Huang, Guan-JieGuan-JieHuangLi, Cheng-WeiCheng-WeiLiLee, Po-YiPo-YiLeeSu, Jia-XuanJia-XuanSuChao, Kuo-ChuanKuo-ChuanChaoLI-AN CHUChiang, Ann-ShynAnn-ShynChiangCheng, Ji-XinJi-XinChengChen, Bo-HanBo-HanChenLu, Chih-HsuanChih-HsuanLuChu, Shi-WeiShi-WeiChuYang, Shang-DaShang-DaYang2026-03-242026-03-242023https://www.scopus.com/inward/record.uri?eid=2-s2.0-85167787595&doi=10.1021%2Facs.jpcb.3c02629&partnerID=40&md5=5a58c302ab51559d69c321a91ed3539ehttps://scholars.lib.ntu.edu.tw/handle/123456789/736659Stimulated Raman scattering (SRS) spectromicroscopy is a powerful technique that enables label-free detection of chemical bonds with high specificity. However, the low Raman cross section due to typical far-electronic resonance excitation seriously restricts the sensitivity and undermines its application to bio-imaging. To address this bottleneck, the electronic preresonance (EPR) SRS technique has been developed to enhance the Raman signals by shifting the excitation frequency toward the molecular absorption. A fundamental weakness of the previous demonstration is the lack of dual-wavelength tunability, making EPR-SRS only applicable to a limited number of species in the proof-of-concept experiment. Here, we demonstrate the EPR-SRS spectromicroscopy using a multiple-plate continuum (MPC) light source able to examine a single vibration mode with independently adjustable pump and Stokes wavelengths. In our experiments, the C?�C vibration mode of Alexa 635 is interrogated by continuously scanning the pump-to-absorption frequency detuning throughout the entire EPR region enabled by MPC. The results exhibit 150-fold SRS signal enhancement and good agreement with the Albrecht A-term preresonance model. Signal enhancement is also observed in EPR-SRS images of the whole Drosophila brain stained with Alexa 635. With the improved sensitivity and potential to implement hyperspectral measurement, we envision that MPC-EPR-SRS spectromicroscopy can bring the Raman techniques closer to a routine in bio-imaging. © 2023 American Chemical Society.journal article10.1021/acs.jpcb.3c026292-s2.0-85167787595