You cannot do what you want to do in the form preprocessor.
Try using hook_form_alter() instead.
Keep reading for more information on why your current code doesn't work.
If you look at drupal_render() you can see that it runs this to theme the element:
if (isset($elements['#theme'])) {
$elements['#children'] = theme($elements['#theme'], $elements);
}
This call to theme() is pretty much where your preprocess code code is running.
The output of that theme function (theme_form() outputs a string of form markup) is then going into $elements['#children'].
Then further down in drupal_render() it does this:
if (!empty($elements['#attached'])) {
drupal_process_attached($elements);
}
But the #attached code you added never ended up back in the $elements of the drupal_render() function though so nothing happened.