electron paramagnetic resonance spectroscopy measurements. A low-temperature injection of chalcogens led to a gradient interface in the alloy, comprised of a CdSe/CdS/ZnSe/ZnS nanostructure. Both steady-state and ultrafast time-resolved absorption studies suggested the formation of a charge-transfer (CT) state due to the inner quasi-type II CdSe/CdS part of the gradient CdZnSSe alloy NCs, in which electrons are delocalized throughout the conduction band (CB) of both CdSe and CdS. The CT-state bleach recovery kinetics gave an additional slow electron cooling component (8 ps) in the undoped alloy NCs, which has been assigned to electron equilibration in the delocalized CB before recombination (or trapping). Interestingly, in the presence of dopant Mn, the slow electron cooling component became even more sluggish at 10 ps due to Mn-mediated electron cooling, in which Mn acts as an electron storage center. An unprecedented increase in the photocurrent conversion efficiency (PCE) of approximately 30% from (3.3±0.11) to (4.29±0.07)% was observed in the Mn-doped gradient alloy compared with the undoped alloy.
机译:为了探讨杂质掺杂在功率转换效率中的重要性,通过高温热解合成季梯度Cdznsse合金纳米晶纳米晶(NC)及其Mn掺杂类似物。未掺杂的和MN掺杂的CDZNSSE合金NCS的特征在于采用高分辨率TEM,X射线衍射,能量渗透X射线光谱测量和电子顺磁共振光谱测量。低温注入胆醌导致合金中的梯度界面,包括CDSE / Cds / ZnSe / ZnS纳米结构。稳态和超快时间分辨吸收研究都提出了由于梯度CDZNSSE合金NCS的内部准型II CDSE / CDS部分而形成的电荷转移(CT)状态,其中电子在整个传导过程中划分CDSE和CD的频段(CB)。 CT状态漂白恢复动力学在未掺杂的合金NCS中提供了额外的慢电子冷却组分(8SP),其在重组(或捕获)之前已被分配给截匙CB中的电子平衡。有趣的是,由于Mn介导的电子冷却,在掺杂剂Mn的存在下,慢电子冷却部件在10 p时变得更加缓慢,其中Mn用作电子存储中心。与未掺杂的合金相比,在MN掺杂的梯度合金中观察到光电流转化效率(PCCE)的前所未有的升高,从(3.3±0.11)至(4.29±0.07)%。

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