Cannot unmount disks

Hi:
I have been reading the post here in the Mac Pro forum for about six months and this is my first answer (and my first problem with my MP)
In short, the problem I am having is that Carbon Copy Cloner, wich I have been using for cloning my start up disk to a second internal HD without any problem since I bought my MP, has stopped doing so. The message “can not unmount disk“ shows up. Can not unmount in Disk Utility neither. So, I can not clone my disk as my normal security routine. Rebuilding start up disk´s directory (wich I do before every week clone) with DW4 is not longer possible, nor even booting from DW4 cd. This started happennig after my first system freeze and the installation of a 3rd HD in bay 3 (the same day and in that order) After freeze I repaired with Maintenance, then I installed the HD.
Any help will be very, very wellcome.
(and excuse for my english, guys.)
Mac Pro   Mac OS X (10.4.10)  

Hi The Hatter:
I do appreciate very much your help in this matter. I have learned a lot reading your answers to another peolpe´s questions.
To the point:
MAINTENANCE is a system maintenance and cleaning app. I switched to it from ONYX. Take a look at it at:
http://www.titanium.free.fr/pgs2/english/maintenance.html
I am sure you know well this app, but maybe I wrote its name in a funny way. I do my cleaning tasks with MAIN MENU as well. Wich one is the best, in your opinion?
I do boot from my clone disk every week. From it I repair the directory of my “main“ disk. Then I restart and boot from my “main“ disk and clone it (using CCC) to my Back Up HD. I do reuild the directoy before cloning following a recommendation I found in Bombich´s forums. This is about not to cloning a already “deffective“ system. When this problem appeared I booted from DW cd as a last option procedure.
You are right!!! I would be doing better with a Emergency Partition. I have been lazy on this point.
Until now, I thought that running maintenance scripts and cleaning with MAINTENANCE (or ONYX) and rebuilding directory before cloning to another HD would keep me safe.
Know I believe that to be safe the best I can do is not to have a computer and move to a deep, fresh and green forest.
So. Wich is your maintenance and back up procedure, Hatter? I am stilI learning and am sure that it would be a good thing to know how do you keep your machine safe.
(But think about the forest, Hatter... Think about it...)
Mac Pro   Mac OS X (10.4.10)  

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    And help would be greatly appriciated. Thank you!!
    -Julien

    There should be a simple explanation. Many background programs on your Mac, including Spotlight, access files on all formatted volumes connected to the computer; most of these programs are designed to allow an in-use volume to be unmounted without causing issue, but one notorious counterexample is the iTunesHelper background process. iTunesHelper coordinates iTunes' interactions with the rest of your computer, and may be using files on your iMac's hard disk, preventing you from unmounting the volume.
    If iTunesHelper is running in the background, it's probably causing your issue, so you can just kill it (quit) from Activity Monitor. Search Spotlight for it, or open your /Applications/Utilities folder - you should see Activity Monitor near the top of the list. In the list of processes you see, find and select iTunesHelper and click the "Quit Process" button up top.
    Now try running Drive Genius's Defrag again. It should be able to unmount your internal drive and run the repair normally. Just remember to leave your iMac alone while it's defragging! You don't want to accidentally interrupt the process.

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