It is not a basic thing at all. No extra code is run just because a method has an attribute, so there is nowhere to put your TransactionScope code.
What you would need to do is at application start-up use reflection to iterate over every method on every class in your assembly and find the methods that are marked with AtomicAttribute, then write a custom proxy around that object. Then somehow get everything else to call your proxy instead of the real implementation, perhaps using a dependency injection framework.
Most AOP frameworks do this at build time. PostSharp for example runs after VisualStudio builds your assembly. It scans your assembly and rewrites the IL code to include the proxies and AOP interceptors. This way the assembly is all set to go when it is run, but the IL has changed from what you originally wrote.
