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Register a new userTemperature dependent anti-Stokes/Stokes ratios under Surface Enhanced Raman Scattering (SERS) conditions
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We make systematic measurements of Raman anti-Stokes/Stokes (aS/S) ratios using two different laser excitations (514 and 633 nm) of rhodamine 6G (RH6G) on dried Ag colloids over a wide range of temperatures (100 to 350 K). We show that a temperature scan allows the separation of the contributions to the aS/S ratios from {it resonance effects} and {it heating/pumping}, thus decoupling the two main aspects of the problem. The temperature rise is found to be larger when employing the 633 nm laser. In addition, we find evidence for mode specific vibrational pumping at higher laser power densities. We analyze our results in the framework of ongoing discussion on laser heating/pumping under SERS conditions.
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Surface Enhanced Raman Scattering (SERS) and Surface-Enhanced Fluorescence (SEF) are studied within the framework of modified Spontaneous Emission (SE), and similarities and differences are highlighted. This description sheds new light into several aspects of the SERS electromagnetic enhancement. In addition, combined with the optical reciprocity theorem it also provides a rigorous justification of a generalized version of the widely used SERS enhancement factor proportional to the fourth power of the field ($|E|^4$). We show, in addition, that this approach also applies to the calculation of Surface-Enhanced Fluorescence cross-sections thus presenting both phenomena SERS and SEF within a unified framework.
We present an in-depth analysis of the experimental estimation of cross sections in Surface Enhanced Raman Scattering (SERS) by vibrational pumping. The paper highlights the advantages and disadvantages of the technique, pinpoints the main aspects and limitations, and provides the underlying physical concepts to interpret the experimental results. Examples for several commonly used SERS probes are given, and a discussion on future possible developments is also presented.
The production of correlated Stokes (S) and anti-Stokes (aS) photons (SaS process) mediated by real or virtual phonon exchange has been reported in many transparent materials. In this work, we investigate the polarization and time correlations of SaS photon pairs produced in a diamond sample. We demonstrate that both S and aS photons have mainly the same polarization of the excitation laser. We also perform a pump-and-probe experiment to measure the decay rate of the SaS pair production, evidencing the fundamental diference between the real and virtual (phonon exchange) processes. In real processes, the rate of SaS pair production is governed by the phonon lifetime of $(2.8 pm 0.3)$ ps, while virtual processes only take place within the time width of the pump laser pulses of approximately 0.2 ps. We explain the diference between real and virtual SaS processes by a phenomenological model, based on probabilities of phonon creation and decay.
Since its first demonstration in the sixties, coherent anti-Stokes Raman scattering (CARS) has become a powerful spectroscopic sensing tool with broad applications in biology and chemistry. However, it is a complex nonlinear optical process that often leads to the lacks of quantitative data outputs. In this letter, we observe how CARS signal builds up gradually and demonstrate how to control its deferral with laser-pulse shaping. A time-resolved three-color CARS that involves a pair of driving broadband femtosecond pulses and delayed shaped probe pulse is realized experimentally. Driving pulses are tuned to the Raman-resonance onto the vibrational ring modes of pyridine and benzene molecules. As a result, CARS-buildup is deferred in picoseconds as delayed probe pulse width varies from 50 down to 10 cm-1. With off-resonant driving of water molecules this effect, in contrary, does not occur. Laser control predicting deferred resonant processes can serve as a novel and important species-specific indicator in, e.g., machine learning applications for future nonlinear optical spectroscopy.
The anti-Stokes scattering and Stokes scattering in stimulated Brillouin scattering (SBS) cascade have been researched by the Vlasov-Maxwell simulation. In the high-intensity laser-plasmas interaction, the stimulated anti-Stokes Brillouin scattering (SABS) will occur after the second stage SBS rescattering. The mechanism of SABS has been put forward to explain this phenomenon. And the SABS will compete with the SBS rescattering to determine the total SBS reflectivity. Thus, the SBS rescattering including the SABS is an important saturation mechanism of SBS, and should be taken into account in the high-intensity laser-plasmas interaction.
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