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1.
Appl Opt ; 61(15): 4602-4609, 2022 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-36256303

RESUMO

By adopting self-injection locking (SIL) technology in an external injection locking (EIL) optoelectronic oscillator (OEO), a highly improved side mode suppression ratio (SMSR) and low phase noise microwave signal generator is designed. The EIL ranging is closely related to the frequency spacing ranging of the free-running OEO, which is the reverse of the oscillation loop length, and limits the phase noise performance. Here SIL technology is introduced to significantly increase the Q-factor of the OEO without degrading the SMSR by setting the longer loop without oscillation. Both the simulation and experimental results are carried out to confirm the conclusion. Additionally, an SMSR up to 86 dB and phase noises as low as -88.80dBc/Hz@100Hz and -122.83dBc/Hz@10kHz, respectively, are demonstrated. Furthermore, the frequency overlapping Allan deviation of the proposed OEO scheme is also enhanced by 103 times, which benefits from the external injection technology compared with the free-running OEO. In addition, the SMSR and phase noise modification dependence on the fiber length, the RF source quality and external injection power, as well as the frequency tunability, are detailed and discussed to reveal the compatibility combination mechanism of the EIL and the SIL.

2.
Phys Rev Lett ; 127(1): 017201, 2021 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-34270292

RESUMO

Sr_{2}CuTe_{0.5}W_{0.5}O_{6} is a square-lattice magnet with superexchange between S=1/2Cu^{2+} spins mediated by randomly distributed Te and W ions. Here, using sub-K temperature and 20 µeV energy resolution neutron scattering experiments we show that this system transits from a gapless disorder-induced spin liquid to a new quantum state below T_{f}=1.7(1) K, exhibiting a weak frozen moment of ⟨S⟩/S∼0.1 and low energy dynamic susceptibility, χ^{''}(ℏω), linear in energy which is surprising for such a weak freezing in this highly fluctuating quantum regime.

3.
Nano Lett ; 20(5): 3331-3337, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32202803

RESUMO

We report on the thermal conductivities of two-dimensional metal halide perovskite films measured by time domain thermoreflectance. Depending on the molecular substructure of ammonium cations and owing to the weaker interactions in the layered structures, the thermal conductivities of our two-dimensional hybrid perovskites range from 0.10 to 0.19 W m-1 K-1, which is drastically lower than that of their three-dimensional counterparts. We use molecular dynamics simulations to show that the organic component induces a reduction of the stiffness and sound velocities along with giving rise to vibrational modes in the 5-15 THz range that are absent in the three-dimensional counterparts. By systematically studying eight different two-dimensional hybrid perovskites, we show that the thermal conductivities of our hybrid films do not depend on the thicknesses of the organic layers and instead are highly dependent on the relative orientation of the organic chains sandwiched between the inorganic constituents.

4.
Inorg Chem ; 59(18): 13390-13397, 2020 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-32869627

RESUMO

Bi and Pb ions with charge degree of freedom depending on 6s2 and 6s0 electronic configurations were combined with the Mn ion in a perovskite oxide. Comprehensive theoretical and experimental investigations revealed the Bi3+0.5Pb2+0.5Mn3+0.5Mn4+0.5O3 charge ordered state with CE-type spin and dz2 orbital orderings as observed in La0.5Ca0.5MnO3, Nd0.5Sr0.5MnO3, and Bi0.5Sr0.5MnO3. The charge and orbital orderings were preserved above 500 K owing to the stereochemical activity of Bi3+ and Pb2+ ions which stabilized the structural distortion.

5.
J Chem Phys ; 152(1): 014703, 2020 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-31914767

RESUMO

The extended charge carrier lifetime in metal halide perovskites is responsible for their excellent optoelectronic properties. Recent studies indicate that the superb device performance in these materials is intimately related to the organic cation dynamics. Here, we focus on the investigation of the two-dimensional hybrid perovskite, (C8H17NH3)2PbI4 (henceforth, OA+ = C8H17NH3 +). Using elastic and quasielastic neutron scattering techniques and group theoretical analysis, we studied the structural phase transitions and rotational modes of the C8H17NH3 + cation in (OA)2PbI4. Our results show that, in the high-temperature orthorhombic (T > 310 K) phase, the OA+ cation exhibits a combination of a twofold rotation of the NH3-CH2 head group about the crystal c-axis with a characteristic relaxation time of ∼6.2 ps, threefold rotations (C3) of NH3 and CH3 terminal groups, and slow librations of the other atoms. Contrastingly, only the C3 rotation is present in the intermediate-temperature orthorhombic (238 K < T < 310 K) and low-temperature monoclinic (T < 238 K) phases.

6.
Proc Natl Acad Sci U S A ; 114(29): 7519-7524, 2017 07 18.
Artigo em Inglês | MEDLINE | ID: mdl-28673975

RESUMO

Long carrier lifetime is what makes hybrid organic-inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic-inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.


Assuntos
Compostos de Cálcio/química , Iodetos/química , Metais Pesados/química , Óxidos/química , Fotoquímica , Titânio/química , Elétrons , Luminescência , Nêutrons , Energia Solar , Luz Solar , Temperatura
7.
Phys Rev Lett ; 122(25): 257204, 2019 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-31347885

RESUMO

We report a new classical spin liquid in which the collective flux degrees of freedom break the translation symmetry of the honeycomb lattice. This exotic phase exists in the frustrated spin-orbit magnets where a dominant off-diagonal exchange, the so-called Γ term, results in a macroscopic ground-state degeneracy at the classical level. We demonstrate that the system undergoes a phase transition driven by thermal order by disorder at a critical temperature T_{c}≈0.04|Γ|. This transition reduces the emergent spherical spin symmetry to a cubic one: spins point predominantly toward the cubic axes, yet seem to remain disordered at T

8.
J Inorg Biochem ; 229: 111745, 2022 04.
Artigo em Inglês | MEDLINE | ID: mdl-35121188

RESUMO

A conservative characteristic of manganese superoxide dismutase is the rapid formation of product inhibition at high temperatures. At lower temperatures, the enzyme is less inhibited and undergoes more catalytic fast cycles before being product-inhibited. The temperature-dependent kinetics could be rationalized by the temperature-dependent coordination in the conserved center of manganese superoxide dismutase. As temperature decreases, a water molecule (WAT2) approaches or even coordinates Mn as the sixth ligand to interfere with O2•--Mn coordination and reduce product inhibition, so the dismutation should mainly proceed in the fast outer-sphere pathway at low temperatures. Cold-activation is an adaptive response to low temperature rather than a passive adaptation to excess superoxide levels since the cold-activated dismutase activity significantly exceeds the amount of superoxide in the cell or mitochondria. Physiologically speaking, cold activation of manganese superoxide dismutase mediates cold stress signaling and transduces temperature (physical signal) degree into H2O2 fluxes (chemical signal), which in turn may act as a second messenger to induce a series of physiological responses such as cold shock.


Assuntos
Superóxido Dismutase/metabolismo , Termorreceptores/metabolismo , Bactérias/enzimologia , Proteínas de Bactérias/química , Proteínas de Bactérias/metabolismo , Temperatura Baixa , Resposta ao Choque Frio/fisiologia , Proteínas Fúngicas/química , Proteínas Fúngicas/metabolismo , Fungos/enzimologia , Humanos , Peróxido de Hidrogênio/metabolismo , Manganês/química , Estresse Oxidativo/fisiologia , Conformação Proteica , Transdução de Sinais/fisiologia , Superóxido Dismutase/química , Superóxidos/química , Superóxidos/metabolismo , Termorreceptores/química
9.
Phys Rev E ; 104(6-1): 064105, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-35030869

RESUMO

We introduce an efficient dynamical tree method that enables us to explicitly demonstrate the thermoremanent magnetization memory effect in a hierarchical energy landscape. Our simulation nicely reproduces the nontrivial waiting-time and waiting-temperature dependences in this nonequilibrium phenomenon. We further investigate the condensation effect, in which a small set of microstates dominates the thermodynamic behavior in the multilayer trap model. Importantly, a structural phase transition of the multilayer tree model is shown to coincide with the onset of the condensation phenomenon. Our results underscore the importance of hierarchical structure and demonstrate the intimate relation between the glassy behavior and structure of barrier trees.

10.
Nat Commun ; 9(1): 1336, 2018 04 06.
Artigo em Inglês | MEDLINE | ID: mdl-29626205

RESUMO

Thin films based on two-dimensional metal halide perovskites have achieved exceptional performance and stability in numerous optoelectronic device applications. Simple solution processing of the 2D perovskite provides opportunities for manufacturing devices at drastically lower cost compared to current commercial technologies. A key to high device performance is to align the 2D perovskite layers, during the solution processing, vertical to the electrodes to achieve efficient charge transport. However, it is yet to be understood how the counter-intuitive vertical orientations of 2D perovskite layers on substrates can be obtained. Here we report a formation mechanism of such vertically orientated 2D perovskite in which the nucleation and growth arise from the liquid-air interface. As a consequence, choice of substrates can be liberal from polymers to metal oxides depending on targeted application. We also demonstrate control over the degree of preferential orientation of the 2D perovskite layers and its drastic impact on device performance.

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