We make use of an inhomogeneous electrostatic dipole field to impart a quantum-state-dependent deflection to a pulsed beam of OCS molecules, and show that those molecules residing in the absolute ground state, X 1 Σ + , 00 0 0 , J = 0, can be separated out by selecting the most deflected part of the molecular beam. Past the deflector, we irradiate the molecular beam by a linearly polarized pulsed nonresonant laser beam that impulsively aligns the OCS molecules. Their alignment, monitored via velocity-map imaging, is measured as a function of time, and the time dependence of the alignment is used to determine the quantum state composition of the beam. We find significant enhancements of the alignment ( cos 2 θ2D = 0.84) and of state purity (> 92%) for a state-selected, deflected beam compared with an undeflected beam.The ability to produce ensembles of atoms and molecules with a narrow distribution of quantum states has been a game-changer in atomic, molecular and optical physics, past and present. Recent examples from molecular physics include crossed beam scattering [1-4] and photodissociation dynamics studies at high resolution [5], as well as the work done with and on cold and ultracold molecules [6,7]. The techniques developed to produce molecules in (nearly) single quantum states include multipole focusing [8][9][10][11][12], Stark deceleration [13,14], Zeeman deceleration [15,16] -all of which isolate molecules that are initially populated in a particular quantum stateand buffer gas cooling [17,18] -which lowers the temperature of a sample such that the resulting thermal statedistribution contains essentially only the absolute ground state. Alternatively, ultracold alkali atoms can be photoor magneto-associated and form ultracold homo-or heteronuclear diatomic molecules occupying a single electronic, vibrational and rotational state [19,20] including, in certain cases, the absolute ground state [21,22]. All methods offer unique opportunities but are also subjected to limitations in terms of the type of molecules that the methods apply to or the particular quantum states that can be selected.Here we demonstrate an alternative method, with a history reaching back to the 1920s [23][24][25], to produce molecules in a single quantum state. Like multipole focusing and Stark or Zeeman deceleration it is based on selecting the molecules that are initially residing in a specific quantum state. We employ a dipolar deflection field * henriks@chem.au.dk † jochen.kuepper@cfel.de to disperse a well-expanded, nearly monoenergetic beam of OCS molecules according to their state-specific electric dipole moments. The inhomogeneous electric field inside the deflector has an almost constant gradient over a large area surrounding the molecular beam axis and enables dispersion of the rotational quantum states of OCS. In particular, we separate out the ground rotational state, J = 0, of the electronic and vibrational ground state, X 1 Σ + and 00 0 0 , and thereby produce a molecular beam of OCS(X 1 Σ + , 00 0 0 , J = 0) with a pu...