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1.
J Phys Condens Matter ; 33(31)2021 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-34030152

RESUMO

The relaxation of excited carriers in α-Al2O3is complex, depending for instance on the type of ionizing radiation. Using femtosecond time-resolved absorption spectroscopy, we can induce a controllable excitation density on a wide range, and follow the relaxation dynamics from 30 fs to 7 ns. We show that the excited carrier decay is non-exponential: it is dependent on the pump intensity, i.e. on the initial carrier concentration. We describe the relaxation as a two-steps process, involving the trapping of initially free electron-hole pairs, followed by recombination. A numerical model taking into account the initial electronic excitation by multiphoton absorption and the subsequent relaxation allows to quantitatively reproduce the amplitude of the measured absorption and its temporal evolution.

2.
Sci Rep ; 11(1): 6859, 2021 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-33767209

RESUMO

Unabated, worldwide trends in CO2 production project growth to > 43-BMT per year over the next two decades. Efficient power electronics are crucial to fully realizing the CO2 mitigating benefits of a worldwide smart grid (~ 18% reduction for the United States alone). Even state-of-the-art SiC high voltage junction devices are inefficient because of slow transition times (~ 0.5-µs) and limited switching rates at high voltage (~ 20-kHz at ≥ 15-kV) resulting from the intrinsically limited charge carrier drift speed (< 2 × 107-cm-s-1). Slow transition times and limited switch rates waste energy through transition loss and hysteresis loss in external magnetic components. Bulk conduction devices, where carriers are generated and controlled nearly simultaneously throughout the device volume, minimize this loss. Such devices are possible using below bandgap excitation of semi-insulating (SI) SiC single crystals. We explored carrier dynamics with a 75-fs single wavelength pump/supercontinuum probe and a modified transient spectroscopy technique and also demonstrated a new class of efficient, high-speed, high-gain, bi-directional, optically-controlled transistor-like power device. At a performance level six times that of existing devices, for the first time we demonstrated prototype operation at multi-10s of kW and 20-kV, 125-kHz in a bulk conduction transistor-like device using direct photon-carrier excitation with below bandgap light.

3.
Phys Chem Chem Phys ; 20(13): 8640-8646, 2018 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-29537023

RESUMO

Transient absorption studies conducted on in vitro lycopene aggregates, as well as on lycopene crystalloids inside tomato chromoplasts, reveal the appearance of a long-lived excited state, which we unambiguously identified as lycopene triplet. These triplet states must be generated by singlet exciton fission, which occurs from the lycopene 2Ag state. This is the first time the singlet fission process has ever been shown to occur in a biological material. We propose that the formation of carotenoid assemblies in chromoplasts may constitute a photoprotective process during chromoplast maturation, in addition to their function in signaling processes.


Assuntos
Carotenoides/química , Plastídeos/metabolismo , Solanum lycopersicum/química , Soluções Cristaloides , Soluções Isotônicas , Licopeno , Solanum lycopersicum/metabolismo , Plastídeos/química
4.
Phys Chem Chem Phys ; 17(27): 17828-37, 2015 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-26087921

RESUMO

Since the introduction of photochromic indolo-benzoxazines, difference absorption of these photoexcited compounds has been assigned to the ground state of the ring-opened isomer. This assignment relies on the alleged resemblance of the spectra of photo- and chemically induced forms. In this paper, we expose the issue of the discrepancy between the absorption spectra of photoproducts and the corresponding chemically opened forms. As a result, a substantial change in the current explanation of photodynamics of photochromic oxazines is proposed. The spectral features earlier ascribed to the photoproduct are suggested to arise due to the absorption of the triplet state. This hypothesis was tested and confirmed in acetonitrile by measuring the effect of oxygen quenching of photoproduct states. In view of this interpretation, light-induced ring opening does not occur in indolo-benzoxazines dissolved in acetonitrile, and, consequently these molecules should no longer be regarded as molecular switches. On the other hand, we show that methanol solution under UV light does produce small amounts of ring-opened form of the molecule.

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