Line-narrowing Speci’roscopy in Amorphous Solids through Polarization Detection of Spectral Holes. I. Principles

Detection of spectral satellite holes by polarization spectroscopy is proposed as a method to measure the line-narrowed eleo tronic absorption spectrum of a large molecule in an amorphous solid at low temperature. The linewidths of the zero-phonon holes yield information about molecular dephasing and the correlation of the inhomogeneous distribution of the two molecular transitions involved in the hole-burning and the detection step. Constructive or destructive interference of the signal light field with an intentionally admixed background light field yields information on the symmetry of vibronic states.