• Advanced Photonics
  • Vol. 4, Issue 1, 016003 (2022)
Walker Peterson1, Julia Gala de Pablo1, Matthew Lindley1, Kotaro Hiramatsu1,2,3,*, and Keisuke Goda1,4,5,6
Author Affiliations
  • 1The University of Tokyo, School of Science, Department of Chemistry, Tokyo, Japan
  • 2The University of Tokyo, Research Center for Spectrochemistry, Tokyo, Japan
  • 3PRESTO, Japan Science and Technology Agency, Saitama, Japan
  • 4Japan Science and Technology Agency, Tokyo, Japan
  • 5University of California, Los Angeles, Department of Bioengineering, Los Angeles, California, United States
  • 6Wuhan University, Institute of Technological Sciences, Wuhan, China
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    DOI: 10.1117/1.AP.4.1.016003 Cite this Article Set citation alerts
    Walker Peterson, Julia Gala de Pablo, Matthew Lindley, Kotaro Hiramatsu, Keisuke Goda, "Ultrafast impulsive Raman spectroscopy across the terahertz–fingerprint region," Adv. Photon. 4, 016003 (2022) Copy Citation Text show less

    Abstract

    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.

    Video Introduction to the Article

    ESEISRS(ω,τ)=HLPF2(ω)[(12+β)2EPr(ω,τ)(12β)2ELO(ω)],

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    EFTCARS(ω,τ)=HSPF(ω)EPr(ω,τ),

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    E˜LPF1(t)=F1[HLPF1(ω)S(ω)],

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    E˜Pr(t,τ)=eiωc[n(t,τ)+n2|E˜LPF1(t)|2]zcE˜LPF1(t),

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    n(t,τ)=n0{1+kNAke(t+τ)γksin[ωk(t+τ)]},

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    IFTCARS(τ)=0|HSPF(ω)EPr(ω,τ)|2dω,

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    E˜CW(t,τ)=F1[HLPF2(ω)EPr(ω,τ)],

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    E˜CCW(t)=F1[F[eiωc[n0+n2|E˜LPF  1(t)|2]zceiδF1[HLPF  2(ω)HLPF  1(ω)S(ω)]]],

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    ISEISRS(τ)=0|F[(12+β)2E˜CW(t,τ)(12β)2E˜CCW(t)]|2dω,

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    Walker Peterson, Julia Gala de Pablo, Matthew Lindley, Kotaro Hiramatsu, Keisuke Goda, "Ultrafast impulsive Raman spectroscopy across the terahertz–fingerprint region," Adv. Photon. 4, 016003 (2022)
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