skip to main content


Title: Photoluminescence Excitation Spectroscopy Characterization of Surface and Bulk Quality for Early-Stage Potential of Material Systems
Abstract — Photoluminescence Excitation Spectroscopy (PLE) is a contactless characterization technique to quantify Shockley-Reed-Hall (SRH) lifetimes and recombination velocities in direct band gap experimental semiconductor materials and devices. It is also useful as to evaluate surface passivation and intermediate fabrication processes, since it can be implemented without the need for development of effective contact technologies. In this paper, we present a novel experimental PLE system for precision-based quantification of the aforementioned parameters as well as a system for which absolute PLE characterization may occur. Absolute PLE measurements can be used to directly calculate VOC for new photovoltaic (PV) material systems and devices. Key system capabilities include a continuous excitation spectrum from 300 nm –1.1 μm, automated characterization, up to 1 nm wavelength resolution (up to 60x higher than prior work), and a reduced ellipsometry requirement for post-processing of data. We utilize a GaAs double heterostructure (DH) and an InP crystalline wafer as calibration standards in comparison with data from an LED-based PLE to demonstrate the validity of the results obtained from this new system. Index Terms – photovoltaic cells, photoluminescence, charge carrier lifetime, gallium arsenide, indium phosphide.  more » « less
Award ID(s):
1735282
NSF-PAR ID:
10184483
Author(s) / Creator(s):
; ;
Date Published:
Journal Name:
Photoluminescence Excitation Spectroscopy Characterization of Surface and Bulk Quality for Early-Stage Potential of Material Systems
Page Range / eLocation ID:
0377 to 0381
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current‐voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter‐laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br)3halide perovskite thin‐film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance‐free JV‐curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra‐grain charge transport is characterized by terahertz sum mobilities of ≈32 cm2V−1s−1. Drift‐diffusion simulations indicate that these intra‐grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best‐realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.

     
    more » « less
  2. Complex alkaline earth silicates have been extensively studied as rare-earth substituted phosphor hosts for use in solid-state lighting. One of the biggest challenges facing the development of new phosphors is understanding the relationship between the observed optical properties and the crystal structure. Fortunately, recent improvements in characterization techniques combined with advances in computational methodologies provide the research tools necessary to conduct a comprehensive analysis of these systems. In this work, a new Ce 3+ substituted phosphor is developed using Ba 5 Si 8 O 21 as the host crystal structure. The compound is evaluated using a combination of experimental and computational methods and shows Ba 5 Si 8 O 21 :Ce 3+ adopts a monoclinic crystal structure that was confirmed through Rietveld refinement of high-resolution synchrotron powder X-ray diffraction data. Photoluminescence spectroscopy reveals a broad-band blue emission centered at ∼440 nm with an absolute quantum yield of ∼45% under ultraviolet light excitation ( λ ex = 340 nm). This phosphor also shows a minimal chromaticity-drift but with moderate thermal quenching of the emission peak at elevated temperatures. The modest optical response of this phase is believed to stem from a combination of intrinsic structural complexity and the formation of defects because of the aliovalent rare-earth substitution. Finally, computational modeling provides essential insight into the site preference and energy level distribution of Ce 3+ in this compound. These results highlight the importance of using experiment and computation in tandem to interpret the relationship between observed optical properties and the crystal structures of all rare-earth substituted complex phosphors. 
    more » « less
  3. Yb 3+ -Doped lead-halide perovskites (Yb 3+ :CsPb(Cl 1−x Br x ) 3 ) have emerged as unique materials combining strong, tunable broadband absorption with near-infrared photoluminescence quantum yields (PLQYs) approaching 200% at ambient temperature. These remarkable properties make Yb 3+ :CsPb(Cl 1−x Br x ) 3 an extremely promising candidate for spectral shaping in high-efficiency photovoltaic devices. Previous theoretical assessments of such “downconversion” devices have predicted single-junction efficiencies up to 40%, but have been highly idealized. Real materials like Yb 3+ :CsPb(Cl 1−x Br x ) 3 have practical limitations such as constrained band-gap and PL energies, non-directional emission, and an excitation-power-dependent PLQY. Hence, it is unclear whether Yb 3+ :CsPb(Cl 1−x Br x ) 3 , or any other non-ideal quantum-cutting material, can indeed boost the efficiencies of real high-performance PV. Here, we examine the thermodynamic, detailed-balance efficiency limit of Yb 3+ :CsPb(Cl 1−x Br x ) 3 on different existing PV under real-world conditions. Among these, we identify silicon heterojunction technology as very promising for achieving significant performance gains when paired with Yb 3+ :CsPb(Cl 1−x Br x ) 3 , and we predict power-conversion efficiencies of up to 32% for this combination. Surprisingly, PL saturation does not negate the improved device performance. Calculations accounting for actual hourly incident solar photon fluxes show that Yb 3+ :CsPb(Cl 1−x Br x ) 3 boosts power-conversion efficiencies at all times of day and year in two representative geographic locations. Predicted annual energy yields are comparable to those of tandem perovskite-on-silicon technologies, but without the need for current matching, tracking, or additional electrodes and inverters. In addition, we show that band-gap optimization in real quantum cutters is inherently a function of their PLQY and the ability to capture that PL. These results provide key design rules needed for development of high-efficiency quantum-cutting photovoltaic devices based on Yb 3+ :CsPb(Cl 1−x Br x ) 3 . 
    more » « less
  4. Abstract High-precision placement of rare-earth ions in scalable silicon-based nanostructured materials exhibiting high photoluminescence (PL) emission, photostable and polarized emission, and near-radiative-limited excited state lifetimes can serve as critical building blocks toward the practical implementation of devices in the emerging fields of nanophotonics and quantum photonics. Introduced herein are optical nanostructures composed of arrays of ultrathin silicon carbide (SiC) nanowires (NWs) that constitute scalable one-dimensional NW-based photonic crystal (NW-PC) structures. The latter are based on a novel, fab-friendly, nanofabrication process. The NW arrays are grown in a self-aligned manner through chemical vapor deposition. They exhibit a reduction in defect density as determined by low-temperature time-resolved PL measurements. Additionally, the NW-PC structures enable the positioning of erbium (Er 3+ ) ions with an accuracy of 10 nm, an improvement on the current state-of-the-art ion implantation processes, and allow strong coupling of Er 3+ ions in NW-PC. The NW-PC structure is pivotal in engineering the Er 3+ -induced 1540-nm emission, which is the telecommunication wavelength used in optical fibers. An approximately 60-fold increase in the room-temperature Er 3+ PL emission is observed in NW-PC compared to its thin-film analog in the linear pumping regime. Furthermore, 22 times increase in the Er 3+ PL intensity per number of exited Er ions in NW-PC was observed at saturation while using 20 times lower pumping power. The NW-PC structures demonstrate broadband and efficient excitation characteristics for Er 3+ , with an absorption cross-section (~2 × 10 −18 cm 2 ) two-order larger than typical benchmark values for direct absorption in rare-earth-doped quantum materials. Experimental and simulation results show that the Er 3+ PL is photostable at high pumping power and polarized in NW-PC and is modulated with NW-PC lattice periodicity. The observed characteristics from these technologically friendly nanophotonic structures provide a promising route to the development of scalable nanophotonics and formation of single-photon emitters in the telecom optical wavelength band. 
    more » « less
  5. Solid-state quantum emitters have emerged as a leading quantum memory for quantum networking applications. However, standard optical characterization techniques are neither efficient nor repeatable at scale. Here we introduce and demonstrate spectroscopic techniques that enable large-scale, automated characterization of colour centres. We first demonstrate the ability to track colour centres by registering them to a fabricated machine-readable global coordinate system, enabling a systematic comparison of the same colour centre sites over many experiments. We then implement resonant photoluminescence excitation in a widefield cryogenic microscope to parallelize resonant spectroscopy, achieving two orders of magnitude speed-up over confocal microscopy. Finally, we demonstrate automated chip-scale characterization of colour centres and devices at room temperature, imaging thousands of microscope fields of view. These tools will enable the accelerated identification of useful quantum emitters at chip scale, enabling advances in scaling up colour centre platforms for quantum information applications, materials science and device design and characterization. 
    more » « less