• 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[J]. Advanced Photonics, 2022, 4(1): 016003 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[J]. Advanced Photonics, 2022, 4(1): 016003
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