Measurements of the linear dichroism and of the polarization of the fluorescence with oriented chloroplasts have revealed a definite orientation of the pigment molecules with respect to the membrane plane. The Qy transition moments of the chlorophyll a molecules are more closely inclined with respect to this plane for the forms absorbing at longer wavelengths than for those absorbing at shorter wavelengths. The fluorescence depolarization by energy transfer, determined with magnetically-oriented chloroplasts, indicates that the degree of local order increases with wavelength for the different (absorption wavelength) forms of chlorophyll a in vivo. Laser pulses of either picosecond or microsecond duration have been used to probe the emission spectrum, lifetime and quantum yield of fluorescence of chloroplasts at various temperatures. With single picosecond pulses, singlet-singlet annihilations occur within the light-harvesting chlorophyll molecules. In the case of microsecond pulses, triplet excitions act as efficient quenchers of the singlets. By monitoring both the yield of carotenoid triplets and of the fluorescence during and after a laser flash, one can show that the carotenoid triplets account for part of but not all the fluorescence quenching.