Advanced Light Source Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
Departments of Physics andChemistry, University of Colorado, Boulder, CO 80309; andJILA, University of Colorado and National Institute of Standards and Technology, Boulder, CO 80309.
Proc Natl Acad Sci U S A. 2014 May 20;111(20):7191-6. doi: 10.1073/pnas.1400502111. Epub 2014 May 6.
Characterizing and ultimately controlling the heterogeneity underlying biomolecular functions, quantum behavior of complex matter, photonic materials, or catalysis requires large-scale spectroscopic imaging with simultaneous specificity to structure, phase, and chemical composition at nanometer spatial resolution. However, as with any ultrahigh spatial resolution microscopy technique, the associated demand for an increase in both spatial and spectral bandwidth often leads to a decrease in desired sensitivity. We overcome this limitation in infrared vibrational scattering-scanning probe near-field optical microscopy using synchrotron midinfrared radiation. Tip-enhanced localized light-matter interaction is induced by low-noise, broadband, and spatially coherent synchrotron light of high spectral irradiance, and the near-field signal is sensitively detected using heterodyne interferometric amplification. We achieve sub-40-nm spatially resolved, molecular, and phonon vibrational spectroscopic imaging, with rapid spectral acquisition, spanning the full midinfrared (700-5,000 cm(-1)) with few cm(-1) spectral resolution. We demonstrate the performance of synchrotron infrared nanospectroscopy on semiconductor, biomineral, and protein nanostructures, providing vibrational chemical imaging with subzeptomole sensitivity.
要描述和最终控制生物分子功能、复杂物质的量子行为、光子材料或催化作用的基础异质性,需要在纳米空间分辨率下对结构、相和化学成分进行同时特异性的大规模光谱成像。然而,与任何超高空间分辨率显微镜技术一样,对空间和光谱带宽的增加的需求通常会导致所需灵敏度的降低。我们使用同步加速器中红外辐射克服了红外振动散射扫描探针近场光学显微镜中的这一限制。通过低噪声、宽带和空间相干的高光谱辐照度同步加速器光来诱导低噪声、宽带和空间相干的同步加速器光,通过外差干涉放大来灵敏地检测近场信号。我们实现了具有快速光谱采集功能的亚 40nm 空间分辨率、分子和声子振动光谱成像,光谱范围横跨整个中红外(700-5000cm(-1)),光谱分辨率为几厘米(-1)。我们在半导体、生物矿化和蛋白质纳米结构上展示了同步加速器红外纳米光谱学的性能,提供了具有亚zeptomole 灵敏度的振动化学成像。