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1.
Phys Rev Lett ; 132(4): 046302, 2024 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-38335369

RESUMO

We present an investigation into the vertical transport through 13 different superlattice structures, where the well and barrier widths, doping concentration, dopant position, and contact layers were varied. Although superlattices have been extensively studied since 1970, there is a lack of publications on transport through superlattices similarly low doped as THz quantum cascade lasers (QCLs), for which the doping is in the 3-5×10^{10} cm^{-2} range. The superlattices presented are doped in the same range as THz QCLs, with contact layers and fabrication comparable to high-temperature THz QCLs. The temperature-dependent current-voltage characteristics were measured starting from 5 K and an anomalous temperature effect was observed at the first plateau. The measured current through the superlattice first decreases before increasing again with increasing temperature, resulting in the lowest current occurring at 75-110 K. This behavior is also observed in some THz QCLs. The effect disappears for thinner barriers, higher quantum well doping, or modified contact layers, indicating a strong dependency on band bending, due to the large difference in the doping of the contact layers and the superlattice, which is confirmed with multiscattering Büttiker simulations.

2.
Opt Express ; 27(15): 20688-20693, 2019 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-31510157

RESUMO

We demonstrate the first lasing emission of a thermo-electrically cooled terahertz quantum cascade laser (THz QCL). A high temperature three-well THz QCL emitting at 3.8 THz is mounted to a novel five-stage thermoelectric cooler reaching a temperature difference of ΔT = 124 K. The temperature and time-dependent laser performance is investigated and shows a peak pulse power of 4.4 mW and a peak average output power of 100 µW for steady-state operation.

3.
Opt Express ; 24(22): 25462-25470, 2016 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-27828484

RESUMO

We demonstrate a convenient and fast method to measure the spectrally resolved far-fields of multimode terahertz quantum cascade lasers by combining a microbolometer focal plane array with an FTIR spectrometer. Far-fields of fundamental TM0 and higher lateral order TM1 modes of multimode Fabry-Pérot type lasers have been distinguished, which very well fit to the results obtained by a 3D finite-element simulation. Furthermore, multimode random laser cavities have been investigated, analyzing the contribution of each single laser mode to the total far-field. The presented method is thus an important tool to gain in-depth knowledge of the emission properties of multimode laser cavities at terahertz frequencies, which become increasingly important for future sensing applications.

4.
J Phys Chem Lett ; 7(14): 2742-7, 2016 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-27352138

RESUMO

The proton transfer reaction H3(+) + CO is one of the cornerstone chemical processes in the interstellar medium. Here, the dynamics of this reaction have been investigated using crossed beam velocity map imaging. Formyl product cations are found to be predominantly scattered into the forward direction irrespective of the collision energy. In this process, a high amount of energy is transferred to internal product excitation. By fitting a sum of two distribution functions to the measured internal energy distributions, the product isomer ratio is extracted. A small HOC(+) fraction is obtained at a collision energy of 1.8 eV, characterized by an upper limit of 24% with a confidence level of 84%. At lower collision energies, the data indicate purely HCO(+) formation. Such low values are unexpected given the previously predicted efficient formation of both HCO(+) and HOC(+) isomers for thermal conditions. This is discussed in light of the direct reaction dynamics that are observed.

5.
Nat Chem ; 8(2): 151-6, 2016 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-26791898

RESUMO

In addition to the nucleophile and solvent, the leaving group has a significant influence on SN2 nucleophilic substitution reactions. Its role is frequently discussed with respect to reactivity, but its influence on the reaction dynamics remains unclear. Here, we uncover the influence of the leaving group on the gas-phase dynamics of SN2 reactions in a combined approach of crossed-beam imaging and dynamics simulations. We have studied the reaction F(-) + CH3Cl and compared it to F(-) + CH3I. For the two leaving groups, Cl and I, we find very similar structures and energetics, but the dynamics show qualitatively different features. Simple scaling of the leaving group mass does not explain these differences. Instead, the relevant impact parameters for the reaction mechanisms are found to be crucial and the differences are attributed to the relative orientation of the approaching reactants. This effect occurs on short timescales and may also prevail in solution-phase conditions.

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