纳米半导体中多重激子效应研究进展
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摘要
多重激子效应是指纳米半导体吸收一个高能光子后产生两个甚至多个电子-空穴对的物理过程,不仅具有重要的基础研究意义,而且在新型太阳电池及高性能光电子器件领域具有潜在应用价值.综述了多重激子效应的发展历程;总结了纳米半导体的材料组分、体系结构甚至表面质量对多重激子效应的影响;介绍了多重激子效应的实验测试分析方法以及解释多重激子效应的理论方法;概括了目前多重激子效应在器件中的应用并对其应用前景进行展望.
The multiple exciton generation(MEG), a process in which two or even more electron-hole pairs are created in nanostructured semiconductors by absorbing a single high-energy photon, is fundamentally important in many fields of physics, e.g., nanotechnology and optoelectronic devices. Many high-performance optoelectronic devices can be achieved with MEG where quite an amount of the energy of an absorbed photon in excess of the band gap is used to generate morei additional electron-hole pairs instead of rapidly lost heat. In this review, we present a survey on both the research context and the recent progress in the understanding of MEG. This phenomenon has been experimentally observed in the OD nanocrystals, such as PbX(X = Se, S, and Te), InX(X = As and P), CdX(X = Se and Te), Si, Ge, and semi-metal quantum dots, which produce the differential quantum efficiency as high as 90%±10%. Even more remarkably, experiment advances have made it possible to realize MEG in the one-dimensional(1 D) semiconductor nanorods and the twodimensional(2 D) nano-thin films. Theoretically, three different approaches, i.e., the virtual exciton generation approach,the coherent multiexciton mode, and the impact ionization mechanism, have been proposed to explain the MEG effect in semiconductor nanostructures. Experimentally, the MEG has been measured by the ultrafast transient spectroscopy, such as the ultrafast transient absorption, the terahertz ultrafast transient absorption, the transient photoluminescence, and the transient grating technique. It is shown that the properties of nanostructured semiconductors, e.g., the composition,structure and surface of the material, have dramatic effects on the occurrence of MEG. As a matter of fact, it is somewhat hard to experimentally confirm the signature of MEG in nanostructured semiconductors due to two aspects:i) the time scale of the MEG process is very short; ii) the excitation fiuence should be extremely low to prevent the multiexcitons from being generated by multiphoton absorption. There are still some controversies with respect to the MEG effect due to the challenge in both the experimental measurement and the explanation of signal data. The successful applications of MEG in practical devices, of which each is composed of the material with lower MEG threshold and higher efficiency, require the extraction of multiple charge carriers before their ultrafast annihilation. Such an extraction can be realized by the ultrafast electron transfer from nanostructured semiconductors to molecular and semiconductor electron acceptors. More recently, an experiment with PbSe quantum dot photoconductor has demonstrated that the multiple charge extraction is even as high as 210%. It is proved that MEG is of applicable significance in optoelectronic devices and in ultra-efficient photovoltaic devices. Although there are still some challenges, the dramatic enhancement of the efficiency of novel optoelectronic devices by the application of MEG can be hopefully realized with the rapid improvement of nanotechnology.
The multiple exciton generation(MEG), a process in which two or even more electron-hole pairs are created in nanostructured semiconductors by absorbing a single high-energy photon, is fundamentally important in many fields of physics, e.g., nanotechnology and optoelectronic devices. Many high-performance optoelectronic devices can be achieved with MEG where quite an amount of the energy of an absorbed photon in excess of the band gap is used to generate morei additional electron-hole pairs instead of rapidly lost heat. In this review, we present a survey on both the research context and the recent progress in the understanding of MEG. This phenomenon has been experimentally observed in the OD nanocrystals, such as PbX(X = Se, S, and Te), InX(X = As and P), CdX(X = Se and Te), Si, Ge, and semi-metal quantum dots, which produce the differential quantum efficiency as high as 90%±10%. Even more remarkably, experiment advances have made it possible to realize MEG in the one-dimensional(1 D) semiconductor nanorods and the twodimensional(2 D) nano-thin films. Theoretically, three different approaches, i.e., the virtual exciton generation approach,the coherent multiexciton mode, and the impact ionization mechanism, have been proposed to explain the MEG effect in semiconductor nanostructures. Experimentally, the MEG has been measured by the ultrafast transient spectroscopy, such as the ultrafast transient absorption, the terahertz ultrafast transient absorption, the transient photoluminescence, and the transient grating technique. It is shown that the properties of nanostructured semiconductors, e.g., the composition,structure and surface of the material, have dramatic effects on the occurrence of MEG. As a matter of fact, it is somewhat hard to experimentally confirm the signature of MEG in nanostructured semiconductors due to two aspects:i) the time scale of the MEG process is very short; ii) the excitation fiuence should be extremely low to prevent the multiexcitons from being generated by multiphoton absorption. There are still some controversies with respect to the MEG effect due to the challenge in both the experimental measurement and the explanation of signal data. The successful applications of MEG in practical devices, of which each is composed of the material with lower MEG threshold and higher efficiency, require the extraction of multiple charge carriers before their ultrafast annihilation. Such an extraction can be realized by the ultrafast electron transfer from nanostructured semiconductors to molecular and semiconductor electron acceptors. More recently, an experiment with PbSe quantum dot photoconductor has demonstrated that the multiple charge extraction is even as high as 210%. It is proved that MEG is of applicable significance in optoelectronic devices and in ultra-efficient photovoltaic devices. Although there are still some challenges, the dramatic enhancement of the efficiency of novel optoelectronic devices by the application of MEG can be hopefully realized with the rapid improvement of nanotechnology.
引文
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