Benzoquinone-Induced Hot Carrier Extraction in Red-Emitting Perovskite Nanocrystals

IF 3.2 3区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry C Pub Date : 2025-07-30 DOI:10.1021/acs.jpcc.5c03551

Shreya Mishra, Debopam Acharjee*, Soumik De, Asit Baran Mahato, Mrinal Kanti Panda, Dipak Samanta, Surajit Ghosh and Subhadip Ghosh*,

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Abstract

We investigate the ultrafast cooling and extraction dynamics of hot carriers (HCs) in red-emitting CsPbI₃ perovskite nanocrystals using femtosecond upconversion spectroscopy. Time-resolved photoluminescence (TRPL) at the red emission wavelength reveals an ∼830 fs rise component under far band-edge excitation (λ_ex ≈ 405 nm), which accelerates to ∼520 fs with near band-edge excitation (λ_ex ≈ 430 nm), consistent with cooling phenomena. Upon the addition of benzoquinone (BQ), these rise time scales shorten to ≤330 fs, suggesting that cooling is at least partially complete prior to charge transfer. Fluorescence correlation spectroscopy reveals that the nanocrystal–BQ complexation reaction occurs on a significantly slower time scale (∼570 μs), confirming that the ultrafast extraction process is complete when the complex remains intact. Our study reveals the intrinsic time scale of HC transfer in the CsPbI₃ nanocrystal–BQ composite and offers key mechanistic insights into their harvesting, highlighting the potential of CsPbI₃ perovskite materials for high-efficiency photovoltaic and optoelectronic applications.

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红光钙钛矿纳米晶体中苯醌诱导的热载流子萃取

利用飞秒上转换光谱研究了红发CsPbI3钙钛矿纳米晶体中热载流子（hc）的超快冷却和萃取动力学。红色发射波长处的时间分辨光致发光（TRPL）在远波段激发（λex≈405 nm）下显示出~ 830 fs的上升分量，在近波段激发（λex≈430 nm）下加速到~ 520 fs，与冷却现象一致。在加入苯醌（BQ）后，这些上升时间尺度缩短到≤330 fs，这表明在电荷转移之前至少部分完成了冷却。荧光相关光谱显示，纳米晶体- bq络合反应发生在明显较慢的时间尺度上（~ 570 μs），证实了当配合物保持完整时，超快萃取过程完成。我们的研究揭示了CsPbI3纳米晶体- bq复合材料中HC转移的内在时间尺度，并为其收获提供了关键的机制见解，突出了CsPbI3钙钛矿材料在高效光伏和光电子应用中的潜力。

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来源期刊

The Journal of Physical Chemistry C 化学-材料科学：综合

CiteScore

6.50

自引率

8.10%

发文量

2047

审稿时长

1.8 months

期刊介绍： The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.