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Register a new userOptimally shaped narrowband pulses for Femtosecond Stimulated Raman Spectroscopy in the range 330-750 nm
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Spectral compression of femtosecond pulses by second harmonic generation in the presence of substantial group velocity dispersion provides a convenient source of narrowband Raman pump pulses for femtosecond stimulated Raman spectroscopy (FSRS). We discuss here a simple and efficient modification that dramatically increases the versatility of the second harmonic spectral compression technique. Adding a spectral filter following second harmonic generation produces narrowband pulses with a superior temporal profile. This simple modification i) increases the Raman gain for a given pulse energy, ii) improves the spectral resolution, iii) suppresses coherent oscillations associated with slowly dephasing vibrations, and iv) extends the useful tunable range to at least 330-750 nm.
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Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is generally restricted to ground state properties. Working in resonance conditions, indeed, enables cross-section enhancement and selective excitation to a targeted electronic level, but is hampered by an increased signal complexity due to the presence of overlapping spectral contributions. Here, we show how detailed information on ground and excited state vibrations can be disentangled, by exploiting the relative time delay between Raman and probe pulses to control the excited state population, combined with a diagrammatic formalism to dissect the pathways concurring to the signal generation. The proposed method is then exploited to elucidate the vibrational properties of ground and excited electronic states in the paradigmatic case of Cresyl Violet. We anticipate that the presented approach holds the potential for selective mapping the reaction coordinates pertaining to transient electronic stages implied in photo-active compounds.
Stimulated Raman spectroscopy has become a powerful tool to study the spatiodynamics of molecular bonds with high sensitivity, resolution and speed. However, sensitivity and speed of state-of-the-art stimulated Raman spectroscopy are currently limited by the shot-noise of the light beam probing the Raman process. Here, we demonstrate an enhancement of the sensitivity of continuous-wave stimulated Raman spectroscopy by reducing the quantum noise of the probing light below the shot-noise limit by means of amplitude squeezed states of light. Probing polymer samples with Raman shifts around 2950 $cm^{-1}$ with squeezed states, we demonstrate a quantum-enhancement of the stimulated Raman signal-to-noise ratio (SNR) of 3.60 dB relative to the shot-noise limited SNR. Our proof-of-concept demonstration of quantum-enhanced Raman spectroscopy paves the way for a new generation of Raman microscopes, where weak Raman transitions can be imaged without the use of markers or an increase in the total optical power.
We propose and theoretically analyze a new vibrational spectroscopy, termed electron- and light-induced stimulated Raman (ELISR) scattering, that combines the high spatial resolution of electron microscopy with the molecular sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but spatially-confined Stokes beam in the presence of a diffraction-limited pump laser. To characterize this technique, we develop a numerical model and conduct full-field electromagnetic simulations to investigate two distinct nanoparticle geometries, nanorods and nanospheres, coated with a Raman-active material. Our results show the significant ($10^6$-$10^7$) stimulated Raman enhancement that is achieved with dual electron and optical excitation of these nanoparticle geometries. Importantly, the spatial resolution of this vibrational spectroscopy for electron microscopy is solely determined by the nanoparticle geometry and the plasmon mode volume. Our results highlight the promise of ELISR for simultaneous high-resolution electron microscopy with sub-diffraction-limited Raman spectroscopy, complementing advances in superresolution microscopy, correlated light and electron microscopy, and vibrational electron energy loss spectroscopy.
The theory of stimulated Raman adiabatic passage in a three-level Lambda-scheme of the interaction of an atom or molecule with light, which takes the nonadiabatic processes at the beginning and the end of light pulses into account, is developed.
The success of non-linear optics relies largely on pulse-to-pulse consistency. In contrast, covariance based techniques used in photoionization electron spectroscopy and mass spectrometry have shown that wealth of information can be extracted from noise that is lost when averaging multiple measurements. Here, we apply covariance based detection to nonlinear optical spectroscopy, and show that noise in a femtosecond laser is not necessarily a liability to be mitigated, but can act as a unique and powerful asset. As a proof of principle we apply this approach to the process of stimulated Raman scattering in alpha-quartz. Our results demonstrate how nonlinear processes in the sample can encode correlations between the spectral components of ultrashort pulses with uncorrelated stochastic fluctuations. This in turn provides richer information compared to the standard non-linear optics techniques that are based on averages over many repetitions with well-behaved laser pulses. These proof-of-principle results suggest that covariance based nonlinear spectroscopy will improve the applicability of fs non-linear spectroscopy in wavelength ranges where stable, transform limited pulses are not available such as, for example, x-ray free electron lasers which naturally have spectrally noisy pulses ideally suited for this approach.
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