Lombardo Chiara, Sottini Andrea, Seiter Sarina, Colas des Francs Gérard, Ortega Arroyo Jaime, Quidant Romain
Nanophotonic Systems Laboratory, Department of Mechanical and Process Engineering, ETH Zurich, Tannenstrasse 3, Zurich 8092, Switzerland.
Université Bourgogne Europe, CNRS, Laboratoire Interdisciplinaire Carnot de Bourgogne ICB UMR 6303, Dijon F-21000, France.
ACS Photonics. 2025 Aug 1;12(8):4376-4387. doi: 10.1021/acsphotonics.5c00744. eCollection 2025 Aug 20.
Interferometric-based microscopies stand as powerful label-free approaches for monitoring and characterizing chemical reactions and heterogeneous nanoparticle systems in real time with single-particle sensitivity. Nevertheless, coherent artifacts, such as speckle and parasitic interferences, together with limited photon fluxes from spatially incoherent sources, pose an ongoing challenge in achieving both high sensitivity and throughput. In this study, we systematically characterize how partial coherence affects the signal contrast and background noise level in inline holography microscopes operated in a reflection geometry, a category that encompasses interferometric scattering microscopy (iSCAT). This approach offers a route to improve the signal-to-noise ratio in the detection of single nanoparticles (NPs), irrespective of their size and composition or the light source used. We first validate that lasers can be modified into partially coherent sources with performance matching that of spatially incoherent ones while providing higher photon fluxes. Second, we demonstrate that tuning the degree of partial coherence not only enhances the detection sensitivity of both synthetic and biological NPs but also affects how signal contrasts vary as a function of the focus position. Finally, we apply our findings to single-protein detection, confirming that these principles extend to differential imaging modalities, which deliver the highest sensitivity. Our results address a critical milestone in the detection of weakly scattering NPs in complex matrices, with wide-ranging applications in biotechnology, nanotechnology, chemical synthesis, and biosensing, ushering in a new generation of microscopes that push both the sensitivity and throughput boundaries without requiring beam scanning.
基于干涉测量的显微镜技术是强大的无标记方法,可用于实时监测和表征化学反应以及具有单粒子灵敏度的异质纳米粒子系统。然而,相干伪像,如散斑和寄生干涉,以及来自空间非相干光源的有限光子通量,在实现高灵敏度和高吞吐量方面仍然是一个持续的挑战。在本研究中,我们系统地表征了部分相干性如何影响在反射几何结构中操作的同轴全息显微镜中的信号对比度和背景噪声水平,该类别包括干涉散射显微镜(iSCAT)。这种方法提供了一种途径,可提高检测单个纳米粒子(NP)时的信噪比,而不论其尺寸、组成或所使用的光源如何。我们首先验证了可以将激光修改为部分相干光源,其性能与空间非相干光源相匹配,同时提供更高的光子通量。其次,我们证明调整部分相干度不仅可以提高合成和生物NP的检测灵敏度,还会影响信号对比度如何随焦点位置变化。最后,我们将我们的发现应用于单蛋白检测,证实这些原理扩展到差分成像模式,可提供最高的灵敏度。我们的结果解决了在复杂基质中检测弱散射NP的一个关键里程碑,在生物技术、纳米技术、化学合成和生物传感中有广泛应用,开创了新一代显微镜,无需光束扫描即可突破灵敏度和吞吐量的界限。