http://arxiv.org/pdf/1012.2139v1

*Coupled-Mode Theory of Field Enhancement in Complex Metal Nanostructures*

Referenced is a simplified sphere based math model of the cascade dipole
amplifier.




On Mon, May 13, 2013 at 10:09 PM, Axil Axil <[email protected]> wrote:

> This post describes the mechanism that produces large power concentrations
> in a multi-nanoparticle system where the particles vary widely in particle
> sizes.
>
> First, let’s set the table.
>
> A cascade amplifier is any diode constructed from a series of amplifiers,
> where each amplifier sends its output to the input of the next amplifier in
> a daisy chain.
>
> Coherent anti-Stokes Raman scattering acts like such a cascade amplifier,
> except that dipoles tuned to various resonant frequencies drive thermal
> power to higher power concentration levels zero loss factors.
>
> In detail, coherent anti-Stokes Raman scattering, also called Coherent
> anti-Stokes Raman scattering spectroscopy (CARS), is a form of spectroscopy
> used primarily in chemistry, physics and related fields.
>
> It is sensitive to the same vibrational signatures of dipoles as seen in
> Raman spectroscopy. Unlike Raman spectroscopy, CARS employs multiple photo
> harmonics.
>
> It produces a signal in which the emitted waves are coherent with one
> another. As a result, CARS is orders of magnitude stronger than spontaneous
> Raman emission.
>
> CARS is a N-order nonlinear optical process involving multiple coupled
> dipole sources.
>
> These dipoles interact and generate a coherent optical signal at the
> anti-Stokes frequency. The high order harmonic is resonantly enhanced when
> the frequency difference between the low order pumps and the dipoles
> coincides with the frequency of a Raman resonance, which is the basis of
> the technique's intrinsic vibrational contrast mechanism.
>
> Multiple nanoparticles of various sizes interact each with their
> respective dipole resonant frequencies.
>
> The CARS process can be physically explained by using either a classical
> oscillator model or by using a quantum mechanical model.
>
> Classically, the Raman active vibrator is modeled as a (damped) harmonic
> oscillator with a characteristic frequency. In CARS, these oscillators are
> not driven by a single optical wave, but by the different resonant
> frequencies between the dipole pumps and the high order harmonic.
>
> This driving mechanism is similar to hearing the low combination beat tone
> when striking two different high tone piano keys: your ear is sensitive to
> the difference frequency of the high tones. Similarly, the Raman oscillator
> is susceptible to the difference frequency of multiple optical waves. When
> the difference frequency approaches beat resonance, the system of dipole
> oscillators are driven very efficiently.
>
>  While intuitive, this classical picture does not take into account the
> quantum mechanical energy levels of the dipole. Quantum mechanically, the
> CARS process can be understood as follows. Our dipole is initially in the
> ground state, the lowest thermal energy state of the system. The pump
> dipole excites the dipole chain to a virtual vibrational state.
>
> A virtual state is not an eigenstate of the dipole and it cannot be
> occupied but it does allow for transitions between otherwise uncoupled real
> states. If a dipole is simultaneously present along with the pumps, the
> virtual state can be used as an instantaneous gateway to address a
> vibrational eigenstate of the dipole.
>
> The joint action of the pumps and the Stokes has effectively established a
> coupling between the ground state and the vibrationally excited state of
> the system.
>
> The system is now in multiple states at the same time: it resides in a
> coherent superposition of states.
>
> This promotes the system to a virtual state. Again, the molecule cannot
> stay in the virtual state and will fall back instantaneously to the ground
> state under the emission of a photon at the anti-Stokes frequency. The pump
> dipoles are no longer in a superposition, as it resides again in the lowest
> thermal state, the ground state.
>
> In the quantum mechanical model, energy is deposited in the dark mode
> highest resonant system during the CARS process. The molecule acts like a
> medium for converting the frequencies of the multiple resonant waves into a
> CARS signal (a parametric process). There are, however, related coherent
> Raman processes that occur simultaneously which do deposit energy into the
> high order resonant cavity at high efficiency.
>
> The maximum sustained energy level achieved in this smallest resonant
> cavity in the cavity chain is determined when losses from the cavity equals
> input energy levels.
>
>
>
>

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