We present a three-dimensional theory of stimulated Raman scattering (SRS) or super-radiance. In particular we address how the spatial and temporal properties of the generated SRS beam or Stokes beam of radiation depends on the spatial properties of the gain medium. Maxwell equations for the Stokes field operators and of the atomic operators are solved analytically and a correlation function for the Stokes field is derived. In the analysis we identify a super-radiating part of the Stokes radiation that exhibit beam characteristics. We show how the intensity in this beam builds up in time and at some point largely dominates the total Stokes radiation of the gain medium. We show how the SRS depends on the Fresnel number and the optical depth and that in fact these two factors are the only factors describing the coherent radiation.
We present a three-dimensional theory of stimulated Raman scattering (SRS) or super-radiance. In particular we address how the spatial and temporal properties of the generated SRS beam or Stokes beam of radiation depends on the spatial properties of the gain medium. Maxwell equations for the Stokes field operators and of the atomic operators are solved analytically and a correlation function for the Stokes field is derived. In the analysis we identify a super-radiating part of the Stokes radiation that exhibit beam characteristics. We show how the intensity in this beam builds up in time and at some point largely dominates the total Stokes radiation of the gain medium. We show how the SRS depends on the Fresnel number and the optical depth and that in fact these two factors are the only factors describing the coherent radiation.
A theory of stimulated Raman scattering (SRS) is presented which treats in a unified manner the buildup of SRS from spontaneous Raman scattering and the spatial propagation which leads to gain. Maxwell-Bloch equations describe the coupling between the Stokes field operator and the collective atomic operators, which are driven by a classical laser field under low-signal-gain conditions, where the atomic ground states and laser field remain undepleted. An analytic expression is derived for the forward-propagating Stokes field operator in a one-dimensional spatial approximation when the Fresnel number of the excited medium is unity. Steady-state and transient Stokes intensities are evaluated under low-gain (spontaneous) and high-gain (stimulated) conditions. The Stokes intensity is found to be exactly independent of a laser bandwidth arising solely from phase fluctuations. The power spectrum of steady-state SRS is evaluated, giving a gain-narrowed spectral profile when the laser is narrow band, and a spectrum identical to the laser spectrum when the laser is broad band. A strong analogy between SRS and two-level superfluorescence is found; in both cases the macroscopic, collective dipole moment is initiated by quantum fluctuations.
A quantum theory of stimulated Raman scattering is presented that takes into account three-dimensional propagation and collisional dephasing, allowing the study of the spatial and temporal coherence properties of the generated Stokes light. Maxwell-Bloch equations for the Stokes field operator and the collective atomic operators are solved analytically under low-signal-gain conditions, where the laser field and the atomic ground states remain undepleted. The intensity and the space-time autocorrelation function of the Stokes field are calculated. The Stokes field is expanded into a set of statistically independent ``coherence modes,'' which are determined explicitly for the case of a cylindrically shaped pumped volume. The Stokes pulse energy W is found to fluctuate from pulse to pulse. The probability distribution function for pulse energies P(W) is calculated for a range of Fresnel numbers of the excited volume and collisional dephasing rates. For small values of Fresnel number and dephasing rate, P(W) is a negative exponential distribution. For large values of either, P(W) narrows and approaches a Gaussian-shaped distribution. This occurs because many independent modes contribute to the Stokes emission, making it spatially and/or temporally incoherent.
A three-dimensional quantum theory of stimulated Raman scattering is presented which takes into account a general transverse shape of the pump laser. The transverse spatial autocorrelation function and the intensity of the Stokes pulse are derived analytically, by use of the Maxwell-Bloch equations in low-signal-gain conditions and introduction of a many-spatial-modes approximation. We find that the spatial and temporal coherence are coupled. The transverse coherence depends on the pump-laser shape, and the coherence area increases with increasing gain. Time scales for the buildup of stimulated intensity and correlations for the various transverse parts of the Stokes pulse are obtained.
A pencil shaped region of a Raman-active medium forms a source for Stokes-shifted light via stimulated Raman Scattering (SRS) when driven by an intense laser pulse. Stokes photons are scattered spontaneously at first, and then amplified during propagation through the medium. Since the scattering is initiated by quantum noise, the actual number of photons produced in any given pulse will be highly uncertain, even if the pulse energy of the driving laser is constant1. As the Stokes light propagates through such an extended region, it's coherence properties will be changed. The spatial coherence is determined by the size and shape of the region, which may be characterized by its Fresnel number F, defined as F= A/λSL, where A is the cross-sectional area of the interaction region, which has length L, and λS is the Stokes wavelength. The rate at which the microscopic scatterers (atoms or molecules) are dephased by collisions affects the temporal coherence of the Stokes light, characterised by the temporal coherence parameter Γτ /gL, where Γ is the collisional dephasing rate, τ is the laser pulse duration and g is the steady-state Raman gain coefficient.
An experimental study of stimulated Raman scattering (SRS) has been performed using a subnanosecond pulse to investigate the statistical properties of Stokes light generation.1 There are macroscopic fluctuations of Stokes pulse energy as well as random generation of spatial mode patterns. When the scattering volume has a low Fresnel number, the spatial patterns of the SRS resemble cavity modes. When the Fresnel number is large, there are irregular structures appearing across the Stokes profile in a random fashion. A theoretical study of the spatial and temporal coherence properties of Raman generation using a Gaussian-profile pump pulse has also been carried out. Using a Gaussian-Laguerre mode expansion technique,2 it is found that the higher-order spatial coherence modes1 experience different gain than the lower-order spatial coherence modes, and consequently the temporal coherence associated with each individual spatial coherence mode is different.
Two-beam stimulated Raman scattering (SRS) has been used in diverse label-free spectroscopy and imaging applications of live cells, biological tissues, and functional materials. Recently, we developed a theoretical framework for the three-beam double SRS processes that involve pump, Stokes, and depletion beams, where the pump-Stokes and pump-depletion SRS processes compete with each other. It was shown that the net Stokes gain signal can be suppressed by increasing the depletion beam intensity. The theoretical prediction has been experimentally confirmed recently. In the previous scheme for a selective suppression of one SRS by making it compete with another SRS, the two SRS processes occur in a parallel manner. However, there is another possibility of three-beam double SRS scheme that can be of use to suppress either Raman gain of the Stokes beam or Raman loss of the pump beam by depleting the Stokes photons with yet another SRS process induced by the pair of Stokes and another (second) Stokes beam. This three-beam double SRS process resembles a cascading energy transfer process from the pump beam to the first Stokes beam (SRS-1) and subsequently from the first Stokes beam to the second Stokes beam (SRS-2). Here, the two stimulated Raman gain-loss processes are associated with two different Raman-active vibrational modes of solute molecule. In the present theory, both the radiation and the molecules are treated quantum mechanically. We then show that the cascading-type three-beam double SRS can be described by coupled differential equations for the photon numbers of the pump and Stokes beams. From the approximate solutions as well as exact numerical calculation results for the coupled differential equations, a possibility of efficiently suppressing the stimulated Raman loss of the pump beam by increasing the second Stokes beam intensity is shown and discussed. To further prove a potential use of this scheme for developing a super-resolution SRS microscopy, we present a theoretical expression and numerical simulation results for the full-width-at-half-maximum of SRS imaging point spread function, assuming that the pump and Stokes beam profiles are Gaussian and the second Stokes beam has a doughnut-shaped spatial profile. It is clear that the spatial resolution with the present 3-beam cascading SRS method can be enhanced well beyond the diffraction limit. We anticipate that the present work will provide a theoretical framework for a super-resolution stimulated Raman scattering microscopy that is currently under investigation.