Femtosecond and Ultraviolet Laser Irradiation of Graphite-Like Hexagonal Boron Nitride

Effect of the femtosecond and nanosecond UV laser irradiation (below the ablation threshold) of graphite-like hexagonal boron nitride (hBN) has been studied. Experiments were carried out with the compacted powder under high vacuum at room temperature using excimer KrF laser (248 nm). In the nanosecond operation mode, the laser-induced fluorescence spectra are found strongly modified depending on the integrated doze, which is attributed to a progressive enrichment of the surface layer by elemental boron. A slow sample recovery after the laser irradiation has been observed. On the other hand, in the femtosecond mode the fluorescence spectra depend on the laser fluence, and the changes are reversible: low energy fluorescence spectra are restored immediately when the laser energy decreases. This effect can be explained by a material bleaching, which favors a bulk centers emission. The ablation threshold has been determined as 78 mJ/cm2 in the femtosecond laser operational mode

Coherent phonons and the interplay between charge density wave and Mott phases in 1TT-TaSe2_{2}

1$T$-TaSe$_{2}$ is host to coexisting strongly-correlated phases including charge density waves (CDWs) and an unusual Mott transition at low temperature. Here, we investigate coherent phonon oscillations in 1$T$-TaSe$_{2}$ using a combination of time- and angle-resolved photoemission spectroscopy (TR-ARPES) and time-resolved reflectivity (TRR). Perturbation by a femtosecond laser pulse triggers a modulation of the valence band binding energy at the $\Gamma$-point, related to the Mott gap, that is consistent with the in-plane CDW amplitude mode frequency. By contrast, TRR measurements show a modulation of the differential reflectivity comprised of multiple frequencies belonging to the distorted CDW lattice modes. Comparison of the temperature dependence of coherent and spontaneous phonons across the CDW transition shows that the amplitude mode intensity is more easily suppressed during perturbation of the CDW state by the optical excitation compared to other modes. Our results clearly identify the relationship of the in-plane CDW amplitude mode with the Mott phase in 1$T$-TaSe$_{2}$ and highlight the importance of lattice degrees of freedom.Comment: 7 pages, 4 figures, supplemental materia

Enhanced generation of VUV radiation by four-wave mixing in mercury using pulsed laser vaporization

The efficiency of a coherent VUV source at 125 nm, based on 2-photon resonant four-wave mixing in mercury vapor, has been enhanced by up to 2 orders of magnitude. This enhancement was obtained by locally heating a liquid Hg surface with a pulsed excimer laser, resulting in a high density vapor plume in which the nonlinear interaction occurred. Energies up to 5 μJ (1 kW peak power) have been achieved while keeping the overall Hg cell at room temperature, avoiding the use of a complex heat pipe. We have observed a strong saturation of the VUV yield when peak power densities of the fundamental beams exceed the GW/cm2 range, as well as a large intensity-dependant broadening (up to ~30 cm-1) of the two-photon resonance. The source has potential applications for high resolution interference lithography and photochemistry

Interface Excitons in Krmnen Clusters : The Role of Electron Affinity in the Formation of Electronic Structure

The formation of the electronic structure of small Kr_m clusters (m<150) embedded inside Ne_N clusters (1200<N<7500) has been investigated with the help of fluorescence excitation spectroscopy using synchrotron radiation. Electronically excited states, assigned to excitons at the Ne/Kr interface, 1i and 1'i were observed. The absorption bands, which are related to the lowest spin-orbit split atomic Kr 3P1 and 1P1 states, initially appear and shift towards lower energy when the krypton cluster size m increases. The characteristic bulk 1t and 1't excitons appear in the spectra, when the cluster radius exceeds some critical value, R_cl>Delta_1i . Kr clusters comprising up to 70 atoms do not exhibit bulk absorption bands. We suggest that this is due to the penetration of the interface excitons into the Kr_m cluster volume, because of the negative electron affinity of surrounding Ne atoms. From the energy shift of the interface absorption bands with cluster size an unexpectedly large penetration depth of delta_1i =7.0+/-0.1 A is estimated, which can be explained by the interplay between the electron affinities of the guest and the host cluster

Near band-gap electronics properties and luminescence mechanisms of boron nitride nanotubes

The deep ultraviolet luminescence (hν ≥ 5 eV) of multiwall boron nitride nanotubes (BNNTs) is studied with time- and energy-resolved photoluminescence spectroscopy. Two luminescence bands are observed at 5.35 and 5.54 eV. Both emissions undergo a large blue shift of several tens of meV with a linear slope ΔE$_{lum}$/ΔE$_{exc}$  < 1 as the excitation energy E$_{exc}$ increases. When E$_{exc}$ ≥5.8 eV, the spectral band positions become fixed, which marks the transition between the excitation of donor-acceptor pairs and creation of free charge carriers. We assign the 5.35 eV band to quasi donor-acceptor pair transitions and the band at 5.54 eV to free-bound transitions. Boron and nitrogen atoms distributed along characteristic defect lines in BNNTs should be involved in the luminescence process. The presented results permit a revision of previous assignments of electronic transitions in BNNTs

Near band gap photoluminescence properties of hexagonal boron nitride

Near band-gap luminescence (hnu > 5 eV) of hexagonal boron nitride has been studied by means of the time- and energy-resolved photoluminescence spectroscopy method. Two emissions have been observed at 5.5 eV and 5.3 eV. The high-energy emission at 5.5 eV is composed of fixed sub-bands assigned to bound excitons at 5.47 eV, 5.56 eV and 5.61 eV. The non-structured low-energy emission at 5.3 eV undergoes a large blue shift (up to 120 meV) with a linear slope 5.7 eV, the band position is fixed and marks the transition from the Raman to the photoluminescence regime. We assign the 5.3 eV band to quasi donor-acceptor pair (q-DAP) states due to electrostatic band fluctuations induced by charged defects. The shift is explained by photo-induced neutralization of charged defect states. The absence of contribution to the q-DAP luminescence from exciton suggests the existence of a large exciton binding energy, which is qualitatively consistent with theoretical predictions.Comment: accepted for publicatio