We present a new subspace iteration method for computing low-lying eigenpairs (excited states) of high-dimensional quantum many-body Hamiltonians with nearest neighbor interactions on two-dimensional lattices. The method is based on a new block isometric projected entangled pair state (block-isoPEPS) ansatz that generalizes the block matrix product state (MPS) framework, widely used for Hamiltonians defined on one-dimensional chains, to two-dimensions. The proposed block-isoPEPS ansatz offers several attractive features for PEPS-based algorithms, including exact block orthogonalization, controlled local truncation via singular value decompositions, and efficient evaluation of observables. We demonstrate the proposed inexact subspace iteration for block-isoPEPS by computing excitations of the two-dimensional transverse-field Ising and Heisenberg models and compare our results with existing PEPS methods. Our results demonstrate that block isometric tensor networks provide a scalable framework for studying excitations in quantum many-body systems beyond one dimension.

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