arXiv subjects

Shohei Fujimoto

Publications and source records attributed to Shohei Fujimoto.

7 recordsLinked to original sources

arXiv2021

Fully automated spectroscopic ellipsometry analyses: Application to MoOx thin films

In spectroscopic ellipsometry, the optical properties of materials are obtained indirectly by generally assuming dielectric function and optical models. This ellipsometry analysis, which typically requires numerous model parameters, has essentially been performed by a try-and-error approach, making this method as a rather time-consuming characterization technique. Here, we propose a fully automated spectroscopic ellipsometry analysis method, which can be applied to obtain dielectric functions of light absorbing materials in a full measured energy range without any prior knowledge of model parameters. The developed method consists of a multiple-step grid search and the following non-linear regression analysis. Specifically, in our approach, the analyzed spectral region is gradually expanded toward higher energy while incorporating an additional optical transition peak whenever the root-mean-square error of the fitting analysis exceeds a critical value. In particular, we have established a unique algorithm that could be employed for the ellipsometry analyses of different types of optical materials. The proposed scheme has been applied successfully for the analyses of MoOx transparent oxides and the complex dielectric function of a MoOx layer that exhibits dual optical transitions due to band-edge and deep-level absorptions has been determined. The developed method can drastically reduce a time necessary for an ellipsometry analysis, eliminating a serious drawback of a traditional spectroscopic ellipsometry analysis method.

physics.optics↗

arXiv2019

Maximum efficiencies and performance limiting factors of inorganic and hybrid perovskite solar cells

The Shockley and Queisser limit, a well-known efficiency limit for a solar cell, is based on unrealistic physical assumptions and its maximum limit is seriously overestimated. To understand the power loss mechanisms of record-efficiency cells, a more rigorous approach is necessary. Here, we have established a new formalism that can accurately predict absolute performance limits of solar cells in conventional thin film form. In particular, we have estimated the maximum efficiencies of 13 well-studied solar cell materials [GaAs, InP, CdTe, a-Si:H, CuInSe2, CuGaSe2, CuInGaSe2, Cu2ZnSnSe4, Cu2ZnSnS4, Cu2ZnSn(S,Se)4, Cu2ZnGeSe4, CH3NH3PbI3, HC(NH2)2PbI3] in a 1-um-thick physical limit. Our calculation shows that over 30% efficiencies can be achieved for absorber layers with sharp absorption edges (GaAs, InP, CdTe, CuInGaSe2, Cu2ZnGeSe4). Nevertheless, many record-efficiency polycrystalline solar cells, including hybrid perovskites, are limited by open-circuit voltage and fill-factor losses. We show that the maximum conversion efficiencies described here present new alternative limits that can predict the power generation of real-world solar cells.

physics.app-ph↗

arXiv2018

Tail state formation in solar cell materials: First principles analyses of zincblende, chalcopyrite, kesterite and hybrid perovskite crystals

Tail state formation in solar cell absorbers leads to a detrimental effect on solar cell performance. Nevertheless, the characterization of the band tailing in experimental semiconductor crystals is generally difficult. In this article, to determine the tail state generation in various solar cell materials, we have developed a quite general theoretical scheme in which the experimental Urbach energy is compared with the absorption edge energy derived from density functional theory (DFT) calculation. For this purpose, the absorption spectra of solar cell materials, including CdTe, CuInSe2 (CISe), CuGaSe2 (CGSe), Cu2ZnSnSe4 (CZTSe), Cu2ZnSnS4 (CZTS) and hybrid perovskites, have been calculated by DFT particularly using very-high-density k meshes. As a result, we find that the tail state formation is negligible in CdTe, CISe, CGSe and hybrid perovskite polycrystals. However, coevaporated CZTSe and CZTS layers exhibit very large Urbach energies, which are far larger than the theoretical counterparts. Based on DFT analysis results, we conclude that the quite large tail state formation observed in the CZTSe and CZTS originates from extensive cation disordering. In particular, even a slight cation substitution is found to generate unusual band fluctuation in CZT(S)Se. In contrast, CH3NH3PbI3 hybrid perovskite shows the sharpest absorption edge theoretically, which agrees with experiment.

cond-mat.mtrl-sci↗

arXiv2017

Carrier loss mechanisms in textured crystalline Si-based solar cells

A quite general device analysis method that allows the direct evaluation of optical and recombination losses in crystalline silicon (c-Si)-based solar cells has been developed. By applying this technique, the optical and physical limiting factors of the state-of-the-art solar cells with ~20% efficiencies have been revealed. In the established method, the carrier loss mechanisms are characterized from the external quantum efficiency (EQE) analysis with very low computational cost. In particular, the EQE analyses of textured c-Si solar cells are implemented by employing the experimental reflectance spectra obtained directly from the actual devices while using flat optical models without any fitting parameters. We find that the developed method provides almost perfect fitting to EQE spectra reported for various textured c-Si solar cells, including c-Si heterojunction solar cells, a dopant-free c-Si solar cell with a MoOx layer, and an n-type passivated emitter with rear locally diffused (PERL) solar cell. The modeling of the recombination loss further allows the extraction of the minority carrier diffusion length and surface recombination velocity from the EQE analysis. Based on the EQE analysis results, the carrier loss mechanisms in different types of c-Si solar cells are discussed.

physics.app-ph↗

arXiv2017

Universal rules for visible-light absorption in hybrid perovskite materials

A variety of organic-inorganic hybrid perovskites (APbX3) consisting of mixed center cations [A = CH3NH3+, HC(NH2)2+, Cs+] with different PbX3- cages (X = I, Br, Cl) have been developed to realize high-efficiency solar cells. Nevertheless, clear understanding for the effects of A and X on the optical transition has been lacking. Here, we present universal rules that allow the unified interpretation of the optical absorption in various hybrid perovskites. In particular, we find that the influence of the A-site cation on the light absorption is rather significant and the absorption coefficient (alpha) reduces to half when CH3NH3+ is replaced with HC(NH2)2+ in the APbI3 system. Our density functional theory (DFT) calculations reproduce all of the fine absorption features observed in HC(NH2)2PbI3 and CH3NH3PbBr3, allowing the unique assignment of the interband transitions in the Brillouin zone. In contrast to general understanding that the A-site cation involves weakly in the optical process, our theoretical calculations reveal that the center cation plays a critical role in the interband transition and the absorption strength in the visible region is modified by the strong A-X interaction. Furthermore, our systematic analyses show that the variation of the absorption spectrum with X can be described simply by the well-known sum rule. The universal rules established in this study explain the large reduction of alpha in HC(NH2)2PbI3 and predict CsPbI3 as the highest alpha material.

cond-mat.mtrl-sci↗

arXiv2016

Quantitative determination of optical and recombination losses in thin-film photovoltaic devices based on external quantum efficiency analysis

In developing photovoltaic devices with high efficiencies, quantitative determination of the carrier loss is crucial. In conventional solar-cell characterization techniques, however, photocurrent reduction originating from parasitic light absorption and carrier recombination within the light absorber cannot be assessed easily. Here, we develop a general analysis scheme in which the optical and recombination losses in submicron-textured solar cells are evaluated systematically from external quantum efficiency (EQE) spectra. In this method, the optical absorption in solar cells is first deduced by imposing the anti-reflection condition in the calculation of the absorptance spectrum, and the carrier extraction from the light absorber layer is then modeled by considering a carrier collection length from the absorber interface. Our analysis method is appropriate for a wide variety of photovoltaic devices, including kesterite solar cells [Cu2ZnSnSe4, Cu2ZnSnS4, and Cu2ZnSn(S,Se)4], zincblende CdTe solar cells, and hybrid perovskite (CH3NH3PbI3) solar cells, and provides excellent fitting to numerous EQE spectra reported earlier. Based on the results obtained from our EQE analyses, we discuss the effects of parasitic absorption and carrier recombination in different types of solar cells.

cond-mat.mtrl-sci↗

arXiv2016

Optical transitions in hybrid perovskite solar cells: Ellipsometry, density functional theory, and quantum efficiency analyses for CH3NH3PbI3

We report artifact-free CH3NH3PbI3 optical constants extracted from ultra-smooth perovskite layers without air exposure and assign all the optical transitions in the visible/ultraviolet region unambiguously based on density functional theory (DFT) analysis that assumes a simple pseudo-cubic crystal structure. From the self-consistent spectroscopic ellipsometry analysis of the ultra-smooth CH3NH3PbI3 layers, we find that the absorption coefficients of CH3NH3PbI3 (alpha = 3.8 x 10^4 cm-1 at 2.0 eV) are comparable to those of CuInGaSe2 and CdTe, and high alpha values reported in earlier studies are overestimated seriously by extensive surface roughness of CH3NH3PbI3 layers. The polarization-dependent DFT calculations show that CH3NH3+ interacts strongly with the PbI3- cage, modifying the CH3NH3PbI3 dielectric function in the visible region rather significantly. When the effect of CH3NH3+ on the optical transition is eliminated in the DFT calculation, CH3NH3PbI3 dielectric function deduced from DFT shows excellent agreement with the experimental result. As a result, distinct optical transitions observed at E0 (Eg) = 1.61 eV, E1 = 2.53 eV, and E2 = 3.24 eV in CH3NH3PbI3 are attributed to the direct semiconductor-type transitions at the R, M, and X points in the pseudo-cubic Brillouin zone, respectively. We further perform the quantum efficiency (QE) analysis for a standard hybrid-perovskite solar cell incorporating a mesoporous TiO2 layer and demonstrate that the QE spectrum can be reproduced almost perfectly when the revised CH3NH3PbI3 optical constants are employed. Depth-resolved QE simulations confirm that Jsc is limited by the material's longer wavelength response and indicate the importance of optical confinement and long carrier diffusion lengths in hybrid perovskite solar cells.

cond-mat.mtrl-sci↗