NOVELTY - Substituted 4H-imidazo(1.2-a)imidazole compounds (I) and (V) are new.    USE - (I) are useful: in an organic electronic device, which is an electroluminescent device, and used in an apparatus comprising stationary visual display units comprising visual display units of computers, televisions, visual display units in printers, kitchen appliances and advertising panels, illuminations, information panels, and mobile visual display units comprising visual display units in cellphones, tablet personal computers, laptops, digital cameras, media player (MP3) players, vehicles and destination displays on buses and trains, illumination units, keyboards, items of clothing, furniture or wallpaper; in electrophotographic photoreceptors, photoelectric converters, organic solar cells (organic photovoltaics), switching elements, organic light emitting field effect transistors, image sensors, dye lasers or electroluminescent devices (all claimed); in organic LEDs, organic field effect transistors, organic thin film transistors and organic solar cells; as matrix and/or hole/exciton blocker materials for blue and green emitters e.g. light blue or deep blue emitters; and as conductor/complementary materials in organic electronics application comprising switching elements and organic solar cells.    ADVANTAGE - (I) provides: electroluminescent devices with improved efficiency, stability, manufacturability and spectral characteristics; and organic LEDs with good efficiencies, good operative lifetimes and high stability to thermal stress and low use and operating voltage.    DETAILED DESCRIPTION - Substituted 4H-imidazo(1.2-a)imidazole compounds of formulae (I) and (V) are new.    X6 = -N=; and    X7 = -NR1-; or    X7 = =N-; and    X6 = -NR1-;    R1 = -A1-(A2)p-(A3)q-(A4)-r-R6;    X6a = -N=; and    X7a = -NR1a-; or    X7a = =N-; and    X6a = -NR1a-;    R1a = -A1-(A2)p-(A3)q-(A4)-r-(R6a);    p, q, r = 0 or 1;    A1-A4 = 6-24C arylene or 2-30C heteroarylene (both optionally substituted by G), and may be interrupted by at least one -(SiR7R8)-;    R2-R4, R6 = 6-24C aryl or 2-30C heteroaryl (both optionally substituted by G), H, 1-25C alkyl (optionally substituted by E and/or interrupted by D);    R6 = 6-24C aryl or 2-30C heteroaryl (both optionally substituted by G), H or -(SiR20R21R22);    R7, R8 = 6-24C aryl (optionally substituted by G) or 1-25C alkyl;    X1 = N or CR9;    X2 = N or CR10; either    R9, R10 = 6-24C aryl or 2-30C heteroaryl (both optionally substituted by G), H, 1-25C alkyl (optionally substituted by E and/or interrupted by D); or    R9R10 = ring (optionally substituted);    R20-R22 = 1-25C alkyl or 6-24C aryl (optionally substituted by G);    D = -CO-, -COO-, -S-, -SO-, -SO2-, -O-, -NR65-, -SiR70R71-, -POR7 2-, -CR63=CR64- or -C=C-;    E = -OR69, -SR69, -NR65R6, -COR68, -COOR67, -CONR65R66, -CN or halo;    G = 6-24C aryl or 2-30C heteroaryl (both optionally substituted by F), 1-18C alkyl (optionally interrupted by O) or E;    R63, R64 = 6-18C aryl (optionally substituted by 1-18C alkyl), 1-18C alkoxy, 1-8C alkyl (optionally interrupted by -O-); either    R65, R66 = R63; or    R65R66 = 5 or 6 membered ring;    R67, R69 = R63;    R68 = R63 or H;    R70, R71 = 1-18C alkyl or 6-18C aryl (optionally substituted by 1-18C alkyl);    R72 = 1-18C alkyl or 6-18C aryl (optionally substituted by 1-8C alkyl);    R6a = halo, ZnX12 or -SnR207R208R209; either    R207-R209 = H or 1-6C alkyl; or    two of R207-R209 = ring, and optionally branched;    X12 = halo, -OS(O)2CF3, -OS(O)2-aryl, -OS(O)2CH3, -B(OH)2, -B(OY1)2, substituted benzo(1,3,2)dioxaborole moiety of formula (c), substituted dioxaborane moiety of formula (d), -BF4Na or -BF4K;    Y1 = 1-10C alkyl;    Y2 = 2-10C alkylene; and    Y13, Y14 = H or 1-10C alkyl.    Provided that (I) are not 9-(1,1';3',1'')terphenyl-5'-yl-9H-4b,9,10-triaza-indeno(1,2-a)indene, 9-tetraphenyl-5-yl-9H-4b,9,10-triaza-indeno(1,2-a)indene, 2,7-diphenyl-9-(1,1';3',1'')terphenyl-5'-yl-9H-4b,9,10-triaza-indeno(1,2-a)indene, 9-(4,6-diphenyl-(1,3,5)triazin-2-yl)-9H-4b,9,10-triaza-indeno(1,2-a)indene, 12-phenyl-12H-4b,11,12-triaza-benzo(5,6)pentaleno(1,2-b)naphthalene, diphenyl-(9-phenyl-9H-4b,9,10-triaza-indeno(1,2-a)inden-2-yl)-amine or 9-phenyl-2-(9-phenyl-9H-carbazol-3-yl)-9H-4b,9,10-triaza-indeno(1,2-a)indene. INDEPENDENT CLAIMS are also included for:    (1) a hole transport layer or an emitting layer comprising (I); and    (2) the preparation of (I).