Quantum-beat spectroscopy has been used to observe excited states of t
he N-V center in diamond. For the 1.945-eV optical transition, direct
evidence is presented for the existence of GHz-scale fine structure, t
ogether with a much larger 46-cm(-1) level splitting in the E state. A
n interference effect observed in transient four-wave-mixing response
is explained with a polarization selection rule involving Zeeman coher
ence among magnetic sublevels. Also, detailed dephasing measurements v
ersus temperature and wavelength have identified the decay mechanisms
operative among the various states. A comparison of these results with
ab initio calculations of excited electronic structure and interactio
ns based on several multielectron models supports the conclusion that
the N-V center is a neutral, two-electron center governed by a strong
Jahn-Teller effect and weak spin-spin interactions.