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Chemistry 352

Anharmonicity

Spectroscopic Units

In vibrational spectroscopy, energies are almost always reported using spectroscopic units (wavenumbers, \(\text{cm}^{-1}\)) rather than joules. This choice reflects how vibrational spectra are measured and how naturally molecular vibrations relate to frequency.

Experimentally, vibrational transitions are observed by measuring the frequency or wavelength of absorbed or emitted radiation. Reporting results in wavenumbers provides a direct measure of this frequency:

\[ \tilde{\nu} = \frac{1}{\lambda} = \frac{\nu}{c}. \]

Because energy is related to frequency by \(E = h\nu\), using \(\text{cm}^{-1}\) is equivalent to dividing all energies by \(hc\). This produces numbers that are more convenient in size and directly comparable to measured spectra.


Vibrational term values

Instead of working with energies \(E_v\), vibrational levels are often expressed as term values, denoted \(G_v\), defined by

\[ G_v \equiv \frac{E_v}{hc}. \]

For the harmonic oscillator, this gives

\[ G_v = \omega_e\left(v + \frac{1}{2}\right), \]

where \(v = 0,1,2,\ldots\) is the vibrational quantum number and \(\omega_e\) is the harmonic vibrational constant, expressed in \(\text{cm}^{-1}\).

The vibrational constant \(\omega_e\) is related to the molecular force constant and reduced mass by

\[ \omega_e = \frac{1}{2\pi c} \sqrt{\frac{k}{\mu}}. \]


Writing vibrational energies in this form emphasizes that adjacent vibrational levels are equally spaced in the harmonic approximation and that their spacing is directly related to the strength of the bond (\(k\)) and the reduced mass (\( \mu \)).

From this point forward, vibrational energies and transitions will be described using term values \(G_v\) and wavenumbers \(\text{cm}^{-1}\), which is the natural language of vibrational spectroscopy.

Big idea: spectroscopic units connect theory directly to experiment, allowing vibrational energy levels and transition frequencies to be discussed using the quantities that are actually measured.

Worked example: force constant of HBr from \( \omega_e \)

For a diatomic harmonic oscillator, the vibrational term-value constant is \( \omega_e = \frac{1}{2\pi c}\sqrt{\frac{k}{\mu}} \), so we can solve for the force constant: \( k = (2\pi c\,\omega_e)^2\,\mu \).

For HBr, use \( \omega_e = 2648.975\ \text{cm}^{-1} \). :contentReference[oaicite:0]{index=0}

  1. Convert \( \omega_e \) to SI (m−1): \( 2648.975\ \text{cm}^{-1} = 2.648975\times 10^5\ \text{m}^{-1} \).
  2. Compute the reduced mass (using isotopes \( ^1\!H \) and \( ^{79}\!Br \)): \( \mu=\frac{m_H m_{Br}}{m_H+m_{Br}} \approx 1.65\times 10^{-27}\ \text{kg} \).
  3. Plug into \( k=(2\pi c\,\omega_e)^2\mu \):
    \[ k \approx \big(2\pi(2.9979\times 10^8\ \text{m s}^{-1})(2.648975\times 10^5\ \text{m}^{-1})\big)^2 (1.65\times 10^{-27}\ \text{kg}) \approx 4.11\times 10^2\ \text{N m}^{-1}. \]

Interpretation: \( k \) measures bond “stiffness.” Larger \( k \) means a steeper potential well near \( r_e \) and a higher vibrational frequency.

Comparison table: \( \omega_e \), reduced mass \( \mu \), and force constant \( k \)

Force constants computed from \( k=(2\pi c\,\omega_e)^2\mu \). (Reduced masses below were calculated using common isotopes: \( ^{35}\!Cl \), \( ^{79}\!Br \), \( ^{127}\!I \), \( ^{19}\!F \), \( ^{16}\!O \), \( ^{14}\!N \).)

Molecule \( \omega_e \) (cm−1) \( \mu \) (kg) \( k \) (N/m)
HCl 2990.95 1.63×10−27 5.16×102
HBr 2648.975 1.65×10−27 4.11×102
HI 2309.01 1.66×10−27 3.14×102
F2 916.64 1.58×10−26 4.70×102
O2 1580 1.33×10−26 1.18×103
N2 2359 1.16×10−26 2.30×103

Source notes for \( \omega_e \): HCl and the O2/N2 values are given in the Oxford notes, while HBr, HI, and F2 are from the NIST Webbook of Chemistry “Constants of Diatomic Molecules” tables.

Although the harmonic oscillator provides a powerful and simple model for molecular vibrations, it has important physical shortcomings. These limitations become apparent when we consider large-amplitude vibrations.


Shortcomings of the harmonic oscillator model

These issues indicate that the harmonic oscillator is best viewed as a small-amplitude approximation to real molecular vibrations.


The Morse potential

A more realistic model of a diatomic bond is provided by the Morse potential:

\[ U(x)=D_e\left(1-e^{-\beta x}\right)^2. \]

Here \(D_e\) is the dissociation energy (the depth of the potential well), and \(\beta\) controls the width and steepness of the potential.

Unlike the harmonic potential, the Morse potential:


Anharmonicity and vibrational energy levels

The Morse potential introduces anharmonicity, meaning that the vibrational energy levels are no longer equally spaced. Instead, the term values are well approximated by

\[ G_v = \omega_e\left(v+\frac{1}{2}\right) - \omega_e x_e\left(v+\frac{1}{2}\right)^2. \]

The anharmonicity constant \(x_e\) causes the spacing between adjacent vibrational levels to decrease as \(v\) increases, eventually leading to dissociation.

Comparison of Harmonic Oscillator and Morse potential energy surfaces

The Morse potential improves on the picture by allowing for dissociation at long bond distances, but still fail at very short bond distances. However, because the Morse potential rises much more quickly as the bond gets shorter, this is less of a problem than with the Harmonic Oscillator.

Big idea: the Morse potential corrects the most serious physical deficiencies of the harmonic oscillator by allowing dissociation and introducing anharmonicity, bringing the vibrational model closer to real molecular behavior.

Your turn

Problem 1
Why are vibrational energies usually reported in \(\text{cm}^{-1}\) rather than joules?
They eliminate Planck’s constant from the equations
They are directly proportional to measured frequencies
They depend only on reduced mass
They remove the need for normalization
Problem 2
What is the value of \(r\) at the minimum of the Morse potential?
\(r_e\)
\(0\)
\(\beta\)
It depends on \(D_e\)
Problem 3
Which parameter in the Morse potential is responsible for molecular dissociation?
\(k\)
\(\omega_e\)
\( (1 - e^{-\beta x})^2 \)
\(D_e\)
Problem 4
In the anharmonic expression \(G_v=\omega_e(v+\tfrac{1}{2})-\omega_e x_e(v+\tfrac{1}{2})^2\), what physical effect does the second term represent?
Zero-point energy
Reduced mass correction
Decreasing level spacing at higher \(v\)
Normalization of wavefunctions
Problem 5
Which statement best explains why the harmonic oscillator predicts equally spaced vibrational levels?
The reduced mass is constant
The potential energy is quadratic in displacement
The wavefunctions are orthogonal
The force constant is large
Problem 6 (Qualitative)
Why does the Morse potential give a more realistic description of molecular vibrations than the harmonic oscillator?
It allows for bond dissociation and anharmonic level spacing
It eliminates zero-point energy
It removes the need for reduced mass
It produces analytic wavefunctions

Key points (one glance)

Big picture: using spectroscopic units and anharmonic corrections connects quantum-mechanical models directly to real vibrational spectra.