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You are on page 1of 10

BEFORE AFTER

hν (No more photon)

Molecule in Molecule in

ground state excited state

This quantum mechanical picture may satisfy conservation of energy (when you

quantize light and molecular energies), but it has lots of problems and doesn’t tell

you much.

(2) Matter: Treat as a harmonic oscillator

(3) Interactions: Oscillating external force field driving harmonic oscillator

1) Light

( ) () (

E r, t = εˆ r E o cos ωt − k ⋅ r − φ )

Polarization vector Wavevector defines

direction of propagation

Amplitude

2π ω

Frequency (rad/sec) k = =

λ c

c = 2.998 × 108 m / s

To simplify:

(1) Propagate along x̂ ; (2) φ = 0 (for the time being we will drop the polarization)

E ( x, t ) = E o cos ( ωt − kx )

2π

λ= oscillations in space

k

E

E0

x

propagating at c

2π 1

time : = oscillations in time

ω ν

Now, we will drop wave vector ( k → 0 , since λ>>x and we consider molecules at x=0)

c

E ( t ) = E o cos ωt

2

I= Eo

4π

(2) Molecules

Why should we be able to call molecules harmonic oscillators? i.e., a mass on a spring?

The covalent bond can be thought of as a spring.

push/pull on this bond, there is a restoring force that pushes the system back to

equilibrium.

distribution. (for instance, benzene pi orbitals)

spins—align with field.

anharmonic curves that

reflect attractive and

repulsive forces.

• A finite amount of energy

pulls the molecule apart.

1 ∂ 2 V

V(q ) = (q − q 0 )2

2 ∂q

2

1 2

= kQ

2

q0 q

Q=0

(Set Q = q − q0)

k is force constant

∂V

Linear restoring force: Fres = − = − kQ

∂Q

∂ 2Q

Equation of Motion from Newton F = ma m

∂t 2

∂ 2Q

m 2 = Fres + Fdamp + Fext driving force

∂t

∂Q

= − kQ − b + Fext

∂t

∂ 2Q b ∂Q kQ Fext

+ + =

∂t 2 m ∂t m m

with light field

Fext (t ) = Fo cos ωt

Solutions:

∂ 2Q

m 2 + kQ = 0

∂t

Solution:

Q ( t ) = A sin ( ωo t ) + B cos ( ωo t )

drop for now

k

resonance frequency: ωo =

m

Oscillations at ω0 continue forever.

Q

A

2π

ω0

b) Now we add damping—H.O. may feel friction that reduces the amplitude of

oscillation

∂ 2Q ∂Q

m 2 = Fres + Fdamp = − kQ − b

∂t ∂t

∂ 2Q b ∂Q kQ

+ + =0

∂t 2

m ∂t m

2

γ = b / 2m Ω o = ωo − γ 2 ≈ ωo

frequency damping

A e − γt

2π

Ω0

5.33 Lecture Notes: A Classical Model for Spectroscopy Page 5

Rewrite equation of motion:

for F (t ) = 0

∂ 2Q ∂Q Fext ( t ) Q(t ) = e −γt sin Ωot

+ 2 γ + ω2

0 Q =

∂t 2 ∂t m

The effect depends on the frequency of the driving field . . . like pushing someone on

a swing.

corresponding to their swinging frequency

• This leads to a big displacement.

• If you push with arbitrary frequency, nothing will happen.

• When you drive the system with frequency ω ≈ ω o there will be an efficient

transfer of power and the displacement of the H.O. will increase

Indeed, that is what an absorption spectrum is! Measure the power absorbed by the

system from the field.

Set: F0 ∝ E0

Fext ( t ) = Fo cos ωt

Fo m

Q ( t ) = A sin ( ωt + β ) = sin ( ωt + β )

( ( ω − ω ) + 4γ ω )

1

2 2

2

2 2 2

o

ω2o − ω2

tan β =

2 γω

Notice that it oscillates 90° out of phase with field when driven on resonance. →

absorbing power from field.

(ω − ω2 ) = ( ωo − ω) ( ωo + ω) ≈ 4ωo2 ( ωo − ω)

2 2 2 2 2

o

Fo m

Q(t) = 1 sin ( ωt + β )

2ωo ( ωo − ω) + γ 2

2 2

∂Q

Pavg = F (t )⋅

∂t avg

Fo2 γ

≈

4 m (ω − ω o )2 + γ 2

LORENTZIAN LINESHAPE

peak is at ω = ωo

At what frequency

shift relative to

Pav(ω) γ maximum is the

absorbed power

reduced by ½?

ω − ω o = ±γ

ω0 ω

The full-width at half-maximum intensity (FWHM) is 2γ .

peak → ω o width → γ

So what are we learning about molecules?

Well, you can see from the spectrum that we have been able to determine ω o and γ.

A

2γ

ω0 ω

ω0

≅ 3000cm−1 γ ≅ 15cm −1

2π c

2π −14

= τ = 1 × 10 s 10 fs

ω0

k

ω0 =

m

Now for the mass m we want to use the reduced mass µ or mR. (This is the

effective mass: we need this for 2 masses on a spring with a fixed center of mass.)

mAmB

µ = mR = for a diatomic molecule A-B.

mA + mB

µ ( H 35Cl ) = 0.97 ( ω0 ) A ( mR )B

=

µ ( D35Cl ) = 1.89 ( ω0 ) B ( mR )A

Therefore, we predict:

ω0 ( DCl ) → 2150cm −1

What about F0 ?

What is a?

• A neutral body should feel no force, but molecules are made of many charges

species and have positive and negative charges.

Dipole moment:

µ H

µ=Σql δ+

Cl

distance

δ-

charge

In an electric field, this dipole will feel a force.

V = −µ ⋅ E

∂V ∂µ

F=− = ⋅E

∂Q ∂Q

• If the bond is aligned with the electric field, then the oscillating field can act to

stretch or compress the bond through attractive and repulsive electrostatic

interactions with the charges.

• The ability of the field to act on Q depends on the alignment of the dipole moment

with the field. If there is an angle θ between µ and E, then

∂µ

F0 = E 0 cos θ (…for a single molecule)

∂Q

So we have also been able to predict:

µ: The strength of the absorption peak is related to how much charge is moved when

you displace a coordinate:

You can study a crystal where all molecules have the same orientation, and how

by rotating the light polarization, you can tell how different vibrations are

oriented.

instance, me << mw .

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