The remarkable optoelectronic properties of metal halide perovskites have generated intense research interest over the last few years. The ability to control and manipulate the crystallisation and stoichiometry of perovskite thin-films has allowed for impressive strides in the development of highly efficient perovskite solar cells. However, being able to effectively modify the interfaces of metal halide perovskites, and to controllably p- or n-type dope the surfaces, may be key to further improvements in the efficiency and long-term stability of these devices. In this study, we use surface doping of the mixed-cation, mixed-halide perovskite FA 0.85 MA 0.15 Pb(I 0.85 Br 0.15 ) 3 (FA – formamidinium; MA – methylammonium) to improve the hole extraction from the perovskite solar cell. By treating the surface of the perovskite film with a strongly oxidizing molybdenum tris(dithiolene) complex, we achieve a shift in the work function that is indicative of p-doping, and a twofold increase in the total conductivity throughout the film. We probe the associated interfacial chemistry through photoelectron and solid-state nuclear magnetic resonance spectroscopies and confirm that charge-transfer occurs between the perovskite and dopant complex. The resulting p-doped interface constitutes a homojunction with increased hole-selectivity. With charge-selective layers, we show that thismore »
DNA‐Based Strategies for Site‐Specific Doping
The development of novel doping strategies compatible with high‐resolution patterning and low cost, large‐scale manufacturing is critical to the future development of electronic devices. Here, an approach to achieve nanoscale site‐specific doping of Si wafer using DNA as both the template and the dopant carrier is reported. Upon thermal treatment, the phosphorous atoms in the DNA diffuse into Si wafer, resulting in doping within the region right around the DNA template. A doping length of 30 nm is achieved for 10 s of thermal treatment at 1000 °C. Prototype field effect transistors are fabricated using the DNA‐doped Si substrate; the device characteristics confirmed that the Si is n‐doped. It is also shown that this approach can be extended to achieve both n‐type and p‐type site‐specific doping of Si by using DNA nanostructures to pattern self‐assembled monolayers. This work shows that the DNA template is a dual‐use template that can both pattern Si and deliver dopants.
- Award ID(s):
- 1901864
- Publication Date:
- NSF-PAR ID:
- 10449613
- Journal Name:
- Advanced Functional Materials
- Volume:
- 31
- Issue:
- 1
- ISSN:
- 1616-301X
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
This paper addresses one of the key issues in the scientific community of Si photonics: thin-film quality and the light emission properties of band-engineered n+Germanium-on-Silicon (Ge-on-Si). Compared to the traditional delta doping approach, which was utilized in the first electrically-pumped Ge-on-Si lasers, we offer an n+Ge-on-Si thin film with better material quality and higher carrier injection efficiency grown by metal-organic chemical vapor deposition (MOCVD). The impacts of thermal cycle annealing and Si substrate offcut on the thin film quality were investigated, including surface roughness, strain, threading dislocation density, Si-Ge interdiffusion, and dopant diffusion. It was revealed that: 1) MOCVD overcomes the outdiffision issue of n-type dopants by having the dopant peaks at the bottom of the Ge films; 2) the characterization of the light emission properties of these MOCVD n+Ge-on-Si samples (1.0 × 1019cm−3doped) compared to delta-doped ultra-high vacuum chemical vapor deposition (UHVCVD) Ge, showing comparable photoluminescence (PL) spectral intensity at 1/4 of the doping level; 3) Detailed PL spectral analyses showed that population inversion from the direct gap transition has been achieved, and the injected electron density in the direct Γ valley is comparable to that of the delta-doped sample even though the n-type doping level is 75% less; and 4)more »
-
Abstract FeN4moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton‐exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe−N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high‐temperature treatment. Here, we elucidate the FeN4site formation mechanisms through hosting Fe ions into a nitrogen‐doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF‐8‐derived nitrogen‐doped carbon is an ideal model with well‐defined nitrogen doping and porosity. This approach is able to deconvolute Fe−N bond formation from complex carbonization and nitrogen doping, which correlates Fe−N bond properties with the activity and stability of FeN4sites as a function of the thermal activation temperature.
-
Abstract FeN4moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton‐exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe−N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high‐temperature treatment. Here, we elucidate the FeN4site formation mechanisms through hosting Fe ions into a nitrogen‐doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF‐8‐derived nitrogen‐doped carbon is an ideal model with well‐defined nitrogen doping and porosity. This approach is able to deconvolute Fe−N bond formation from complex carbonization and nitrogen doping, which correlates Fe−N bond properties with the activity and stability of FeN4sites as a function of the thermal activation temperature.
-
Abstract Electrocatalysts are required for clean energy technologies (for example, water‐splitting and metal‐air batteries). The development of a multifunctional electrocatalyst composed of nitrogen, phosphorus, and fluorine tri‐doped graphene is reported, which was obtained by thermal activation of a mixture of polyaniline‐coated graphene oxide and ammonium hexafluorophosphate (AHF). It was found that thermal decomposition of AHF provides nitrogen, phosphorus, and fluorine sources for tri‐doping with N, P, and F, and simultaneously facilitates template‐free formation of porous structures as a result of thermal gas evolution. The resultant N, P, and F tri‐doped graphene exhibited excellent electrocatalytic activities for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The trifunctional metal‐free catalyst was further used as an OER–HER bifunctional catalyst for oxygen and hydrogen gas production in an electrochemical water‐splitting unit, which was powered by an integrated Zn–air battery based on an air electrode made from the same electrocatalyst for ORR. The integrated unit, fabricated from the newly developed N, P, and F tri‐doped graphene multifunctional metal‐free catalyst, can operate in ambient air with a high gas production rate of 0.496 and 0.254 μL s−1for hydrogen and oxygen gas, respectively, showing great potential for practical applications.
