Spectral Line Shape Broadening Mechanisms

Problem: What does the phrase “spectral line shape” mean?

Solution: A spectrum is typically a plot of the intensity \(I(\omega)\sim|E(\omega)|^2\) of some underlying time domain signal \(E(t)\).

Problem: What are the \(2\) most prominent kinds of spectra one encounters?

Solution: There are both emission spectra and absorption spectra (and also, it seems there are only broadening mechanisms, no such thing as narrowing mechanisms).

Problem: Distinguish between homogeneous broadening mechanisms and inhomogeneous broadening mechanisms.

Solution: Homogeneous broadening mechanisms affect all atoms indistinguishably, giving rise to a Lorentzian spectral line shape. By contrast, inhomogeneous broadening mechanisms affect atoms distinguishably; this leads to non-Lorentzian spectral broadening.

Problem: In the presence of Doppler broadening alone, what is the spectral line shape?

Solution: Along \(1\)-dimension, the Maxwell-Boltzmann distribution of velocities is normally distributed (no factor of \(4\pi v^2\)):

\[\rho(v)=\sqrt{\frac{\beta m}{2\pi}}e^{-\beta mv^2/2}\]

The non-relativistic Doppler shift gives the angular frequency random variable \(\omega\) as an affine transformation of the velocity random variable \(v\):

\[\omega=\omega_0+k_0v\]

so:

\[\rho(\omega)=\frac{dv}{d\omega}\rho(v)=\sqrt{\frac{\beta m}{2\pi k_0^2}}e^{-\beta m(\omega-\omega_0)^2/2k_0^2}\]

In particular it is also a Gaussian (hence Doppler broadening is inhomogeneous) but with expectation \(\omega_0\) and standard deviation (aka line width) \(\Delta\omega\):

\[\Delta\omega=\omega_0\sqrt{\frac{k_BT}{mc^2}}\propto\sqrt{T}\]

(slogan: variance proportional to temperature) so the quality factor \(Q:=\omega_0/\Delta\omega_D\) of depends on the ratio of rest mass energy \(mc^2\) of each particle to their thermal energy \(k_BT\).

Problem: In the presence of natural/lifetime/radiative broadening alone, what is the spectral line shape?

Solution: For a \(2\)-level system with ground state \(|0\rangle\) and excited state \(|1\rangle\) associated to a lifetime \(\tau\) of spontaneous emission, then the natural line width is:

\[\Gamma\sim\omega\sim\frac{1}{\tau}\]

and the spectral line shape is a Lorentzian \(\sim\frac{1}{(\omega-\omega_0)^2+\Gamma^2}\) (is there a clear way to understand why? From optical Bloch equations for instance…). So natural broadening is a homogeneous broadening mechanism.

Problem: In the presence of pressure/collisional broadening alone, what is the spectral line shape?

Solution: Also a Lorentzian as with natural broadening (so also homogeneous), but the line width is determined from the relaxation time \(\tau=\ell/\langle v_{\text{rel}}\rangle\) between collisions. Using the fact that the mean free path is \(\ell=1/n\sigma\), this yields the line width due to pressure broadening:

\[\Delta\omega=n\sigma\langle v\rangle\]

Problem: What does the overall spectral line shape look like when multiple broadening mechanisms are at play?

Solution:

sum of independent random variables yields convolution.

Power Broadening

This is also homogeneous.

Doppler Broadening

Need to use that formula for converting a probability distribution of one random variable into another function of it with the derivative…(this is how you can experimentally verify the Maxwell distribution btw).

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