A new guest-host composition of 3-(4-nitrophenyl) azo-9-(2-ethyl) hexyl-2-(2-ethyl) hexyloxycarbazole as chromophore and 2,2-bis{4-[2-hydroxy-9-(carbazol-9-yl)-5-(carbazol-9-methyl)-4,7-dioxanonyloxy] phenyl} propane (molecular glass) as host for all-optical poling application was developed and investigated. A comparison between molecular glass and commonly used bisphenol Z polycarbonate as host showed a slightly better ability for the molecular glass to keep the azophenylcarbazole molecules oriented. Erasure while reading the non-centrosymmetry created is demonstrated and explained. Using an adopted model orientational diffusion coefficient, lifetime of cis isomer and probabilities of redistribution were evaluated.