| 1. |
- An, Rui, et al.
(författare)
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Photostability and Photodegradation Processes in Colloidal CsPbI3 Perovskite Quantum Dots
- 2018
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 10:45, s. 39222-39227
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Tidskriftsartikel (refereegranskat)abstract
- All-inorganic CsPbI3 perovskite quantum dots (QDs) have attracted intense attention for their successful application in photovoltaics (PVs) and optoelectronics that are enabled by their superior absorption capability and great photoluminescence (PL) properties. However, their photostability remains a practical bottleneck and further optimization is highly desirable. Here, we studied the photostability of as-obtained colloidal CsPbI3 QDs suspended in hexane. We found that light illumination does induce photodegradation of CsPbI3 QDs. Steady-state spectroscopy, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and transient absorption spectroscopy verified that light illumination leads to detachment of the capping agent, collapse of the CsPbI3 QD surface, and finally aggregation of surface Pb0. Both dangling bonds containing surface and Pb0 serve as trap states causing PL quenching with a dramatic decrease of PL quantum yield. Our work provides a detailed insight about the correlation between the structural and photophysical consequences of the photodegradation process in CsPbI3 QDs and may lead to the optimization of such QDs toward device applications.
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| 2. |
- Becker, Christiane, et al.
(författare)
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Nanophotonic-Enhanced Two-Photon-Excited Photoluminescence of Perovskite Quantum Dots
- 2018
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 5:11, s. 4668-4676
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Tidskriftsartikel (refereegranskat)abstract
- All-inorganic CsPbBr3 perovskite colloidal quantum dots have recently emerged as a promising material for a variety of optoelectronic applications, among others for multiphoton-pumped lasing. Nevertheless, high irradiance levels are generally required for such multiphoton processes. One strategy to enhance the multiphoton absorption is taking advantage of high local light intensities using photonic nanostructures. Here, we investigate two-photon-excited photoluminescence of CsPbBr3 perovskite quantum dots on a silicon photonic crystal slab. By systematic excitation of optical resonances using a pulsed near-infrared laser beam, we observe an enhancement of two-photon-pumped photoluminescence by more than 1 order of magnitude when comparing to using a bulk silicon film. Experimental and numerical analyses allow relating these findings to near-field enhancement effects on the nanostructured silicon surface. The results reveal a promising approach for significantly decreasing the required irradiance levels for multiphoton processes being of advantage in applications such as biomedical imaging, lighting, and solar energy.
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| 3. |
- Chen, Junsheng, et al.
(författare)
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Evidence of High-Order Nonlinearities in Supercontinuum White-Light Generation from a Gold Nanofilm
- 2018
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 5:5, s. 1927-1932
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Tidskriftsartikel (refereegranskat)abstract
- White-light supercontinuum generation can be readily observed when gold nanostructures are irradiated with short pulses of light. It is believed that the nanostructures enhance the optical fields, which facilitates the supercontinuum white-light generation from the surrounding environment or the substrate. Here, we investigate the different nonlinear processes that contribute to the generation of the supercontinuum from plasmonic nanostructures themselves using a technique that isolates the different nonlinear contributions. By exciting a gold nanofilm with a pair of frequency shifted optical frequency combs, we demonstrate multiple modulation frequencies in the supercontinuum. Their dependence on the excitation intensity reveals that the supercontinuum originates from different orders of nonlinear light-matter interactions. This contrasts with the supercontinuum generation by a cascaded third-order optical nonlinear response in traditional dielectric-based white-light sources. The while-light emission from the gold nanofilm is efficient even under relatively weak excitation indicating that nonlocal effects in nanostructures may facilitate the supercontinuum generation by adding new pathways in the nonlinear interactions. The results provide experimental basis for the understanding of the collective nonlinear response of free-electrons in the metallic nanostructures and associated nonlinear processes, which are crucial in development of nonlinear metasurfaces and nanophotonic devices.
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| 4. |
- Finkelstein-Shapiro, Daniel, et al.
(författare)
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Two-dimensional Fano lineshapes : Excited-state absorption contributions
- 2018
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 148:18
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Tidskriftsartikel (refereegranskat)abstract
- Fano interferences in nanostructures are influenced by dissipation effects as well as many-body interactions. Two-dimensional coherent spectroscopies have just begun to be applied to these systems where the spectroscopic signatures of a discrete-continuum structure are not known. In this article, we calculate the excited-state absorption contribution for different models of higher lying excited states. We find that the characteristic asymmetry of one-dimensional spectroscopies is recovered from the many-body contributions and that the higher lying excited manifolds have distorted lineshapes that are not anticipated from discrete-level Hamiltonians. We show that the Stimulated Emission cannot have contributions from a flat continuum of states. This work completes the Ground-State Bleach and Stimulated Emission signals that were calculated previously [D. Finkelstein-Shapiro et al., Phys. Rev. B 94, 205137 (2016)]. The model reproduces the observations reported for molecules on surfaces probed by 2DIR.
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| 5. |
- Ghosh, Supriya, et al.
(författare)
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Phonon Coupling with Excitons and Free Carriers in Formamidinium Lead Bromide Perovskite Nanocrystals
- 2018
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Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 9:15, s. 4245-4250
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Tidskriftsartikel (refereegranskat)abstract
- Organometal halide perovskites in the form of nanocrystals (NCs) have attracted enormous attention due to their unique optoelectronic and photoluminescence (PL) properties. Here, we examine the phase composition and the temperature dependence of emission line width broadening in formamidinium lead bromide (FAPbBr3) perovskite nanocrystals (NCs) for light-emitting applications and identify different charge-carrier scattering mechanisms. Our results show most of the emission is from the orthorhombic phase. The PL line width broadening at high temperature is dominated by the Fröhlich interaction between the free charge carriers and the optical phonons. At low temperatures, the peak of the PL spectrum exhibits a continuous red shift indicating an increase of excitons contribution at lower temperatures, and concurrently the line width also narrows down due to the inhibition of the optical phonons. From the temperature-dependent measurements, the coupling strength of both the charge phonon interaction and the exciton phonon interaction have been determined. The obtained results indicate that the charge phonon coupling strengths are higher compared to the exciton phonon coupling.
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| 6. |
- Mostovyi, Andrii I., et al.
(författare)
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Physical properties of the heterojunction MoOx/n-CdTe as a function of the parameters of CdTe crystals
- 2018
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Ingår i: Thirteenth International Conference on Correlation Optics. - : SPIE. - 9781510617278 ; 10612
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Konferensbidrag (refereegranskat)abstract
- MoOx/n-CdTe photosensitive heterostructures were prepared by the deposition of molybdenum oxide thin films onto three different n-type CdTe substrates (ρ1=0.4 Ωfirst>cm, ρ2=10 Ωfirst>cm, ρ3=40 Ωfirst>cm) by DC reactive magnetron sputtering. The height of the potential barrier and series resistance of the MoOx/CdTe heterojunctions were investigated. The dominating current transport mechanisms through the heterojunctions were determined at forward and reverse biases.
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| 7. |
- Schröter, Marco, et al.
(författare)
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Using fluorescence detected two-dimensional spectroscopy to investigate initial exciton delocalization between coupled chromophores
- 2018
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 149:11
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Tidskriftsartikel (refereegranskat)abstract
- Förster theory describes electronic exciton energy migration in molecular assemblies as an incoherent hopping process between donor and acceptor molecules. The rate is expressed in terms of the overlap integral between donor fluorescence and acceptor absorption spectra. Typical time scales for systems like photosynthetic antennae are on the order of a few picoseconds. Prior to transfer, it is assumed that the initially excited donor molecule has equilibrated with respect to the local environment. However, upon excitation and during the equilibration phase, the state of the system needs to be described by the full density matrix, including coherences between donor and acceptor states. While being intuitively clear, addressing this regime experimentally has been a challenge until the recently reported advances in fluorescence detected two-dimensional spectroscopy. Here, we demonstrate using fourth order perturbation theory the conditions for the presence of donor-acceptor coherence induced cross-peaks at zero waiting time between the first and the second pair of pulses. The approach is illustrated for a heterodimer model which facilitates an analytical solution.
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| 8. |
- Shi, Qi, et al.
(författare)
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Variations in the Composition of the Phases Lead to the Differences in the Optoelectronic Properties of MAPbBr3 Thin Films and Crystals
- 2018
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 122:38, s. 21817-21823
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Tidskriftsartikel (refereegranskat)abstract
- Photoluminescence (PL) spectra from thin films (TFs) and bulk crystals (BCs) of hybrid organo-halide perovskites are significantly different, the origin of which and their impact on the efficiency of the perovskite-based photoactive devices have been debated. We have used two-photon PL to study the temperature-dependent changes in the spectra of the TFs and the BCs of methylammonium lead bromide (MAPbBr3) perovskites in order to clarify the origin of the differences. Our results show that the differences in the spectra are due to the variation in the phase composition. At room temperature, the tetragonal (TE) phase is dominant in the BCs, while the orthorhombic (OR) phase is dominant in the TFs. The PL spectra of the TFs also show discernible contributions from the TE and the cubic phases. At lower temperatures, the increase in excitonic recombination causes a red shift of the PL spectra from the TFs, while a phase transition from the TE to the OR phase results in a blue shift of the PL from the BCs. The temperature-dependent narrowing of the PL linewidths shows a stronger coupling between the longitudinal optical phonons and the free carriers in the OR phase as compared to the TE phase, implying a reduced carrier mobility. However, as the OR phase is metastable at the room temperature, the slow phase transition to the TE phase should improve the photocurrent yield in the TFs, provided that the sample is shielded from other types of degradation.
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| 9. |
- Yang, Bin, et al.
(författare)
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High Resolution Mapping of Two-Photon Excited Photocurrent in Perovskite Microplate Photodetector
- 2018
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 9:17, s. 5017-5022
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Tidskriftsartikel (refereegranskat)abstract
- We fabricate photodetectors based on solution-processed single CH3NH3PbBr3 microcrystals (MCs) and map the two-photon absorption (TPA) excited photocurrent (PC) with spatial resolution of 1 μm. We find that the charge carrier transport length in the MCs depends on the applied electric field, and increases from 5.7 μm for 0.02 V bias (dominated by carrier diffusion) to 23.2 μm for 2 V bias (dominated by carrier drift). Furthermore, PC shows strong spatial variations. Combining the PC mapping results with time-resolved photoluminescence microscopy, we demonstrate that the spatial distribution of PC mainly originates from the inhomogeneous distribution of trap-states across perovskite MCs. This suggests that there is still large margin for improvement of perovskite single crystal devices by better controlling of the traps.
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| 10. |
- Yang, Bin, et al.
(författare)
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Lead-Free Silver-Bismuth Halide Double Perovskite Nanocrystals
- 2018
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Ingår i: Angewandte Chemie - International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 57:19, s. 5359-5363
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Tidskriftsartikel (refereegranskat)abstract
- Lead-free perovskite nanocrystals (NCs) were obtained mainly by substituting a Pb2+ cation with a divalent cation or substituting three Pb2+ cations with two trivalent cations. The substitution of two Pb2+ cations with one monovalent Ag+ and one trivalent Bi3+ cations was used to synthesize Cs2AgBiX6 (X=Cl, Br, I) double perovskite NCs. Using femtosecond transient absorption spectroscopy, the charge carrier relaxation mechanism was elucidated in the double perovskite NCs. The Cs2AgBiBr6 NCs exhibit ultrafast hot-carrier cooling (<1 ps), which competes with the carrier trapping processes (mainly originate from the surface defects). Notably, the photoluminescence can be increased by 100 times with surfactant (oleic acid) added to passivate the defects in Cs2AgBiCl6 NCs. These results suggest that the double perovskite NCs could be potential materials for optoelectronic applications by better controlling the surface defects.
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