The Potential of Spot Size Control in Shaping the Thickness Distribution in Ultrashort Laser Deposition

The availability of new-generation femtosecond lasers capable of delivering pulses with energies in the hundreds of mJ, or even in the joules range, has called for a revision of the effect of scaling spot size on the material distribution within the plasma plume. Employing a state-of-the-art Szatmári-type hybrid dye-excimer laser system emitting 248 nm pulses with a maximum energy of 20 mJ and duration of 600 fs, copper films were grown in the classical pulsed laser deposition geometry. The exceptionally clean temporal profile of the laser pulses yielded a femtosecond component of 4.18 ± 0.19 mJ, accompanied by a 0.22 ± 0.01 mJ ASE pedestal on the target surface. While varying the spot sizes, the plasma plume consistently exhibited an extremely forward-peaked distribution. Deposition rates, defined as peak thickness per number of pulses, ranged from 0.030 to 0.114 nm/pulse, with a gradual narrowing of the thickness distribution as the spot area increased from 0.085 to 1.01 mm² while keeping the pulse energy constant. The material distribution on the silicon substrates was characterized using the f(Θ) = AcosΘ + (1 - A)cosΘ formalism, revealing exponents characterizing the forward-peaked component of the thickness profile of the film material along the axes, ranging from k = 15 up to exceptionally high values exceeding 50, as the spot area increased. Consequently, spot size control and outstanding beam quality ensured that majority of the ablated material was confined to the central region of the plume, indicating the potential of PLD (pulsed laser deposition) for highly efficient localized deposition of exotic materials.