Fi lms of e th y le n e co nd e nse d o nt o a co ld fin ge r ma int a ine d a t 20 K we re ir radi a ted with ph ot o ns wh ose e ne rgy ra nged fro m 8.4 to 21.2 e V. At th e h ig he r ph oto n e ne rgies th e re la tiv e yie ld s of produ c ts co mp a re we ll with th ose see n in th e radi o lys is o f so lid e th y le ne. Expe rime nt s o n C H2C D2 d e m o ns tra te th a t in th e p hoto lys is h ydrogen is ma inl y fo rm ed b y th e e limin a ti o n processes C H 2C D~ ---> H AD 2)The re la tiv e proba biliti es o f th ese three pro-cesses a re ind e pe nd e nt o f th e e n e rgy o f th e in c id e nt p hoto ns fr o m 8.4 to 11. 6 e V a nd a re within expe rim e nt a l e rror id e ntic a l to th ose o bse rved in ea rl ie r g as p hase photolys is expe rim e nts . Re la t ive to ace tyle ne, cyc lo but a ne is a mi no r pro du c t a t 8.4 eV but in c reases b y a n o rd e r o f magn it ud e a t hi ghe r e ne rg ies wh e re ion s pla y a role. C yc lo buta n e , I · bute ne a nd me th ylcyclopro pa n e fo rm ed up on irradia tio n of froze n C 2H, -C 2D, mixtures cons isted ma inl y of C,DB, C.,D,H" a nd C.,H 8. Pl a us ib le m ec ha ni sm s wh ic h m ay acco u nt fo r th e fo r ma tio n of the la tt e r p rodu c ts a re exa min e d. In t he so lid p hase as in th e gas ph ase th e re la ti ve impo rta nce of H·a to m produ c t io n is see n to in c rease with in c reas in g ph oto n e ne rgy. Cyc lo propa ne, a ppa re ntl y form ed b y in se rtion of C H, int o C, H." is o bse r ved as a p rodu c t a t a ll wave · le n gth s in th e ph oto lys is, a nd in t he ra d io lys is. Key wo rd s: Et hy le ne; free rad ica l reac t ions; io n-m o lec u le reac ti o ns; ph oto lys is: po lyme ri zati o n ; ra d io lys is .