Recently, an alternative Hamiltonian constraint for Loop Quantum Cosmology has been put forward by Dapor and Liegener, inspired by previous work on regularization due to Thiemann. Here, we quantize this Hamiltonian following a prescription for cosmology proposed by Mart\'{\i}n-Benito, Mena Marug\'an, and Olmedo. To this effect, we first regularize the Euclidean and Lorentzian parts of the Hamiltonian constraint separately in the case of a Bianchi I cosmology. This allows us to identify a natural symmetrization of the Hamiltonian which is apparent in anisotropic scenarios. Preserving this symmetrization in isotropic regimes, we then determine the Hamiltonian constraint corresponding to a Friedmann-Lema\^itre-Robertson-Walker cosmology, which we proceed to quantize. We compute the action of this Hamiltonian operator in the volume eigenbasis and show that it takes the form of a fourth-order difference equation, unlike in standard Loop Quantum Cosmology, where it is known to be of second order. We investigate the superselection sectors of our constraint operator, proving that they are semilattices supported only on either the positive or the negative semiaxis, depending on the triad orientation. Remarkably, the decoupling between semiaxes allows us to write a closed expression for the generalized eigenfunctions of the geometric part of the constraint. This expression is totally determined by the values at the two points of the semilattice that are closest to the origin, namely the two contributions with smallest eigenvolume. This is in clear contrast with the situation found for the standard Hamiltonian of Loop Quantum Cosmology, where only the smallest value is free. This result indicates that the degeneracy of the new geometric Hamiltonian operator is equal to two, doubling the possible number of solutions with respect to the conventional quantization considered until now.
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