论文标题
自适应尖端增强的纳米光谱
Adaptive tip-enhanced nano-spectroscopy
论文作者
论文摘要
尖端增强的纳米光谱和成像,例如尖端增强的光致发光(TEPL),尖端增强的拉曼光谱(TERS)等,从材料科学到单个分子研究已成为必不可少的。然而,由于缺乏对尖端顶端结构的纳米级控制,这些技术的性能不一致,这通常会导致不可重复的光谱,空间和极化解决成像。我们采用自适应光学元件来优化尖端矢量场的逆方法,而是采用逆方法,而是通过适应性的方法来解决此问题。具体而言,我们展示了激发场的动态波前塑形,以有效地将光线与尖端搭配,并自适应地控制,以增强灵敏度和极化控制的TEPL和TER,其性能超过了传统的尖端装饰和最佳激发偏置可以实现的目标。 Employing a sequence feedback algorithm, we achieve 4.4$\times$10$^4$-fold TEPL enhancement of a WSe$_2$ monolayer which is >2$\times$ larger than the normal TEPL intensity without wavefront shaping, as well as the largest plasmon-enhanced PL intensity of a transition metal dichalcogenide (TMD) monolayer reported to date.此外,在TERS中,动态近极化控制,我们证明了亮甲三甲蓝色(BCB)分子的构象异质性以及由于较大的梯度场效应而对IR活性模式的可控观察。因此,自适应尖端增强的光谱和成像为计算纳米镜检查提供了一种新的系统方法,从而使光学纳米成像更健壮,多功能且可部署。
Tip-enhanced nano-spectroscopy and -imaging, such as tip-enhanced photoluminescence (TEPL), tip-enhanced Raman spectroscopy (TERS), and others, have become indispensable from materials science to single molecule studies. However, the techniques suffer from inconsistent performance due to lack of nanoscale control of tip apex structure, which often leads to irreproducible spectral, spatial, and polarization resolved imaging. Instead of refining tip-fabrication to resolve this problem, we pursue the inverse approach of optimizing the nano-optical vector-field at the tip apex via adaptive optics. Specifically, we demonstrate dynamic wavefront shaping of the excitation field to effectively couple light to the tip and adaptively control for enhanced sensitivity and polarization-controlled TEPL and TERS, with performance exceeding what can be achieved by conventional tip-fabrication and optimal excitation polarization. Employing a sequence feedback algorithm, we achieve 4.4$\times$10$^4$-fold TEPL enhancement of a WSe$_2$ monolayer which is >2$\times$ larger than the normal TEPL intensity without wavefront shaping, as well as the largest plasmon-enhanced PL intensity of a transition metal dichalcogenide (TMD) monolayer reported to date. In addition, with dynamical near-field polarization control in TERS, we demonstrate the investigation of conformational heterogeneity of brilliant cresyl blue (BCB) molecules as well as the controllable observation of IR-active modes due to a large gradient field effect. Adaptive tip-enhanced spectroscopy and imaging thus provides for a new systematic approach towards computational nanoscopy making optical nano-imaging more robust, versatile, and widely deployable.