Although geometric phases in quantum evolution were historically overlooked, their active control now stimulates strategies for constructing robust quantum technologies. Here, we demonstrate arbitrary single-qubit holonomic gates from a single cycle of non-adiabatic evolution, eliminating the need to concatenate two separate cycles. Our method varies the amplitude, phase, and detuning of a two-tone optical field to control the non-Abelian geometric phase acquired by a nitrogen-vacancy center in diamond over a coherent excitation cycle. We demonstrate the enhanced robustness of detuned gates to excited-state decoherence and provide insights for optimizing fast holonomic control in dissipative quantum systems.Besides its central role in the understanding of contemporary physics [1,2], the quantum geometric phase is gaining recognition as a powerful resource for practical applications using quantum systems [3][4][5]. The manipulation of nanoscale systems has progressed rapidly towards realizing quantum-enhanced information processing and sensing, but also revealed the necessity for new methods to combat noise and decoherence [6][7][8]. Due to their intrinsic tolerance to local fluctuations [9,10], geometric phases offer an attractive route for implementing high-fidelity quantum logic. This approach, termed holonomic quantum computation (HQC) [3,[11][12][13][14][15], employs the cyclic evolution of quantum states and derives its resilience from the global geometric structure of the evolution in Hilbert space. Arising both for adiabatic [16] and non-adiabatic [17] cycles, geometric phases can be either Abelian (phase shifts) or non-Abelian (matrix transformations) [18] by acting on a single state or a subspace of states, respectively.Recently, non-Abelian, non-adiabatic holonomic gates using three-level dynamics [19] were proposed to match the computational universality of earlier adiabatic schemes [3,[11][12][13], but also eliminate the restriction of slow evolution. By reducing the run-time of holonomic gates, and thus their exposure to decoherence, this advance enabled experimental demonstration of HQC in superconducting qubits [20], nuclear spin ensembles in liquid [21], and nitrogen-vacancy (NV) centers in diamond [22,23]. However, these initial demonstrations were limited to fixed rotation angles about arbitrary axes, and thus required two non-adiabatic loops of evolution, from two iterations of experimental control, to execute an arbitrary gate [20][21][22][23]. Alternatively, variable angle rotations from a single non-adiabatic loop can be achieved using Abelian geometric phases [14,24] or hyperbolic secant pulses [25][26][27], but these approaches are complicated by a concomitant dynamic phase. To address these shortcomings, non-Abelian, non-adiabatic single-loop schemes * awsch@uchicago.edu [28,29] were designed to allow purely geometric, arbitrary angle rotations about arbitrary axes with a single experimental iteration.In this Letter, we realize single-loop, single-qubit holonomic gates by implementing th...