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First demonstrated in 1994, femtosecond stimulated Raman scattering (FSRS) has gained popularity since the early 2000s as an ultrafast pump–probe vibrational spectroscopy technique with the potential to circumvent the time and energy limitations imposed by the Heisenberg uncertainty principle. This Primer explores whether, why, when and how the temporal precision and frequency resolution of traditional time-resolved spontaneous Raman spectroscopy can be surpassed by its coherent counterpart (FSRS), while still adhering to the uncertainty principle. We delve into the fundamental concepts behind FSRS and its most common experimental implementations, focusing on instrumentation details, measurement techniques, data analysis and modelling. This includes discussions on synthesizing the Raman pump beam, artificial intelligence (AI)-assisted baseline removal methods and analytical expressions for reproducing experimental data and extracting key parameters such as relaxation times and out-of-equilibrium temperature profiles. Recent applications of FSRS from physics, chemistry and biology are showcased, demonstrating how this approach has facilitated cross-disciplinary studies. We also address the technical and conceptual limitations of FSRS to aid in designing optimal experiments based on specific goals. Finally, we explore future directions, including multidimensional extensions to address vibrational couplings and the use of quantum light to untangle temporal and spectral resolution.

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A nonlinear optical effect that occurs when the refractive index of a material changes, typically in a quadratic manner, in response to an applied electric field. Such a modification can affect the propagation of pulses and their spectral profiles.

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The energy difference with respect to the laser energy expressed in wavenumbers, evaluated as \(\Delta \widetilde{{\rm{\nu }}}\) (in units of cm–1) = 107 × (\({\lambda }_{{\rm{L}}}^{-1}\) – λ−1) (where wavelength is in units of nm).

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Kuramochi, H., Takeuchi, S. & Tahara, T. Ultrafast structural evolution of photoactive yellow protein chromophore revealed by ultraviolet resonance femtosecond stimulated Raman spectroscopy. J. Phys. Chem. Lett. 3, 2025–2029 (2012).

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Bera, K., Douglas, C. J. & Frontiera, R. R. Femtosecond stimulated Raman spectroscopy-guided library mining leads to efficient singlet fission in rubrene derivatives. Chem. Sci. 12, 13825–13835 (2021).

Fang, C., Frontiera, R. R., Tran, R. & Mathies, R. A. Mapping GFP structure evolution during proton transfer with femtosecond Raman spectroscopy. Nature 462, 200–204 (2009). To our knowledge, this article presents the first FSRS application to track nuclear motion underlying proton transfer.

Apr 10, 2011 — The Nyquist limit applies because each photo site is a sample of the incident wave form. The Nyquist Limit says that we can only reproduce a ...

Zhu, L., Liu, W. & Fang, C. A versatile femtosecond stimulated Raman spectroscopy setup with tunable pulses in the visible to near infrared. Appl. Phys. Lett. 105, 041106 (2014).

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Fingerhut, B. P., Dorfman, K. E. & Mukamel, S. Probing the conical intersection dynamics of the RNA base uracil by UV-pump stimulated-Raman-probe signals; ab initio simulations. J. Chem. Theory Comput. 10, 1172–1188 (2014).

Kukura, P., McCamant, D. W., Davis, P. H. & Mathies, R. A. Vibrational structure of the S2 (1Bu) excited state of diphenyloctatetraene observed by femtosecond stimulated Raman spectroscopy. Chem. Phys. Lett. 382, 81–86 (2003).

Aluminum has a high reflectance over the entire visible and near infrared spectrum. It is simple to deposit as a thin film, making it the ideal choice for most non-critical applications. The aluminum is over coated with a single layer of MgF2 to make it considerably more durable than bare aluminum.

Liu, W. et al. Tracking ultrafast vibrational cooling during excited-state proton transfer reaction with anti-Stokes and Stokes femtosecond stimulated Raman spectroscopy. J. Phys. Chem. Lett. 8, 997–1003 (2017).

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Yoon, S., Kukura, P., Stuart, C. M. & Mathies, R. A. Direct observation of the ultrafast intersystem crossing in tris(2,2′-bipyridine)ruthenium(II) using femtosecond stimulated Raman spectroscopy. Mol. Phys. 104, 1275–1282 (2006).

Wang, Z., Jiang, J., Huang, Y. & Liu, W. Tracking twisted intramolecular charge transfer and isomerization dynamics in 9-(2,2-dicyanovinyl) julolidine using femtosecond stimulated Raman spectroscopy. Chin. J. Chem. Phys. 36, 397–403 (2023).

Pontecorvo, E., Ferrante, C., Elles, C. G. & Scopigno, T. Spectrally tailored narrowband pulses for femtosecond stimulated Raman spectroscopy in the range 330–750 nm. Opt. Express 21, 6866–6872 (2013).

Oscar, B. G., Chen, C., Liu, W., Zhu, L. & Fang, C. Dynamic Raman line shapes on an evolving excited-state landscape: insights from tunable femtosecond stimulated Raman spectroscopy. J. Phys. Chem. A 121, 5428–5441 (2017).

Batignani, G. et al. Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet. Nat. Photon. 9, 506–510 (2015). This article presents the measurement of sub-100-fs dynamics in a solid-state sample with high-resolution FSRS.

Kuramochi, H., Takeuchi, S., Kamikubo, H., Kataoka, M. & Tahara, T. Skeletal structure of the chromophore of photoactive yellow protein in the excited state investigated by ultraviolet femtosecond stimulated Raman spectroscopy. J. Phys. Chem. B 125, 6154–6161 (2021).

Shanghai Optics is a custom optics manufacturer with over 60 years of optics manufacturing experience. We produce high precision Metalized Mirrors according to customers’ specifications.

Kuramochi, H., Takeuchi, S. & Tahara, T. Femtosecond time-resolved impulsive stimulated Raman spectroscopy using sub-7-fs pulses: apparatus and applications. Rev. Sci. Instrum. 87, 43107 (2016).

Dorfman, K. E., Schlawin, F. & Mukamel, S. Stimulated Raman spectroscopy with entangled light: enhanced resolution and pathway selection. J. Phys. Chem. Lett. 5, 2843–2849 (2014).

Divergence describes the expansion of a laser beam over a long distance. The value is given in mrad (milliradiant), a unit to specify angles. What is better, a ...

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Femtosecond spectroscopyNobel Prize

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Ferrante, C. et al. Ultrafast dynamics and vibrational relaxation in six-coordinate heme proteins revealed by femtosecond stimulated Raman spectroscopy. J. Am. Chem. Soc. 142, 2285–2292 (2020).

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Kayal, S., Roy, K. & Umapathy, S. Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: ultrafast transient absorption and ultrafast Raman loss spectroscopic studies. J. Chem. Phys. 148, 024301 (2018).

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The authors are grateful to G. Cerullo, P. Kukura, S. Mukamel and M. H. Vos for several inspiring discussions. They acknowledge early contributions by E. Pontecorvo to the planning and development of their first FSRS prototype. G.B. acknowledges funding from the PRIN 2022 Project (Dynamat) (grant number 2022PR7CCY).

Hall, C. R. et al. Femtosecond stimulated Raman study of the photoactive flavoprotein AppABLUF. Chem. Phys. Lett. 683, 365–369 (2017).

Han, X. X., Rodriguez, R. S., Haynes, C. L., Ozaki, Y. & Zhao, B. Surface-enhanced Raman spectroscopy. Nat. Rev. Methods Primers 1, 87 (2022).

Introduction (T.S., G.B., C.F., G.F. and M.M.); Experimentation (T.S., G.B., C.F., G.F. and M.M.); Results (T.S., G.B., C.F., G.F. and M.M.); Applications (T.S., G.B., C.F., G.F. and M.M.); Reproducibility and data deposition (T.S., G.B., C.F., G.F. and M.M.); Limitations and optimizations (T.S., G.B., C.F., G.F. and M.M.); Outlook (T.S., G.B., C.F., G.F. and M.M.); overview of the Primer (T.S.).

Han, F., Liu, W. & Fang, C. Excited-state proton transfer of photoexcited pyranine in water observed by femtosecond stimulated Raman spectroscopy. Chem. Phys. 422, 204–219 (2013).

Audier, X., Heuke, S., Volz, P., Rimke, I. & Rigneault, H. Noise in stimulated Raman scattering measurement: from basics to practice. APL Photon. 5, 011101 (2020).

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Kloz, M., Weißenborn, J., Polívka, T., Frank, H. A. & Kennis, J. T. M. Spectral watermarking in femtosecond stimulated Raman spectroscopy: resolving the nature of the carotenoid S* state. Phys. Chem. Chem. Phys. 18, 14619–14628 (2016).

by DRHW GAUSMAN · Cited by 369 — 1 cally some research about the reflectance tance compared with normal, uninfiltrated of near-infrared light from plant leaves and leaves, represented by ...

Diaz, S. A. & McCamant, D. W. Diffuse reflectance-based femtosecond stimulated Raman spectroscopy of opaque suspensions. Anal. Chem. 95, 15856–15860 (2023).

Laimgruber, S., Schachenmayr, H., Schmidt, B., Zinth, W. & Gilch, P. A femtosecond stimulated Raman spectrograph for the near ultraviolet. Appl. Phys. B 85, 557–564 (2006). To our knowledge, this article is the first demonstration of FSRS with a fixed-wavelength ultraviolet Raman pump.

Roy, P., Al-Kahtani, F., Cammidge, A. N. & Meech, S. R. Solvent tuning excited state structural dynamics in a novel bianthryl. J. Phys. Chem. Lett. 14, 253–259 (2023).

Batignani, G., Fumero, G., Mukamel, S. & Scopigno, T. Energy flow between spectral components in 2D broadband stimulated Raman spectroscopy. Phys. Chem. Chem. Phys. 17, 10454–10461 (2015).

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Polli, D., Kumar, V., Valensise, C. M., Marangoni, M. & Cerullo, G. Broadband coherent Raman scattering microscopy. Laser Photon Rev. 12, 1800020 (2018).

Liu, W., Han, F., Smith, C. & Fang, C. Ultrafast conformational dynamics of pyranine during excited state proton transfer in aqueous solution revealed by femtosecond stimulated Raman spectroscopy. J. Phys. Chem. B 116, 10535–10550 (2012).

Sun, Z., Lu, J., Zhang, D. H. & Lee, S.-Y. Quantum theory of (femtosecond) time-resolved stimulated Raman scattering. J. Chem. Phys. 128, 144114 (2008).

Sandoval, J. S. & McCamant, D. W. The best models of Bodipy’s electronic excited state: comparing predictions from various DFT functionals with measurements from femtosecond stimulated Raman spectroscopy. J. Phys. Chem. A 127, 8238–8251 (2023).

Chen, C. et al. Structural characterization of fluorescent proteins using tunable femtosecond stimulated Raman spectroscopy. Int. J. Mol. Sci. 24, 11991 (2023).

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Monacelli, L. et al. Manipulating impulsive stimulated Raman spectroscopy with a chirped probe pulse. J. Phys. Chem. Lett. 8, 966–974 (2017).

Zong, C. & Cheng, J. X. Origin of dispersive line shapes in plasmon-enhanced stimulated Raman scattering microscopy. Nanophotonics 10, 617–625 (2020).

Roy, P. et al. Ultrafast bridge planarization in donor-π-acceptor copolymers drives intramolecular charge transfer. Nat. Commun. 8, 1716 (2017).

Ashner, M. N. & Tisdale, W. A. High repetition-rate femtosecond stimulated Raman spectroscopy with fast acquisition. Opt. Express 26, 18331 (2018).

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Shenje, L., Qu, Y., Popik, V. & Ullrich, S. Femtosecond photodecarbonylation of photo-ODIBO studied by stimulated Raman spectroscopy and density functional theory. Phys. Chem. Chem. Phys. 23, 25637–25648 (2021).