Central to the understanding of high-temperature superconductivity is the evolution of the electronic structure as doping alters the density of charge carriers in the CuO 2 planes. Superconductivity emerges along the path from a normal metal on the overdoped side to an antiferromagnetic insulator on the underdoped side. This path also exhibits a severe disruption of the overdoped normal metal's Fermi surface 1-3 . Angle-resolved photoemission spectroscopy (ARPES) on the surfaces of easily cleaved materials such as Bi 2 Sr 2 CaCu 2 O 8+δ shows that in zero magnetic field the Fermi surface breaks up into disconnected arcs 4-6 . However, in high magnetic field, quantum oscillations 7 at low temperatures in YBa 2 Cu 3 O 6.5 indicate the existence of small Fermi surface pockets [8][9][10][11][12][13][14][15][16][17][18] . Reconciling these two phenomena through ARPES studies of YBa 2 Cu 3 O 7−δ (YBCO) has been hampered by the surface sensitivity of the technique [19][20][21] . Here, we show that this difficulty stems from the polarity and resulting self-doping of the YBCO surface. Through in situ deposition of potassium atoms on cleaved YBCO, we can continuously control the surface doping and follow the evolution of the Fermi surface from the overdoped to the underdoped regime. The present approach opens the door to systematic studies of hightemperature superconductors, such as creating new electrondoped superconductors from insulating parent compounds.In the heavily overdoped regime, angular magnetoresistance oscillation 1 and angle-resolved photoemission spectroscopy (ARPES) experiments 2,3 on Tl 2 Ba 2 CuO 6+δ have arrived at a quantitative consensus in observing a large hole-like Fermi surface. On reducing the number of holes in the CuO 2 planes, the Fermi surface volume decreases in the manner expected by Luttinger's theorem, but below optimal doping the single-particle Fermi surface seems to reduce to four disconnected nodal Fermi arcs. This scenario was suggested from ARPES studies of Bi cuprates 4,5 and Ca 2−x Na x CuO 2 Cl 2 (ref. 6), and is thought to be connected to the existence of the pseudogap. The detection of quantum oscillations in oxygen-ordered ortho-II YBa 2 Cu 3 O 6.5 (YBCO6.5) suggests a different scenario involving Fermi surface reconstruction into hole and/or electron pockets 7,9,10 . These two pictures are derived from quite different measurement techniques, carried out on different materials, and under conditions of high magnetic field in one case, but zero field in the other. Owing to the complex multiband and correlated character of the electronic structure of YBCO6.5 (ref. 11), the determination of the nature of these pockets and their generality to the underdoped cuprates requires connecting transport and single-particle spectroscopy information on the same underdoped system. The study of YBCO6.5 by ARPES is thus crucial. Unfortunately, this material is complicated by the lack of a natural [001] cleavage plane (Fig. 1a)