title: Quantitative chemical imaging with background-free multiplex coherent anti-Stokes Raman scattering by dual-soliton Stokes pulses.
abstract: Coherent anti-Stokes Raman microscopy (CARS) is a quantitative, chemically specific, and label-free optical imaging technique for studying inhomogeneous systems. However, the complicating influence of the nonresonant response on the CARS signal severely limits its sensitivity and specificity and especially limits the extent to which CARS microscopy has been used as a fully quantitative imaging technique. On the basis of spectral focusing mechanism, we establish a dual-soliton Stokes based CARS microspectroscopy and microscopy scheme capable of quantifying the spatial information of densities and chemical composition within inhomogeneous samples, using a single fiber laser. Dual-soliton Stokes scheme not only removes the nonresonant background but also allows robust acquisition of multiple characteristic vibrational frequencies. This all-fiber based laser source can cover the entire fingerprint (800-2200 cm-1) region with a spectral resolution of 15 cm-1. We demonstrate that quantitative degree determination of lipid-chain unsaturation in the fatty acids mixture can be achieved by the characterization of C = C stretching and CH2deformation vibrations. For microscopy purposes, we show that the spatially inhomogeneous distribution of lipid droplets can be further quantitatively visualized using this quantified degree of lipid unsaturation in the acyl chain for contrast in the hyperspectral CARS images. The combination of compact excitation source and background-free capability to facilitate extraction of quantitative composition information with multiplex spectral peaks will enable wider applications of quantitative chemical imaging in studying biological and material systems.
authors.affiliation: Key Lab of Precision Measurement Technology & Instrument, Department of Precision Instrument, Tsinghua University, Beijing 100084, China.
authors.forename: Kun
authors.initials: K
authors.lastname: Chen
authors.affiliation: Key Lab of Precision Measurement Technology & Instrument, Department of Precision Instrument, Tsinghua University, Beijing 100084, China.
authors.forename: Tao
authors.initials: T
authors.lastname: Wu
authors.affiliation: Key Lab of Precision Measurement Technology & Instrument, Department of Precision Instrument, Tsinghua University, Beijing 100084, China; luckiwei@mail.tsinghua.edu.cn.
authors.forename: Haoyun
authors.initials: H
authors.lastname: Wei
authors.affiliation: Key Lab of Precision Measurement Technology & Instrument, Department of Precision Instrument, Tsinghua University, Beijing 100084, China.
authors.forename: Tian
authors.initials: T
authors.lastname: Zhou
authors.affiliation: Key Lab of Precision Measurement Technology & Instrument, Department of Precision Instrument, Tsinghua University, Beijing 100084, China.
authors.forename: Yan
authors.initials: Y
authors.lastname: Li
keywords: (180.4315) Nonlinear microscopy; (180.5655) Raman microscopy; (300.6230) Spectroscopy, coherent anti-Stokes Raman scattering