Dynamics of new phase formation in silicon during femtosecond laser ablation

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Abstract

We experimentally demonstrated (using micro-Raman spectroscopy and transmission electron microscopy) and through numerical modeling that when an intense (1013−1014 W/cm²) femtosecond (~100 fs) laser pulse impacts the surface of silicon with (111) orientation, new polymorphic phases Si-III and Si-XII are formed on the surface and in the volume, localized in lattice defects as well as at the periphery of the ablation crater. This localization of phases is caused by the multi-stage nature of laser-induced phase transitions in silicon, specifically, the phase transitions are initiated by a shock wave, resulting in a cascading transformation process on sub-nanosecond timescales: Si-I => Si-II => => Si-III/Si-XII. The phase transition Si-I => Si-II occurs at the front of the shock wave, while at the rear of the shock wave, a field of dynamic stresses arises in the material, allowing the phase transition Si-II => Si-III/Si-XII to occur. On sub-microsecond timescales, most of the new phases disappear as the material relaxes back to its original state.

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About the authors

Е. I. Mareev

Shubnikov Institute of Crystallography of Kurchatov Complex of Crystallography and Photonics of NRC “Kurchatov Institute”

Author for correspondence.
Email: mareev.evgeniy@physics.msu.ru
Russian Federation, Moscow

D. N. Khmelenin

Shubnikov Institute of Crystallography of Kurchatov Complex of Crystallography and Photonics of NRC “Kurchatov Institute”

Email: mareev.evgeniy@physics.msu.ru
Russian Federation, Moscow

F. V. Potemkin

Lomonosov Moscow State University

Email: potemkin@physics.msu.ru

Faculty of Physics

Russian Federation, Moscow

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Supplementary files

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2. Fig. 1. Image of the region of action of the laser pulse on silicon, as well as Raman spectra in the frequency range of 250–475 cm−1: 1 – spectrum of undamaged silicon, 2 – spectrum of amorphous silicon, 3 – region where the peak characteristic of the Si-III phase at 430 cm−1 is recorded in the spectra, 4 – spectrum containing peaks of the Si-III and Si-XII phases, 5 – spectrum with nanosecond laser action on silicon. Rectangles in the microscopic image indicate the regions in which the corresponding spectra are measured.

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3. Fig. 2. TEM images of the laser-induced microcrater region: a – general view, dark areas on top are typical for amorphous silicon, oblique lines in the figures are lattice dislocations; b, c – enlarged areas marked with rectangles in Fig. a; g, d – electron diffraction patterns from areas marked with dots.

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4. Fig. 3. Visualization of the numerical simulation results – a cross-section of a 10 Å thick silicon sample along the laser pulse propagation axis (from left to right) (a): the brightness shows the atomic volume of the Si-I phases, compressed Si-I, Si-II and Si-XI, Si-III and Si-XII, and regions with lower density. The time delay for each image is indicated in the figure. Evolution of the dynamics of the rocking curve calculated for the near-surface region (b): the arrows indicate the peaks and atomic volumes characteristic of silicon phases other than Si-I.

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5. Fig. 4. Time dynamics of changes in the histogram of atomic volume distribution after laser exposure: a – three-dimensional heat map, b – histograms of atomic volume distribution for times of 2, 5, 10, 15, 20, 30 ps. The dashed line indicates the original histogram.

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6. Fig. 5. Schematic representation of the dynamics of laser-induced phase transitions in silicon.

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