Summary: A frequency square is a matrix in which each row and column is a permutation of the same multiset of symbols. We consider only binary frequency squares of order \(n\) with \(n/2\) zeros and \(n/2\) ones in each row and column. Two such frequency squares are orthogonal if, when superimposed, each of the 4 possible ordered pairs of entries occurs equally often. In this context we say that a set of \(k\text{-MOFS}(n)\) is a set of \(k\) binary frequency squares of order \(n\) in which each pair of squares is orthogonal. A set of \(k\text{-MOFS}(n)\) must satisfy \(k\le(n-1)^2\), and any set of MOFS achieving this bound is said to be complete. For any \(n\) for which there exists a Hadamard matrix of order \(n\) we show that there exists at least \(2^{n^2/4-O(n\log n)}\) isomorphism classes of complete sets of \(\text{MOFS}(n)\). For \(2<n\equiv2\pmod4\) we show that there exists a set of \(17\text{-MOFS}(n)\) but no complete set of \(\text{MOFS}(n)\). A set of \(k\text{-maxMOFS}(n)\) is a set of \(k\)-MOFS \((n)\) that is not contained in any set of \((k+1)\text{-MOFS}(n)\). By computer enumeration, we establish that there exists a set of \(k\text{-maxMOFS} (6)\) if and only if \(k\in\{1,17\}\) or \(5\le k\le 15\). We show that up to isomorphism there is a unique \(1\text{-maxMOFS}(n)\) if \(n\equiv2\pmod4\), whereas no \(1\text{-maxMOFS}(n)\) exists for \(n\equiv0\pmod4\). We also prove that there exists a set of \(5\text{-maxMOFS}(n)\) for each order \(n\equiv 2\pmod{4}\) where \(n\geq 6\).
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