Ultrafast light induced unusually broad transient absorption in the sub-bandgap region of GeSe2 thin film.
Ontology highlight
ABSTRACT:
SUBMITTER: Barik AR
PROVIDER: S-EPMC3890940 | biostudies-other | 2014
REPOSITORIES: biostudies-other
Similar Datasets
Project description:The light-matter interaction in materials is of remarkable interest for various photonic and optoelectronic applications, which is intrinsically determined by the bandgap of the materials involved. To extend the applications beyond the bandgap limit, it is of great significance to study the light-matter interaction below the material bandgap. Here, we report the ultrafast transient absorption of monolayer molybdenum disulfide in its sub-bandgap region from ~0.86 µm to 1.4 µm. Even though this spectral range is below the bandgap, we observe a significant absorbance enhancement up to ~4.2% in the monolayer molybdenum disulfide (comparable to its absorption within the bandgap region) due to pump-induced absorption by the excited carrier states. The different rise times of the transient absorption at different wavelengths indicate the various contributions of the different carrier states (i.e., real carrier states in the short-wavelength region of ~<1 µm, and exciton states in the long wavelength region of ~>1 µm). Our results elucidate the fundamental understanding regarding the optical properties, excited carrier states, and carrier dynamics in the technologically important near-infrared region, which potentially leads to various photonic and optoelectronic applications (e.g., excited-state-based photodetectors and modulators) of two-dimensional materials and their heterostructures beyond their intrinsic bandgap limitations.
| S-EPMC7846580 | biostudies-literature
Project description:The trade-off between light absorption and carrier transport in semiconductor thin film photoelectrodes is a major limiting factor of their solar-to-hydrogen efficiency for photoelectrochemical water splitting. Herein, we develop a heterogeneous doping strategy that combines surface doping with bulk gradient doping to decouple light absorption and carrier transport in a thin film photoelectrode. Taking La and Mg doped Ta3N5 thin film photoanode as an example, enhanced light absorption is achieved by surface La doping through alleviating anisotropic optical absorption, while efficient carrier transport in the bulk is maintained by the gradient band structure induced by gradient Mg doping. Moreover, the homojunction formed between the La-doped layer and the gradient Mg-doped layer further promotes charge separation. As a result, the heterogeneously doped photoanode yields a half-cell solar-to-hydrogen conversion efficiency of 4.07%, which establishes Ta3N5 as a leading performer among visible-light-responsive photoanodes. The heterogeneous doping strategy could be extended to other semiconductor thin film light absorbers to break performance trade-offs by decoupling light absorption and carrier transport.
| S-EPMC9755297 | biostudies-literature
Project description:In this article, we report the first observation of nanosecond laser induced transient dual absorption bands, one in the bandgap (TA₁) and another in the sub-bandgap (TA₂) regions of a-Ge₅As₃₀Se₆₅ thin films. Strikingly, these bands are thermally tunable and exhibit a unique contrasting characteristic: the magnitude of TA₁ decreases while that of TA₂ increases with increasing temperature. Further, the decay kinetics of these bands is strongly influenced by the temperature, which signifies a strong temperature dependent exciton recombination mechanism. The induced absorption shows quadratic and the decay time constant shows linear dependence on the laser beam fluence.
| S-EPMC4192641 | biostudies-other
Project description:The efficiency of perovskite solar cells has surged in the past few years, while the bandgaps of current perovskite materials for record efficiencies are much larger than the optimal value, which makes the efficiency far lower than the Shockley-Queisser efficiency limit. Here we show that utilizing the below-bandgap absorption of perovskite single crystals can narrow down their effective optical bandgap without changing the composition. Thin methylammonium lead triiodide single crystals with tuned thickness of tens of micrometers are directly grown on hole-transport-layer covered substrates by a hydrophobic interface confined lateral crystal growth method. The spectral response of the methylammonium lead triiodide single crystal solar cells is extended to 820?nm, 20?nm broader than the corresponding polycrystalline thin-film solar cells. The open-circuit voltage and fill factor are not sacrificed, resulting in an efficiency of 17.8% for single crystal perovskite solar cells.
| S-EPMC5709415 | biostudies-other
Project description:Transient absorption spectra (TAS) of lead halide perovskites can provide important insights into the nature of the photoexcited state dynamics of this prototypical class of materials. Here, we perform ground and excited state molecular dynamics (MD) simulations within a restricted open shell Kohn-Sham (ROKS) approach in order to interpret the characteristic features of the TAS of CsPbBr3 . Our results reveal that properties such as the finite temperature band gap, the Stokes shift, and therefore, also the TAS are strongly size-dependent. Our TAS simulations show an early positive red-shifted feature on the fs scale that can be explained by geometric relaxation in the excited state. As excited-state processes can crucially affect the electronic properties of this class of photoactive materials, our observations are an important ingredient for further optimization of lead halide based optoelectronic devices.
| S-EPMC9305422 | biostudies-literature
Project description:Recently rediscovered black phosphorus is a layered semiconductor with promising electronic and photonic properties. Dynamic control of its bandgap can allow for the exploration of new physical phenomena. However, theoretical investigations and photoemission spectroscopy experiments indicate that in its few-layer form, an exceedingly large electric field in the order of several volts per nanometre is required to effectively tune its bandgap, making the direct electrical control unfeasible. Here we reveal the unique thickness-dependent bandgap tuning properties in intrinsic black phosphorus, arising from the strong interlayer electronic-state coupling. Furthermore, leveraging a 10 nm-thick black phosphorus, we continuously tune its bandgap from ∼300 to below 50 meV, using a moderate displacement field up to 1.1 V nm-1. Such dynamic tuning of bandgap may not only extend the operational wavelength range of tunable black phosphorus photonic devices, but also pave the way for the investigation of electrically tunable topological insulators and semimetals.
| S-EPMC5399305 | biostudies-literature
Project description:The charge separation/transport efficiency is relatively high in thin-film hematite photoanodes in which the distance for charge transport is short, but simultaneously the high loss of light absorption due to transmission is confronted. To increase light absorption in thin-film Fe2O3:Ti, commercial substrates such as Cu foil, Ag foil, and a mirror are adopted acting as back-reflectors and individually integrated with the Fe2O3:Ti electrode. The promotion effect of the commercial back-reflectors on the light absorption efficiency and photoelectrochemical (PEC) performance of the hydrothermally prepared Fe2O3:Ti electrodes with a variety of film thicknesses is investigated. As a result, Ag foil and the mirror show favorable and equal efficacy while the promoting effect of Cu foil is limited. In addition, the photocurrent increment achieved by the Ag back-reflector decreases linearly along with the logarithmic of the film thickness and the optimized film thickness of the Fe2O3:Ti electrode is decreased from 520 to 290 nm. The high durability of Ag foil in the alkaline electrolyte during solar light irradiation is demonstrated. Furthermore, the reflective substrate also shows a promotion effect on the BiVO4 photoanode and CuBi2O4 photocathode, as well as the unbiased photocurrent from a tandem cell constituted by TiO2 and CuBi2O4.
| S-EPMC9031256 | biostudies-literature
Project description:The competition between different spatiotemporal carrier relaxation determines the carrier harvesting in optoelectronic semiconductors, which can be greatly optimized by utilizing the ultrafast spatial expansion of highly energetic carriers before their energy dissipation via carrier-phonon interactions. Here, the excited-state dynamics in layered tungsten disulfide (WS2 ) are primarily imaged in the temporal, spatial, and spectral domains by transient absorption microscopy. Ultrafast hot carrier expansion is captured in the first 1.4 ps immediately after photoexcitation, with a mean diffusivity up to 980 cm2 s-1 . This carrier diffusivity then rapidly weakens, reaching a conventional linear spread of 10.5 cm2 s-1 after 2 ps after the hot carriers cool down to the band edge and form bound excitons. The novel carrier diffusion can be well characterized by a cascaded transport model including 3D thermal transport and thermo-optical conversion, in which the carrier temperature gradient and lattice thermal transport govern the initial hot carrier expansion and long-term exciton diffusion rates, respectively. The ultrafast hot carrier expansion breaks the limit of slow exciton diffusion in 2D transition metal dichalcogenides, providing potential guidance for high-performance applications and thermal management of optoelectronic technology.
| S-EPMC8981895 | biostudies-literature
Project description:Understanding the mechanism of charge dynamics in photocatalysts is the key to design and optimize more efficient materials for renewable energy applications. In this study, the charge dynamics of a CuO thin film are unraveled via transient absorption spectroscopy (TAS) on the picosecond to microsecond timescale for three different excitation energies, i.e., above, near, and below the band gap, to explore the role of incoherent broadband light sources. The shape of the ps-TAS spectra changes with the delay time, while that of the ns-TAS spectra is invariant for all the excitation energies. Regardless of the excitations, three time constants, τ1 ∼ 0.34-0.59 ps, τ2 ∼ 162-175 ns, and τ3 ∼ 2.5-3.3 μs, are resolved, indicating the dominating charge dynamics at very different timescales. Based on these observations, the UV-vis absorption spectrum, and previous findings in the literature, a compelling transition energy diagram is proposed. Two conduction bands and two defect (deep and shallow) states dominate the initial photo-induced electron transitions, and a sub-valence band energy state is involved in the subsequent transient absorption. By solving the rate equations for the pump-induced population dynamics and implementing the assumed Lorentzian absorption spectral shape between two energy states, the TAS spectra are modeled which capture the main spectral and time-dependent features for t > 1 ps. By further considering the contributions from free-electron absorption during very early delay times, the modeled spectra reproduce the experimental spectra very well over the entire time range and under different excitation conditions.
| S-EPMC10103062 | biostudies-literature
Project description:Ultrashort light pulses induce rapid deformations of crystalline lattices. In ferroelectrics, lattice deformations couple directly to the polarization, which opens the perspective to modulate the electric polarization on an ultrafast time scale. Here, we report on the temporal and spatial tracking of strain and polar modulation in a single-domain BiFeO3 thin film by ultrashort light pulses. To map the light-induced deformation of the BiFeO3 unit cell, we perform time-resolved optical reflectivity and time-resolved x-ray diffraction. We show that an optical femtosecond laser pulse generates not only longitudinal but also shear strains. The longitudinal strain peaks at a large amplitude of 0.6%. The access of both the longitudinal and shear strains enables to quantitatively reconstruct the ultrafast deformation of the unit cell and to infer the corresponding reorientation of the ferroelectric polarization direction in space and time. Our findings open new perspectives for ultrafast manipulation of strain-coupled ferroic orders.
| S-EPMC10651133 | biostudies-literature