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This is about photons.

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Phonons can be created by thermal excitation of the lattice and play a very important role in

the thermal properties of materials. We will now look at two such properties:

1. Heat capacity, which can be treated within the harmonic approximation.

2. Thermal conductivity, which requires us to go beyond the harmonic approximation

and consider interactions between phonons (anharmonic effects)

Heat capacity

The total heat capacity of a crystal can be written as

௦ ௧௦ ௧

ܥ = ᇣᇧ

ܥᇧᇤᇧ

ᇧᇥ + ܥ

ᇣᇧ

ᇧᇤᇧ ᇧᇥ + ᇣᇧ

ܥᇧᇤᇧᇧᇥ

௦ௗ௦ ௧௦௬ ௧௦௬

߲ℰ

ܥ = ൬ ൰

߲ܶ

Note, for solids ܥ ≈ ܥ .

Classically, if we think of a solid as ܰ atoms, equipartition theorem would give

1

ℰ = 6ܰ × ݇ ܶ

2

Where the factor of 6 comes from 6 degrees of freedom per atom (KE + PE × 3 spatial

degrees of freedom each). Hence

ܥ = 3ܰ݇

This is known as the Dulong and Petit law (~1819). It holds for some solids at room

temperature but fails at low temperature where a quantum mechanical treatment is

necessary.

Let’s first take a look at the heat capacity of a single quantum harmonic oscillator (QHO).

The energy eigenvalues are

1

ℰ = ൬݊ + ൰ ℏ߱

2

To find the average thermal equilibrium occupancy 〈݊〉 of this QHO (i.e., how many phonons

are in mode ߱ at a given temperature), we use the usual statistical mechanics approach.

݁ ିℰ /ಳ ் ∑ ݊൫݁ ିℏఠ/ଶಳ ் ൯݁ ିℏఠ/ಳ ்

〈݊〉 = ݊ = ݊ =

ܼ ∑ (݁ ିℏఠ/ଶಳ ் )݁ ିℏఠ/ಳ்

4-1

ିℰ /ಳ ்

where is the probability of state ݊ being occupied and ܼ = ∑ ݁ is the partition

function. Cancelling out the two terms in brackets,

∑ ݊݁ ିℏఠ/ಳ ் ݇ ܶ ଶ ߲ ln ܣ

〈݊〉 = =

∑ ݁ ିℏఠ/ಳ ் ℏ߱ ߲ܶ

ିଵ

where ∑ = ܣஶୀ ݁

ିℏఠ/ಳ ்

= 1 + ݁ ିℏఠ/ಳ் + ݁ ିଶఠ/ಳ ் + ⋯ = ൫1 − ݁ ିℏఠ/ಳ் ൯ (geometric

series). Now,

݇ ܶ ଶ ߲ (−ln(1 − ݁ ିℏఠ/ಳ் )) ݇ ܶ ଶ 1 ℏ߱ ିℏఠ/ ்

〈݊〉 = = ൬− ݁ ಳ ൰

ℏ߱ ߲ܶ ℏ߱ ݁ ିℏఠ/ಳ் ݇ ܶ

which simplifies to

1

〈݊〉 =

݁ ℏఠ/ಳ ் −1

This is just the Bose-Einstein factor, the same as the well-known expression for the Planck

distribution for black body radiation. Therefore, the average energy of this oscillator is

1 1 ℏ߱

ℰ̅ = ൬〈݊〉 + ൰ ℏ߱ = ℏ߱ + ℏఠ/ ்

2 2 ݁ ಳ −1

߲ℰ̅ 1 ℏ߱

ܥ = ቆ ቇ = ℏ߱ ൬− ℏఠ/ ் ൰ ൬− ൰ ݁ ℏఠ/ಳ ்

߲ܶ ݁ ಳ −1 ݇ ܶ ଶ

ℏ߱ ଶ ݁ ℏఠ/ಳ்

ܥ = ݇ ൬ ൰

݇ ܶ (݁ ℏఠ/ಳ் − 1)ଶ

ℏఠ

or, defining a characteristic temperature Θ ≡

ಳ

Θ ଶ ݁ /்

ܥ = ݇ ൬ ൰

ܶ (݁ /் − 1)ଶ

ଶ

In the low-temperature limit, as ܶ → 0, ݁ /் ≫ 1 and ܥ → ݇ ቀ ቁ ݁ ି/் .

்

ଶ ଵ

In the high-temperature limit, as ܶ → ∞, ݁ /் ≈ 1 + + ⋯ and ܥ → ݇ ቀ ቁ మ = ݇ ,

் ் ౸

ቀଵା ିଵቁ

as expected from equipartition.

Einstein considered the solid as a collection of ܰ simple QHOs all with the same frequency

12

߱ா (corresponding to typical optical mode frequency ~10 Hz). If we define an Einstein

temperature as Θா = ℏ߱/݇ , then in 3D

Θ ଶ ݁ ు /்

ܥ = 3ܰ݇ ൬ ൰

ܶ (݁ ు /் − 1)ଶ

For ܶ ≫ Θா , ܥ ≈ 3ܰ݇ , i.e. we recover the law of Dulong and Petit.

4-2

For ܶ اȣா , ܥ ି ݁ ןు Ȁ் . This explains qualitatively the observed decrease of ܥ at low

temperature, but experimental data do not decrease as quickly— to explain this we need low

frequency (acoustic) phonons.

Einstein theory fit (dashed line) to experimental heat capacity data for diamond (open

circles); Θா = 1,320 K. Reproduced from Einstein’s seminal 1907 article in Annalen der

Physik [vol. 22, pp. 180-190].

To calculate the total lattice energy at a certain temperature more accurately we need to

sum up the contributions from all phonon modes, i.e., over all ܓand for all branches ݆

1

ࣟ ൌ ߱ܓǡ ൬݊൫߱ܓǡ ൯ + ൰

2

ܓ

Since the spacing between the states ȟ݇ ൌ ʹߨȀ ܮis very small compared to ʹߨȀܽ, the width

1

of the Brilouin zone , we can replace the sum with an integral

ஶ

1

ࣟ ൌ න ݃(߱)߱ ൬݊(߱) + ൰ ݀߱

2

where ݃ሺ߱ሻ is the density of states such that the number of states between ߱ and ߱ ݀߱ is

݃(߱)݀߱. In reality, ݃(߱) is a complicated function of ߱, so we need some approximations.

Debye theory

Einstein assumed a single frequency ߱ா . Debye took into account different frequencies

assuming a linear dependence of ߱ on ݇, i.e., ߱ ൌ ݒௌ ݇. We now know these as acoustic

phonons (though Debye’s theory predates the phonon theory of lattice dynamics and was

based on classical elasticity). The assumptions of the model are:

ଶగȀ

Typically ̱ܽͳͲିଵ m, ̱݇ͳͲିଶ mିଵ so that ~10଼

1

ଶగȀ

4-3

- The crystal is harmonic (the phonon modes are independent)

- Elastic waves are non-dispersive (߱ ൌ ݒ௦ ݇)

- The crystal is isotropic

- There is a high-frequency cut off ߱ chosen in such a way that the total number of

ఠವ

modes is correct, i.e. that per branch ∫ ݃(߱)݀߱ ൌ ܰ, the number of atoms in the

crystal

Density of states

We now need an expression for the density of states.

ଶగ

In 1D, the states are separated by ȟ݇௫ = , where ܮis the dimension (length) of the crystal.

ଶగ

In 2D, the allowed states form a grid with spacing ȟ݇௫ ൌ ȟ݇௬ = .

Consider an annulus of radius ݇ and thickness ݀݇. The area occupied by 1 state in k-space

ଶగ ଶ ଶ

is ቀ ቁ or, equivalently, there are ቀ ቁ states per unit area. So within the annulus area

ଶగ

మ

ʹߨ݇݀݇ there are ʹߨ݇݀݇ (ଶగ)మ states, hence in 2D

ܮଶ

݃(݇)݀݇ ൌ ݇݀݇ሺʹሻ

ʹߨ

where ݃(݇) is the density of states (DOS).

ଶగ ଷ

In 3D, we have to consider a shell of volume Ͷߨ݇ ଶ ݀݇. The volume of each state is ቀ ቁ or

ଷ య

there are ቀ ቁ states per unit volume. Hence ݃(݇)݀݇ ൌ Ͷߨ݇ ଶ (ଶగ)య ݀݇or using ܸ ൌ ܮଷ

ଶగ

ܸ ଶ

݃(݇)݀݇ ൌ ݇ ݀݇ሺ͵ሻ

ʹߨ ଶ

The corresponding DOS per unit frequency ݃ሺ߱ሻ is given by

4-4

݃(߱)݀߱ = ݃(݇)݀݇

ܸ ଶ ݀݇

݃(߱) = ݇ (in 3D)

2ߨ ଶ ݀߱

per branch of the dispersion curve (e.g., for a monoatomic crystal in 3D there are 2T and 1L

branches).

To calculate the Debye frequency ߱ , we use

ఠವ

ܰ=න ݃(߱)݀߱ (per branch)

݀݇ 1 ܸ ߱ଶ

= → ݃(߱) = ଶ ଷ

݀߱ ݒ௦ 2ߨ ݒ௦

Therefore

ఠವ

ܸ ߱ଶ ܸ 1 ߱ ଷ ଷ

6ܰߨ ଶ ଷ

ܰ=න ݀߱ = ൬ ൰ → ߱ = ቆ ቇ ݒ௦

2ߨ ଶ ݒ௦ଷ 2ߨ ଶ 3 ݒ௦ ܸ

With three acoustic branches, the total lattice energy

ஶ ஶ

This is 3 because we are 1

considering 3D (?) ℰ = 3න ℏ߱݃(߱)݀߱ + 3 න ℏ߱݃(߱)݊(߱)݀߱

2

ᇣᇧᇧᇧᇧᇧᇤᇧᇧᇧᇧᇧᇥ

ℰೋು

ఠವ

ܸ ߱ଶ 1

ℰ = ℰ + 3 න ℏ߱ ଶ ଷ ℏఠ/ ் ݀߱

2ߨ ݒ௦ ݁ ಳ −1

ଵ ଷே

or, using =

ଶగమ ௩ೞయ య

ఠವ

9ܰ ఠವ ℏ߱ଷ

ℰ = ℰ + ଷ න ݀߱

߱ ݁ ℏఠ/ಳ ் − 1

Noting that the zero-point energy ℰ is independent of temperature and therefore doesn’t

contribute to the heat capacity, we can now calculate the heat capacity as

߲ℰ 9ܰ ఠವ ℏ߱ଷ ℏ߱

ܥ = = ଷන ݁ ℏఠ/ಳ ் ൬− ൰ ݀߱

߲ܶ ߱ −(݁ ℏఠ/ ்

ಳ − 1)ଶ ݇ ܶ ଶ

= න ݀߱

make everything easier. ߱ଷ ݇ ܶ ଶ (݁ ℏఠ/ಳ் − 1)ଶ

Letting = ݔℏ߱/݇ ܶ, ݀߱ = (݇ ܶ/ℏ)݀ ݔand the limits of integration become ߱ = 0 → = ݔ0

and ߱ = ߱ → = ݔℏ߱ /݇ ܶ = Θ /ܶ, so that

9ܰ ವ /் ℏ ݇ ܶ ସ ݔସ ݁ ௫

ܥ = ଷ න ൬ ൰ ݀ݔ

߱ ܶ ℏ (݁ ௫ − 1)ଶ

ܶ ଷ ವ /் ݔସ ݁ ௫

ܥ = 9ܰ݇ ൬ ൰ න ݀ݔ

Θ (݁ ௫ − 1)ଶ

ℏఠ

In the high-temperature limit, as ܶ → ∞, = ݔ → 0 so that the integrand in the above

ಳ ்

expression can be approximated to

4-5

ݔସ (1 + ݔ+ ݔଶ /2 + ⋯ )

≈ ݔଶ

(1 + ݔ+ ݔଶ /2 + ⋯ − 1)ଶ

ଵ ವ ଷ

which integrates to ቀ ቁ and therefore the heat capacity in the high temperature limit

ଷ ்

ܥ → 3ܰ݇

consistent with the Dulong & Petit law.

In the low-temperature limit, as ܶ → 0, ∞ → ݔand we can replace ߱ in the upper limit of the

integration with ∞. The integral then becomes a standard integral

ஶ

ݔସ݁ ௫ 4ߨ ସ

න ݀ݔ =

(݁ ௫ − 1)ଶ 15

This is the the low temperature T -> 0 result

and for the 3D model

12 ܶ ଷ

ܥ → ܰ݇ ߨ ସ ൬ ൰

5 Θ

This expression gives good agreement with experiment.

4-6

Density of states as a function of frequency for (a) the Debye solid and (b) an actual

crystal structure. The spectrum for the crystal starts as ߱ଶ for small ߱, but

discontinuities develop at singular points. Reproduced from Kittel’s book.

(a) Dispersion relation for a diatomic crystal. (b) Dispersion relation within the Debye

approximation.

(a) Heat capacity of solid argon at low temperature plotted against ܶ ଷ . (b) Comparison

of Debye and Einstein models. Inset shows the difference in behaviour at low

temperatures. Experimental data for silver. Reproduced from Kittel.

4-7

Anharmonicity

So far, we have considered our interatomic potential to be harmonic, i.e., our model springs

exert the same force whether extended or compressed and the spring constant is

independent of the magnitude of the displacement. The Harmonic approximation works well

for small deviations from the equilibrium positions but for large displacements (high ܶ) it

becomes bad.

Core

repulsion

Harmonic approx.

(symmetric)

Coulomb/van der

Waals attraction

For a more accurate description, we need to go beyond the harmonic terms in the expansion

( ݎ− ܽ)ଶ ߲ ଶ ܷ ( ݎ− ܽ)ଷ ߲ ଷ ܷ

ܷ( )ܽ(ܷ = )ݎ+ ቆ ଶቇ + ቆ ଷቇ +⋯

2 ߲ ݎୀ ᇣᇧᇧᇧᇧᇧᇧᇧᇤᇧᇧᇧᇧᇧᇧᇧᇥ

ᇣᇧᇧᇧᇧᇧᇧᇧᇧᇤᇧᇧᇧᇧᇧᇧᇧᇧᇥ 6 ߲ ݎୀ

ு௫௧ ௧௦

1. Thermal expansion—the average interatomic distance 〈( ܽ > 〉ݎit costs less energy to

expand than to contract)

2. Phonons interact with each other—they are no longer pure normal modes. In an

anharmonic crystal, a phonon (lattice wave) causes momentary local

contraction/expansion of the lattice. This causes a second phonon to ‘see’ a different

spring constant and the modes are therefore not independent; phonons scatter off

each other and this determines the thermal conductivity of the solid.

We will not discuss thermal expansion here as this was covered in PHAS1228.

4-8

Conservation laws for phonon-phonon collisions

Phonon-phonon collisions obey the following conservation laws

energy: ℏωଵ + ℏωଶ = ℏωଷ

but we must not forget that phonon momentum is only defined modulo a reciprocal lattice

vector and therefore one distinguishes between two types of scattering events:

st

1. The resulting wavevector ܓ lies within the 1 BZ. This is known as a ‘Normal’ event

(N). In an N event, two phonons travelling to the right combine to produce a phonon

travelling to the right.

st st

2. The resulting wavevector ܓ lies outside the 1 BZ but can be translated into the 1

2

BZ by a reciprocal lattice vector ۵. Such events are called ‘Umklapp’ events (U) . In a

U event, two phonons travelling to the right combine to produce a phonon travelling

to the left!

Heat flow carried by phonons is unaffected by N events but is impeded by Umklapp

scattering and therefore U events contribute to thermal resistivity ቀ1ൗthermal conductivityቁǤ

Thermal conductivity

Thermal conductivity ߢ relates the steady-state flow of heat across a solid to the temperature

gradient, i.e.

݀ܶ

݆௨ ൌ െߢ

݀ݔ

thermal current density [Wmିଶ ] = −thermal conductity [Wmିଵ K ିଵ ] × temp. gradient [Kmିଵ ]

2

‘Umklapp’ means ‘flip-over’ in German. Umklapp events were discovered by Peierls.

4-9

From kinetic theory of gases:

1

ߢ = ݒҧ ݈ܥሚ

3

where ݒҧ is the average particle velocity, ݈ is the mean free path and ܥሚ is the specific heat

per unit volume.

Importantly, particle conservation is not used in the derivation of this result and therefore it

3

can be applied to phonons, which are bosons and hence do not conserve particle number.

hot cold

end end

(more phonons) (less phonons)

In metals, electrons contribute to ߢ (we will evaluate this contribution later); in insulators, the

only contribution is from phonons.

Imagine that the two ends of a solid are held at

different temperatures. Moving by Δ ݔfrom ܶ + Δܶ to ܶ,

the particle (phonon) gives up energy ܿΔܶ, where ܿ is

the specific heat per particle (if ݊ is the particle density

per unit volume, ܿ = ܥሚ /݊).

If the time between collisions (scattering time) is ߬

݀ܶ ݀ܶ

Δܶ = Δ= ݔ ߬ ݒ

݀ݔ ݀ ݔ௫

where ݒ௫ is the component of the velocity along ݔ. The thermal current density is then

݆௨ = ณ

݊ × (−ܿΔܶ)

ᇣᇧᇤᇧᇥ × 〈ݒ

ต ௫〉

ௗ௦௧௬ ௧ ௩௧௬

݀ܶ

= −݊ܿ〈ݒ௫ 〉ଶ ߬

݀ݔ

Therefore ߢ = ݊ܿ〈ݒ௫ 〉ଶ ߬ = ܥሚ 〈ݒ௫ 〉ଶ ߬. For an isotropic distribution of velocities, 〈ݒ௫ 〉ଶ = 〈ݒ௬ 〉ଶ =

ଵ ଵ ଵ

〈ݒ௭ 〉ଶ = 〈〉ݒଶ, so that ߢ = ܥሚ 〈〉ݒଶ ߬ = ܥሚ 〈݈〉ݒ, or

ଷ ଷ ଷ

1

ߢ = ܥሚ ݒҧ ݈

3

Only Umklapp collisions contribute.

(Remember, ܥሚ is the heat capacity per unit volume)

3

In fact, it works even better for phonons because the speed of sound ݒௌ is a constant for acoustic

phonons not too close to the BZB, unlike ݒfor ideal gas particles, which follows the Maxwell-

Boltzmann distribution.

4-10

Temperature dependence of thermal conductivity

The temperature dependence of the thermal conductivity is determined mostly by ܥሚ and ݈ (ݒҧ

is approximately constant). The mean free path ݈ is inversely proportional to the number of

phonons.

High T (ܶtΘ ): all phonon modes up to ℏ߱ are excited; there are many phonons with large

enough |݇| to produce U-events. The number of phonons is proportional to the thermal

energy (݇ ܶ), hence ݈ ∝ ܶ ିଵ . The heat capacity is approximately constant (classical value).

Intermediate T (ܶ~Θ ): U-processes start to freeze out as average energy of phonons

decreases. The number of phonons ~ exp(−Θ /ܶ), hence ݈ ∝ exp(Θ /ܶ).

Low T (ܶ ≪ Θ ): all U-processes switch off. ݈ is limited by the size and shape of the crystal.

The temperature dependence comes entirely from ܥሚ ~(ܶ/Θ )ଷ.

crystal

size

limited by limited by

4-11

Thermal conductivity of natural abundance

(1.1% 13C) diamond (lower squares),

isotopically enriched (0.1% 13C) diamond

(upper squares), together with the low

temperature data of Slack (circles) and the

high temperature data of Vandersande et al.

(plusses). Reproduced from Wei et al. Physical

Review Letters 70, 3764 (1993).

showing the effect of boundaries for

sandblasted crystals. Mean crystal widths: (A)

7.25 mm, (B) 4.00 mm, (C) 2.14 mm, (D) 1.06

mm. Reproduced from Thatcher Physical

Review 156, 975 (1967).

4-12

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