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Molecular alignment induced by laser fields has been investigated in research laboratories for over two decades. It led to a better understanding of the fundamental processes at play in the interaction of strong laser fields with molecules, and also provided significant contributions to the fields of high harmonic generation, laser spectroscopy, and laser filamentation. In this chapter, we discuss molecular alignment produced under field-free conditions, as resulting from the interaction of a laser pulse of duration shorter than the rotational period of the molecule. The experimental results presented will be confined to the optically probed alignment of linear as well as asymmetric top molecules. Special care will be taken to describe and compare various optical methods that can be employed to characterize laser-induced molecular alignment. Promising applications of optically probed molecular alignment will be also demonstrated.