Coherent Raman scattering microscopy can provide high-contrast tissue and single-cell images based on the inherent molecular vibrations of the sample.However,conventional techniques face a three-way trade-off between ...Coherent Raman scattering microscopy can provide high-contrast tissue and single-cell images based on the inherent molecular vibrations of the sample.However,conventional techniques face a three-way trade-off between Raman spectral bandwidth,imaging speed,and image fidelity.Although currently challenging to address via optical design,this trade-off can be overcome via emerging computational tools such as compressive sensing and machine learning.展开更多
Broadband Raman spectroscopy(detection bandwidth>1000 cm^(−1))is a valuable and widely used tool for understanding samples via label-free measurements of their molecular vibrations.Two important Raman spectral regi...Broadband Raman spectroscopy(detection bandwidth>1000 cm^(−1))is a valuable and widely used tool for understanding samples via label-free measurements of their molecular vibrations.Two important Raman spectral regions are the chemically specific“fingerprint”(200 to 1800 cm^(−1))and“low-frequency”or“terahertz”(THz)(<200 cm^(−1);<6 THz)regions,which mostly contain intramolecular and intermolecular vibrations,respectively.These two regions are highly complementary;broadband simultaneous measurement of both regions can provide a big picture comprising information about molecular structures and interactions.Although techniques for acquiring broadband Raman spectra covering both regions have been demonstrated,these methods tend to have spectral acquisition rates<10 spectra∕s,prohibiting high-speed applications,such as Raman imaging or vibrational detection of transient phenomena.Here,we demonstrate a single-laser method for ultrafast(24,000 spectra∕s)broadband Raman spectroscopy covering both THz and fingerprint regions.This is achieved by simultaneous detection of Sagnac-enhanced impulsive stimulated Raman scattering(SE-ISRS;THz-sensitive)and Fourier-transform coherent anti-Stokes Raman scattering(FT-CARS;fingerprint-sensitive).With dual-detection impulsive vibrational spectroscopy,the SE-ISRS signal shows a>500×enhancement of<6.5 THz sensitivity compared with that of FT-CARS,and the FT-CARS signal shows a>10×enhancement of fingerprint sensitivity above 1000 cm^(−1)compared with that of SE-ISRS.展开更多
文摘Coherent Raman scattering microscopy can provide high-contrast tissue and single-cell images based on the inherent molecular vibrations of the sample.However,conventional techniques face a three-way trade-off between Raman spectral bandwidth,imaging speed,and image fidelity.Although currently challenging to address via optical design,this trade-off can be overcome via emerging computational tools such as compressive sensing and machine learning.
基金supported by JST PRESTO (JPMJPR1878)JSPS Grant-in-Aid for Young Scientists (20K15227)+4 种基金Grant-in-Aid for JSPS Fellows (19F19805 and 21J15001)JSPS Core-to-Core ProgramWhite Rock FoundationNakatani FoundationOgasawara Foundation for the Promotion of Science and Engineering
文摘Broadband Raman spectroscopy(detection bandwidth>1000 cm^(−1))is a valuable and widely used tool for understanding samples via label-free measurements of their molecular vibrations.Two important Raman spectral regions are the chemically specific“fingerprint”(200 to 1800 cm^(−1))and“low-frequency”or“terahertz”(THz)(<200 cm^(−1);<6 THz)regions,which mostly contain intramolecular and intermolecular vibrations,respectively.These two regions are highly complementary;broadband simultaneous measurement of both regions can provide a big picture comprising information about molecular structures and interactions.Although techniques for acquiring broadband Raman spectra covering both regions have been demonstrated,these methods tend to have spectral acquisition rates<10 spectra∕s,prohibiting high-speed applications,such as Raman imaging or vibrational detection of transient phenomena.Here,we demonstrate a single-laser method for ultrafast(24,000 spectra∕s)broadband Raman spectroscopy covering both THz and fingerprint regions.This is achieved by simultaneous detection of Sagnac-enhanced impulsive stimulated Raman scattering(SE-ISRS;THz-sensitive)and Fourier-transform coherent anti-Stokes Raman scattering(FT-CARS;fingerprint-sensitive).With dual-detection impulsive vibrational spectroscopy,the SE-ISRS signal shows a>500×enhancement of<6.5 THz sensitivity compared with that of FT-CARS,and the FT-CARS signal shows a>10×enhancement of fingerprint sensitivity above 1000 cm^(−1)compared with that of SE-ISRS.
