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Plasmon-Induced Ultrafast Hot Hole Transfer in Nonstoichiometric CuxInyS/CdS Heteronanocrystals
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2024-05-03 , DOI: 10.1021/acs.jpclett.4c00712
Nitika Kharbanda 1 , Manvi Sachdeva 1 , Nandan Ghorai 1 , Arshdeep Kaur 1 , Vikas Kumar 1 , Hirendra N. Ghosh 2
Affiliation  

Plasmonic semiconductors are promising candidates for developing energy conversion devices due to their tunable band gap, cost-effectiveness, and nontoxicity. Such materials exhibit remarkable capabilities for harvesting infrared photons, which constitute half of the solar energy spectrum. Herein, we have synthesized near-infrared (NIR) active CuxInyS nanocrystals and CuxInyS/CdS heterostructure nanocrystals (HNCs) to investigate plasmon-induced charge transfer dynamics on an ultrafast time scale. Employing femtosecond transient absorption spectroscopy, we demonstrate that upon exciting the HNCs with sub-band gap NIR photons (λ = 840 nm), the hot holes are generated in the valence band of plasmonic CuxInyS and transferred to the adjacent semiconductor. The decreased signal intensity and accelerated hole phonon relaxation dynamics for HNCs reveal efficient transfer of plasmon-induced hot carriers from CuxInyS to CdS under both 840 and 350 nm laser excitations, providing a pathway for enhanced carrier utilization. These findings shed light on the potential of ternary chalcogenides in plasmonic applications, highlighting efficient hot carrier extraction to adjacent semiconductors.

中文翻译:


非化学计量 CuxInyS/CdS 异质晶体中等离激元诱导的超快热空穴传输



等离激元半导体由于其带隙可调、成本效益和无毒性,是开发能量转换器件的有希望的候选者。此类材料在收集红外光子方面表现出卓越的能力,红外光子占太阳能光谱的一半。在此,我们合成了近红外(NIR)活性Cu x In y S纳米晶和Cu x In y S/CdS异质结构纳米晶体(HNC)用于在超快时间尺度上研究等离激元诱导的电荷转移动力学。采用飞秒瞬态吸收光谱,我们证明在用子带隙近红外光子(λ = 840 nm)激发 HNC 时,等离激元 Cu x 的价带中会产生热空穴。 S并转移到相邻的半导体。 HNC 的信号强度降低和空穴声子弛豫动力学加速揭示了在 840 和 350 nm 激光激发下等离激元诱导的热载流子从 Cu x In y S 到 CdS 的有效转移,提供提高载体利用率的途径。这些发现揭示了三元硫属化物在等离子体应用中的潜力,强调了对相邻半导体的有效热载流子提取。
更新日期:2024-05-03
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