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제121회 대한화학회 학술발표회, 총회 및 기기전시회 안내 Spectral modulation of stimulated Raman scattering signal: Beyond weak Raman pump limit

2018년 3월 7일 09시 03분 53초
PHYS.P-254 이곳을 클릭하시면 발표코드에 대한 설명을 보실 수 있습니다.
4월 20일 (금요일) 11:00~12:30
Physical Chemistry
저자 및
Hanju Rhee*, Sohee Lim1, Minhaeng Cho1,*
Seoul Center, Korea Basic Science Institute, Korea
1Department of Chemistry, Korea University / Center for Molecular Spectroscopy and Dynamics, Korea
Stimulated Raman scattering has recently been used in label-free vibrational imaging studies of live cells. Important attempts to develop super-resolution Raman imaging with intense Raman pump or decoherence beam have been made. However, the intense beams beyond weak stimulated Raman scattering limit could complicate spectral characteristics of Raman gain or loss signals. Here, the dependences of stimulated Raman loss (SRL) signal on Raman pump intensity and pump-probe delay time are specifically investigated through both experimental and simulation studies. In the strong pump regime, a pronounced spectral modulation in SRL is observed at the Raman peaks of aromatic compounds with relatively large optical Kerr nonlinearities. We perform a numerical simulation for the coupled wave propagation of the Raman pump and anti-Stokes probe pulses to investigate the effect of cross-phase modulation (XPM) on the stimulated Raman scattering (SRS). Our simulation involving both vibrationally resonant SRS and non-resonant XPM effects in part accounts for the pump-probe delay time-dependent peak shift and spectral broadening as well as the appearance of a gain signal at negative time delays. At the high pump intensity, it is found that the anti-symmetric XPM signal with respect to the time zero cannot be selectively eliminated to produce pure SRS signal by time-integration over the pump-probe delay time because of the increased interference term of the SRS and XPM at the Raman-active frequency region. We believe that the experimental and simulation results discussed here would be of use in developing a super-resolution coherent Raman imaging microscope in the near future.