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1.
J Phys Chem Lett ; 14(41): 9357-9364, 2023 Oct 19.
Article in English | MEDLINE | ID: mdl-37820389

ABSTRACT

We study structural and morphological transformations caused by multipulse femtosecond-laser exposure of Bridgman-grown ϵ-phase GaSe crystals, a van der Waals semiconductor promising for nonlinear optics and optoelectronics. We unveil, for the first time, the laser-driven self-organization regimes in GaSe allowing the formation of regular laser-induced periodic surface structures (LIPSSs) that originate from interference of the incident radiation and interface surface plasmon waves. LIPSSs formation causes transformation of the near-surface layer to amorphous Ga2Se3 at negligible oxidation levels, evidenced from comprehensive structural characterization. LIPSSs imprinted on both output crystal facets provide a 1.2-fold increase of the near-IR transmittance, while the ability to control local periodicity by processing parameters enables multilevel structural color marking of the crystal surface. Our studies highlight direct fs-laser patterning as a multipurpose application-ready technology for precise nanostructuring of promising van der Waals semiconductors, whose layered structure restricts application of common nanofabrication approaches.

2.
Phys Chem Chem Phys ; 16(45): 24884-91, 2014 Dec 07.
Article in English | MEDLINE | ID: mdl-25322208

ABSTRACT

Ba5(BO3)3F single crystals of high optical quality and up to 1.5 cm in diameter were grown. Its transparency range is 0.23 to 6.6 µm (on 10% level). Direct allowed electronic transitions at the Γ-point give band gap values of 5.31 and 5.40 eV at 300 and 80 K, respectively. Luminescence is excited in the near-edge absorption bands near 265 and 365 nm. X-ray irradiation induces an additional absorption in dominant 252, 317 and 710 nm bands. Combined electron spin-resonance spectroscopy and theoretical analysis allow one to associate the three absorption peaks with O(5-), O(1-) and e6(-) (fluorine vacancy), respectively. The original transparency is restored after heating the crystal to 400 K and charge carrier release from traps with ET = 0.87 eV and s = 10(12) s(-1). Dispersion curves for the refractive indices were calculated and Sellmeier equations were built. Theoretical analysis shows strong localization of the Ba 5s and F 2s orbitals, strong ionicity of the Ba cations and strong covalency of the B-O bond. The optical properties of Ba5(BO3)3F are dominantly determined by electron transitions within the (BO3)(3-) groups, despite the transition between barium and oxygen also having a little contribution.

3.
Opt Lett ; 26(9): 617-9, 2001 May 01.
Article in English | MEDLINE | ID: mdl-18040401

ABSTRACT

Phase-matched second-harmonic generation is obtained in various LiInS(2) crystals by use of the tunable picosecond output of the free-electron laser for infrared experiments (FELIX) as the pump source in the mid-IR range from 2.75 to 6.0 microm. Deviations from the phase-matching curve calculated from Boyd's refractive-index data are observed. Furthermore, the optical damage threshold of the crystals has been measured to be 1.1. J/cm(2)(>6 GW/cm(2)) at the 5-microm wavelength. LiInS(2) holds great promise for parametric interaction in the 1-13-microm range.

4.
Article in English | MEDLINE | ID: mdl-18238574

ABSTRACT

We report on the improvement of a tunable, high resolution, diode laser-based, difference-frequency spectrometer using an AgGaS(2) nonlinear crystal. We use a type-II cut crystal as a part of the improvement compared with a type-I cut, which was used in our preliminary setup. The two tunable laser-diodes are operating near lambda(3)=778 nm (pump) and lambda(2)=842 nm (signal) with a sub-100-kHz linewidth. The high resolution spectrometer is being developed as an alternative to CO(2) laser spectrometers in the 9- to Il-mum range. Using a dual-arm cavity to enhance the two radiation powers, and with 35 mW in front of the 778-nm arm and 100 mW in front of the 842 nm arm, about 70 nW of the tunable 10-mum radiation are generated. This power level is enough to investigate the linear absorption spectroscopy of SF(6). Doppler-limited spectra over 2 GHz, are recorded, showing the wide continuous tunability of the spectrometer.

5.
Article in English | MEDLINE | ID: mdl-18238651

ABSTRACT

Frequency divide-by-two (2:1) and divide-by-three (3:1) optical parametric oscillators (OPOs) are basic devices for the implementation of future accurate optical frequency division chains. We report our latest development toward a phase-locked 3:1 frequency division of a radiation at lambda(p) approximately 843 nm (355.9 THz), using doubly resonant oscillators (DROs) based on silver gallium sulfide (AgGaS(2 ) or AGS) and multigrating periodically poled lithium niobate (PPLN). Although stable single-mode pair operation is achievable without any active cavity length servo with the AGS-DRO, because of a strong passive thermal feedback servo, the PPLN-DRO requires an active intensity side-of-fringe locking servo to maintain long-term, single-mode pair operation. To overcome the limited idler output power (<1 mW) due to the weak mirror transmissivity at 2.53 mum, a CaF (2) Brewster-oriented plate was inserted in a longer-cavity PPLN-DRO as a variable output coupler. About 3 mW of idler wave is thus coupled outside the cavity, yielding 15 nW of doubled-idler. We obtained a 30 dB signal-to-noise ratio beatnote in a 100 kHz resolution bandwidth of a spectrum analyser. This beat signal will be used to phase-lock the divider.

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