Disentangling the components of a multiconfigurational excited state in isolated chromophore with light-scanning-tunneling microscopy

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Rodrigo Cezar de Campos Ferreira, Amandeep Sagwal, Jiří Doležal, Tomáš Neuman, Martin Švec
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引用次数: 0

Abstract

Molecular radicals are efficient electroluminescent emitters due to the spin multiplicity of their electronic states. The excited states often exhibit a complex composition with multiple significant electronic configurations, which are essential for their optoelectronic properties but difficult to probe directly. Here we use light-scanning tunneling microscopy to investigate such an excited state by visualizing the response of a single radical molecule to a laser excitation. We observe characteristic atomic-scale spatial photocurrent patterns that can be tuned by applied bias voltage. We interpret these patterns as resulting from decay of an excited doublet state through sequential electron transfers with the tip and the substrate. The relative contributions of two dominating electronic configurations involved in this excited state are tuned by the applied voltage. This approach thus allows for disentangling the components of multiconfigurational excited states in single molecules.

Abstract Image

用光扫描-隧道显微镜分离孤立发色团中多构型激发态的组分
分子自由基由于其电子态的自旋多重性而成为高效的电致发光体。激发态通常表现出具有多个重要电子构型的复杂组成,这对其光电特性至关重要,但难以直接探测。在这里,我们使用光扫描隧道显微镜通过观察单个自由基分子对激光激发的响应来研究这种激发态。我们观察到可以通过施加偏置电压来调谐的原子级空间光电流模式。我们解释这些图案是由于激发态的衰变,通过顺序的电子转移与尖端和衬底。在激发态中涉及的两种主要电子构型的相对贡献由外加电压调节。因此,这种方法允许解开单个分子中多构型激发态组分的纠缠。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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