期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 33, 页码 15175-15184出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c05316
关键词
-
资金
- SNSF [200020_178860]
- H2020 Marie Sklodowska-Curie Individual fellowship [101024144]
- KACST
- Marie Curie Actions (MSCA) [101024144] Funding Source: Marie Curie Actions (MSCA)
By studying layered hybrid perovskite analogues, we identified the factors that limit the efficiency of DNP NMR for perovskite samples. We found that the fast-relaxing dynamic cation is the major impediment, but this can be mitigated by deuteration, leading to significant DNP enhancement.
Surface and bulk molecular modulators are the key to improving the efficiency and stability of hybrid perovskite solar cells. However, due to their low concentration, heterogeneous environments, and low sample mass, it remains challenging to characterize their structure and dynamics at the atomic level, as required to establish structure-activity relationships. Nuclear magnetic resonance (NMR) spectroscopy has revealed a wealth of information on the atomic-level structure of hybrid perovskites, but the inherent insensitivity of NMR severely limits its utility to characterize thin-film samples. Dynamic nuclear polarization (DNP) can enhance NMR sensitivity by orders of magnitude, but DNP methods for perovskite materials have so far been limited. Here, we determined the factors that limit the efficiency of DNP NMR for perovskite samples by systematically studying layered hybrid perovskite analogues. We find that the fast-relaxing dynamic cation is the major impediment to higher DNP efficiency, while microwave absorption and particle morphology play a secondary role. We then show that the former can be mitigated by deuteration, enabling 1H DNP enhancement factors of up to 100, which can be harnessed to enhance signals from dopants or additives present in very low concentrations. Specifically, using this new DNP methodology at a high magnetic field and with small sample volumes, we have recorded the NMR spectrum of the 20 nm (6 mu g) passivating layer on a single perovskite thin film, revealing a two-dimensional (2D) layered perovskite structure at the surface that resembles the n = 1 homologue but which has greater disorder than in bulk layered perovskites.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据