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Time-Dependent Perturbation Theory

For a time-dependent perturbation V^(t)=V^eiωt\hat{V}(t) = \hat{V}\,e^{-i\omega t} applied to an initial state i|i\rangleThe transition rate to a continuum of final states f|f\rangle is:

Γif=2πfV^i2ρ(Ef)\Gamma_{i \to f} = \frac{2\pi}{\hbar}|\langle f|\hat{V}|i\rangle|^2\rho(E_f)

Where ρ(Ef)\rho(E_f) is the density of final states at energy Ef=Ei+ωE_f = E_i + \hbar\omega.

Derivation. Using first-order time-dependent perturbation theory, the transition amplitude to state f|f\rangle is:

cf(t)=i0tfV^ieiωfitdtc_f(t) = -\frac{i}{\hbar}\int_0^t \langle f|\hat{V}|i\rangle\,e^{i\omega_{fi}t'}\, dt'

For a sinusoidal perturbation at frequency ω\omega:

cf2=fV^i22sin2[(ωfiω)t/2](ωfiω)2/4|c_f|^2 = \frac{|\langle f|\hat{V}|i\rangle|^2}{\hbar^2}\frac{\sin^2[(\omega_{fi} - \omega)t/2]}{(\omega_{fi} - \omega)^2/4}

In the long-time limit, sin2(xt)/x22πtδ(x)\sin^2(xt)/x^2 \to 2\pi t\,\delta(x)Giving:

cf2t=2π2fV^i2δ(EfEiω)\frac{|c_f|^2}{t} = \frac{2\pi}{\hbar^2}|\langle f|\hat{V}|i\rangle|^2\,\delta(E_f - E_i - \hbar\omega)

Summing over all final states with density ρ(Ef)\rho(E_f):

Γ=dcf2dtρ(Ef)dEf=2πfV^i2ρ(Ef)\Gamma = \int \frac{d|c_f|^2}{dt}\,\rho(E_f)\,dE_f = \frac{2\pi}{\hbar}|\langle f|\hat{V}|i\rangle|^2\rho(E_f) \quad \blacksquare

11.2 Selection Rules for Electric Dipole Transitions

Section titled “11.2 Selection Rules for Electric Dipole Transitions”

The electric dipole matrix element:

fd^i=efri\langle f|\hat{\mathbf{d}}|i\rangle = -e\langle f|\mathbf{r}|i\rangle

For hydrogen-like atoms, the selection rules are:

  • Δl=±1\Delta l = \pm 1 (parity change required)
  • Δm=0,±1\Delta m = 0, \pm 1 (for zz, x±iyx \pm iy polarisation respectively)
  • Δn\Delta n unrestricted

The transition rate for 2p1s2p \to 1s in hydrogen:

A2p1s=ω33πε0c31ser2p2A_{2p \to 1s} = \frac{\omega^3}{3\pi\varepsilon_0\hbar c^3}|\langle 1s|e\mathbf{r}|2p\rangle|^2

With 1sz2p,m=0=27235a0|\langle 1s|z|2p, m=0\rangle| = \frac{2^7\sqrt{2}}{3^5}a_0This gives A2p1s6.3×108A_{2p \to 1s} \approx 6.3 \times 10^8 s1^{-1}Corresponding to a lifetime τ1.6\tau \approx 1.6 ns.

11.3 Spontaneous Emission and Einstein Coefficients

Section titled “11.3 Spontaneous Emission and Einstein Coefficients”

The Einstein AA coefficient (spontaneous emission rate) is related to the BB coefficient (stimulated emission/absorption):

A21=ω3π2c3B21A_{21} = \frac{\hbar\omega^3}{\pi^2 c^3}B_{21}

This relation, derived by Einstein in 1917 using thermodynamic arguments (detailed balance in a blackbody radiation field), was one of the first indications that spontaneous emission requires quantum electrodynamics.

Worked Example 11.1: Selection Rules for Hydrogen

Consider the transition 3d1s3d \to 1s in hydrogen. Is this an allowed E1 transition?

The matrix element involves the integral nlmrnlm=1,0,0rq3,2,m\langle n'l'm'|\mathbf{r}|nlm\rangle = \langle 1,0,0|r_q|3,2,m\rangle where rqr_q is a spherical tensor component.

By the Wigner—Eckart theorem and parity selection rules:

  • Δl=02=2±1\Delta l = 0 - 2 = -2 \neq \pm 1: forbidden for E1

The 3d1s3d \to 1s transition can proceed via:

  • E2 (electric quadrupole): Δl=0,±2\Delta l = 0, \pm 2Rate α(kR)2\sim \alpha(kR)^2 times slower than E1
  • M1 (magnetic dipole): requires Δl=0\Delta l = 0Not applicable here
  • Two-photon decay: 3d2p1s3d \to 2p \to 1s (two successive E1 transitions)

The 3d2p3d \to 2p transition (Δl=1\Delta l = -1) is E1-allowed and dominates, with A3d2p6.4×107A_{3d \to 2p} \sim 6.4 \times 10^7 s1^{-1}.

FormulaNameApplication
$\Gamma_{i\to f} = \frac{2\pi}{\hbar}\langle f\hat{V}
Δl=±1\Delta l = \pm 1, Δm=0,±1\Delta m = 0, \pm 1E1 selection rulesElectric dipole transitions
A21=ω3π2c3B21A_{21} = \frac{\hbar\omega^3}{\pi^2 c^3}B_{21}Einstein relationConnects spontaneous/stimulated rates
$c_f^2 = \frac{
  1. Fermi’s Golden Rule requires a continuum: For transitions between discrete states (e.g., two bound states in an atom), the Rabi formula must be used. The density of states ρ(Ef)\rho(E_f) in FGR ensures energy conservation is satisfied with finite probability.
  2. First-order perturbation fails for strong fields: When the Rabi frequency Ω=fV^i/\Omega = |\langle f|\hat{V}|i\rangle|/\hbar is comparable to the detuning, higher-order effects (AC Stark shift, Rabi oscillations) become important.
  3. Selection rules are not absolute: Forbidden transitions can proceed via higher multipole orders (E2, M1) or multiphoton processes, albeit at slower rates. A transition is truly forbidden only when all contributing channels vanish.
  4. The rotating wave approximation (RWA): Dropping counter-rotating terms requires ωωfiω+ωfi|\omega - \omega_{fi}| \ll \omega + \omega_{fi}. For very strong fields or ultrastrong coupling, the RWA breaks down.
  • Laser cooling: Doppler cooling relies on repeated absorption—spontaneous emission cycles, with each cycle reducing atomic momentum by k\hbar k.
  • Optical pumping: Polarised light selectively populates magnetic sublevels via dipole selection rules, preparing spin-polarised atomic samples.
  • Quantum optics: Spontaneous emission is the fundamental source of decoherence in quantum optical systems, limiting qubit lifetimes in cavity QED.
  • Spectroscopy: Fermi’s Golden Rule underlies the interpretation of absorption spectra, photoemission, and inelastic scattering cross sections.
  • Photovoltaics: The solar cell efficiency limit (Shockley—Queisser) derives from detailed balance between absorption and spontaneous emission.
  • Quantum electrodynamics: Spontaneous emission is not predicted by non-relativistic quantum mechanics alone — it requires coupling to the quantised electromagnetic field vacuum.
  • Scattering theory: The TT-matrix formalism generalises FGR to higher orders. The optical theorem (σtot=(4π/k)Imf(0)\sigma_{\text{tot}} = (4\pi/k)\,\text{Im}\,f(0)) relates the forward scattering amplitude to the total cross section.
  • Solid-state physics: Fermi’s Golden Rule describes electron—phonon scattering, carrier relaxation, and exciton decay in semiconductors.

Additional Worked Example: Photoionisation Rate

Section titled “Additional Worked Example: Photoionisation Rate”

Problem. A hydrogen atom in the ground state is illuminated by monochromatic light at λ=50\lambda = 50 nm, well above the ionisation threshold (13.6 eV). Estimate the photoionisation rate using Fermi’s Golden Rule.

Solution. The dipole matrix element for 1s1s \to continuum is approximately ϵper1sea0\langle \epsilon_p | e\mathbf{r} | 1s \rangle \sim ea_0. The density of continuum states at photoelectron energy ϵ=ω13.6\epsilon = \hbar\omega - 13.6 eV:

k=2mϵ/,ρ(ϵ)=Vmk(2π)32dΩk = \sqrt{2m\epsilon}/\hbar, \quad \rho(\epsilon) = \frac{V m k}{(2\pi)^3 \hbar^2} d\Omega

The photoionisation cross section near threshold is σ6.3×1018\sigma \approx 6.3 \times 10^{-18} cm2^2 for hydrogen. At intensity I=1012I = 10^{12} W/m2^2, the rate Γ=σI/(ω)1014\Gamma = \sigma I / (\hbar\omega) \approx 10^{14} s1^{-1} — complete ionisation occurs within femtoseconds for intense fields.

TransitionSelection RulesRateTypical Timescale
Electric dipole (E1)Δl=±1\Delta l = \pm 1, Δm=0,±1\Delta m = 0,\pm 1A107A \sim 10^710910^9 s1^{-1}ns
Magnetic dipole (M1)Δl=0\Delta l = 0, Δs=±1\Delta s = \pm 1 (spin-flip)A103A \sim 10^3 s1^{-1}μ\mus—ms
Electric quadrupole (E2)Δl=0,±2\Delta l = 0, \pm 2A103A \sim 10^{-3}1010 s1^{-1}ms—s
Two-photonNo parity constraintAI2A \propto I^2Depends on intensity
Forbidden (all channels)None allowedA=0A = 0Metastable if no decay path