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A practical method utilising three-dimensional image pattern matching isproposed which, in principle, is capable of unambiguous determination of thetypes and positions of atoms in small molecules from defocus series collectedat only a few different angular orientations of the molecule. Numerical testsof the method are presented using multislice calculations of defocus series ofsmall biological molecules. The proposed technique can in future gain fromBayesian or machine-learning approaches and is likely to be useful in cryogenicelectron microscopy.

On electron imaging of small molecules, Part II: tomographic reconstruction from defocus series