We demonstrated that the weak van der Waals-force-bound argon dimer can be nonadiabatically aligned by nonresonant femtosecond laser pulses, showing periodic alignment and anti-alignment revivals after the extinction of the laser pulse. Based on the measured nonadiabatic alignment trace, the rotational constant of the argon dimer ground state is determined to be B 0 = 0.05756 ± 0.00004 cm −1 . Noticeable alignment dependence of frustrated tunneling ionization and bond-softening induced dissociation of the argon dimer are observed. PACS number(s): 32.80. Rm, 33.15.Bh, 42.65.Re Moderately intense laser pulses can efficiently align molecules, i.e., confine the molecular axes to axes fixed in space. In the nonadiabatic limit where the pulse duration is much smaller than the inherent rotational period a rotational wave packet is induced in each molecule by stimulated Raman transitions. The quantum beats between the states leads to field-free alignment and anti-alignment revivals of the nonadiabatically aligned molecular ensemble after the laser pulse [1]. In the past, the nonadiabatic molecular alignment has attracted a lot of interest for its extensive range of applications such as tomographic imaging of molecular orbitals [2], laser induced electron diffraction [3], quantum interference in high-harmonic generation [4], and ultrashort laser pulse manipulation and characterization [5,6]. The degree of molecular alignment could be increased by using a train of sequential pulses [7] or shaped ultrashort pulses [8]. Threedimensional alignment of complex molecules were created by using elliptically polarized laser pulses [9,10]. Recently, adiabatic alignments of rare-gas dimers with nanosecond pulses were demonstrated to characterize the polarizability anisotropies [11]. Nonadiabatic alignment of molecular cluster was achieved to extract the rotational constant [12], which requires a molecular cluster to possess a long-lived excited state and thus cannot be applied to the rare-gas dimer.In this Rapid Communication, we demonstrate that the weak van der Waals-force-bound rare-gas argon dimer (Ar 2 ) can be nonadiabatically aligned by using nonresonant femtosecond laser pulses. The field-free alignment and antialignment revival structures were measured up to ∼1 ns after the nonadiabatic excitation of the laser pulse without noticeable decay of alignment contrast and change of the shape, indicating a well-preserved coherence of the rotational wave packets. We extracted the ground state rotational constant from the nonadiabatic alignment trace and determine it to be B 0 = 0.05756 ± 0.00004 cm −1 . The alignment dependence of the bond-softening induced dissociation and frustrated tunneling ionization of argon dimer are observed.The Ar 2 bound by the weak van der Waals force (∼12.3 meV or 99.2 cm −1 ) at a large internuclear distance (R e ∼7.1 a.u.) [13,14] shows features of both atoms and molecules * doerner@atom.uni-frankfurt.de and has attracted growing interest for its interaction with ions [15], synchrotron radiation [16...