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中国物理学会期刊

厚度梯度MoS2的能带漏斗效应及其电荷转移行为

CSTR: 32037.14.aps.74.20250661

Energy funneling effect and charge transfer behavior of MoS2 with thickness gradient

CSTR: 32037.14.aps.74.20250661
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  • 二维层状材料的能带漏斗效应为调控电荷转移提供了重要手段. 然而, 关于能带漏斗的实现及其对电荷转移速率的影响仍缺乏理解. 本文通过解析推导和第一性原理计算方法, 提出通过构建具有厚度梯度的MoS2实现能带漏斗效应, 并分析能带漏斗效应对电荷转移速率的影响. 结果表明, MoS2的带隙随层数减少呈单调递增趋势, 使得双厚度梯度和三厚度梯度MoS2均可实现能带漏斗效应, 电荷会从薄层区域往厚层区域定向传输. 此外, 不同层数MoS2界面处能级差诱导的驱动力是调控载流子聚集能力的重要因素, 在双厚度梯度单层/块体MoS2的电荷转移速率可达 4.97 \times 10^13\text s^ - 1 . 这些结果为设计能带漏斗以及理解能带漏斗效应调控电荷转移行为提供物理基础.

     

    Energy funneling effect of two-dimensional materials provides an important method for modulating carrier transfer. However, the formation of energy funneling and its influences on the carrier transfer are still relatively uncharacterized. In this work, the energy funneling induced by the layer number gradient effect in MoS2 is investigated through atomic-bond-relaxation approach and first-principles calculations. It is found that the bandgap of MoS2 monotonically increases with the decrease of the layer number, leading the conduction band minimum (valence band maximum) of thin layer MoS2 to be higher than (lower than) that of thick layer MoS2. Therefore, both dual thickness gradient and triple thickness gradient MoS2 can achieve the energy funneling effect. As a result, the carriers will be directionally transferred from the thin layer region to the thick layer region. According to Marcus theory, the carrier transfer rate is dependent on drive force caused by the energy level difference with different thicknesses of MoS2. For the dual thickness gradient MoS2, when the thickness difference between adjacent layers is the largest, the driving force is the highest, which is 1L/bulk. In addition, owing to the driving force smaller than the reorganization energy in dual thickness gradient MoS2, a large driving force corresponds to a high carrier transfer rate, resulting in a higher carrier transfer rate of 1L/bulk than those in other dual thickness gradient systems. For the triple thickness gradient MoS2, there are two consecutive interface energy differences that induce driving forces. However, the carrier transfer rate is exponentially correlated with the driving force. Therefore, the carrier transfer rate of dual thickness gradient MoS2 will be higher than that of the corresponding triple thickness gradient MoS2. Our results demonstrate that the energy funneling effect induced by thickness gradient can realize carrier accumulation in the thick layer region without the need for p-n junctions, which is of great benefit in collecting photogenerated carriers. The atomic force microscopy lithography and chemical vapor deposition will be used to engineer thickness-gradient two-dimensional materials with enhanced optoelectronic properties in future.

     

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