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DOE OSTI2017

Multichannel Interdiffusion Driven FASnI 3 Film Formation Using Aqueous Hybrid Salt/Polymer Solutions toward Flexible Lead-Free Perovskite Solar Cells

Tin (Sn)-based perovskites are increasingly attractive because they offer lead-free alternatives in perovskite solar cells. Yet, depositing high-quality Sn-based perovskite films is still a challenge, particularly for low-temperature planar heterojunction (PHJ) devices. In this work, a “multichannel interdiffusion” protocol is demonstrated by annealing stacked layers of aqueous solution deposited formamidinium iodide (FAI)/polymer layer followed with an evaporated SnI 2 layer to create uniform FASnI 3 films. In this protocol, tiny FAI crystals, significantly inhibited by the introduced polymer, can offer multiple interdiffusion pathways for complete reaction with SnI 2 . What is more, water, rather than traditional aprotic organic solvents, is used to dissolve the precursors. The best-performing FASnI 3 PHJ solar cell assembled by this protocol exhibits a power conversion efficiency (PCE) of 3.98%. In addition, a flexible FASnI 3 -based flexible solar cell assembled on a polyethylene naphthalate–indium tin oxide flexible substrate with a PCE of 3.12% is demonstrated. This novel interdiffusion process can aid to further boost the performance of lead-free Sn-based perovskites.

14 SOLAR ENERGY↗
DOE OSTI2017

Improved Performance of All‐Polymer Solar Cells Enabled by Naphthodiperylenetetraimide‐Based Polymer Acceptor

A new polymer acceptor, naphthodiperylenetetraimide‐vinylene (NDP‐V), featuring a backbone of altenating naphthodiperylenetetraimide and vinylene units is designed and applied in all‐polymer solar cells (all‐PSCs). With this polymer acceptor, a new record power‐conversion efficiencies (PCE) of 8.59% has been achieved for all‐PSCs. The design principle of NDP‐V is to reduce the conformational disorder in the backbone of a previously developed high‐performance acceptor, PDI‐V, a perylenediimide‐vinylene polymer. The chemical modifications result in favorable changes to the molecular packing behaviors of the acceptor and improved morphology of the donor–acceptor (PTB7‐Th:NDP‐V) blend, which is evidenced by the enhanced hole and electron transport abilities of the active layer. Moreover, the stronger absorption of NDP‐V in the shorter‐wavelength range offers a better complement to the donor. All these factors contribute to a short‐circuit current density ( J sc ) of 17.07 mA cm −2 . With a fill factor (FF) of 0.67, an average PCE of 8.48% is obtained, representing the highest value thus far reported for all‐PSCs.

Guo, Yikun↗
DOE OSTI2017

Enhancing Performance of Nonfullerene Acceptors via Side‐Chain Conjugation Strategy

A side‐chain conjugation strategy in the design of nonfullerene electron acceptors is proposed, with the design and synthesis of a side‐chain‐conjugated acceptor (ITIC2) based on a 4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐ b :4,5‐ b′ ]di(cyclopenta‐dithiophene) electron‐donating core and 1,1‐dicyanomethylene‐3‐indanone electron‐withdrawing end groups. ITIC2 with the conjugated side chains exhibits an absorption peak at 714 nm, which redshifts 12 nm relative to ITIC1. The absorption extinction coefficient of ITIC2 is 2.7 × 10 5 m −1 cm −1 , higher than that of ITIC1 (1.5 × 10 5 m −1 cm −1 ). ITIC2 exhibits slightly higher highest occupied molecular orbital (HOMO) (−5.43 eV) and lowest unoccupied molecular orbital (LUMO) (−3.80 eV) energy levels relative to ITIC1 (HOMO: −5.48 eV; LUMO: −3.84 eV), and higher electron mobility (1.3 × 10 −3 cm 2 V −1 s −1 ) than that of ITIC1 (9.6 × 10 −4 cm 2 V −1 s −1 ). The power conversion efficiency of ITIC2‐based organic solar cells is 11.0%, much higher than that of ITIC1‐based control devices (8.54%). Our results demonstrate that side‐chain conjugation can tune energy levels, enhance absorption, and electron mobility, and finally enhance photovoltaic performance of nonfullerene acceptors.

Wang, Jiayu↗
DOE OSTI2017

Hole‐Transfer Dependence on Blend Morphology and Energy Level Alignment in Polymer: ITIC Photovoltaic Materials

Abstract Bulk‐heterojunction organic photovoltaic materials containing nonfullerene acceptors (NFAs) have seen remarkable advances in the past year, finally surpassing fullerenes in performance. Indeed, acceptors based on indacenodithiophene (IDT) have become synonymous with high power conversion efficiencies (PCEs). Nevertheless, NFAs have yet to achieve fill factors (FFs) comparable to those of the highest‐performing fullerene‐based materials. To address this seeming anomaly, this study examines a high efficiency IDT‐based acceptor, ITIC , paired with three donor polymers known to achieve high FFs with fullerenes, PTPD3T , PBTI3T , and PBTSA3T . Excellent PCEs up to 8.43% are achieved from PTPD3T:ITIC blends, reflecting good charge transport, optimal morphology, and efficient ITIC to PTPD3T hole‐transfer, as observed by femtosecond transient absorption spectroscopy. Hole‐transfer is observed from ITIC to PBTI3T and PBTSA3T , but less efficiently, reflecting measurably inferior morphology and nonoptimal energy level alignment, resulting in PCEs of 5.34% and 4.65%, respectively. This work demonstrates the importance of proper morphology and kinetics of ITIC → donor polymer hole‐transfer in boosting the performance of polymer: ITIC photovoltaic bulk heterojunction blends.

Eastham, Nicholas D.↗
DOE OSTI2017

Naphthodithiophene‐Based Nonfullerene Acceptor for High‐Performance Organic Photovoltaics: Effect of Extended Conjugation

Abstract Naphtho[1,2‐ b :5,6‐ b′ ]dithiophene is extended to a fused octacyclic building block, which is end capped by strong electron‐withdrawing 2‐(5,6‐difluoro‐3‐oxo‐2,3‐dihydro‐1H‐inden‐1‐ylidene)malononitrile to yield a fused‐ring electron acceptor (IOIC2) for organic solar cells (OSCs). Relative to naphthalene‐based IHIC2, naphthodithiophene‐based IOIC2 with a larger π‐conjugation and a stronger electron‐donating core shows a higher lowest unoccupied molecular orbital energy level (IOIC2: −3.78 eV vs IHIC2: −3.86 eV), broader absorption with a smaller optical bandgap (IOIC2: 1.55 eV vs IHIC2: 1.66 eV), and a higher electron mobility (IOIC2: 1.0 × 10 −3 cm 2 V −1 s −1 vs IHIC2: 5.0 × 10 −4 cm 2 V −1 s −1 ). Thus, IOIC2‐based OSCs show higher values in open‐circuit voltage, short‐circuit current density, fill factor, and thereby much higher power conversion efficiency (PCE) values than those of the IHIC2‐based counterpart. In particular, as‐cast OSCs based on FTAZ: IOIC2 yield PCEs of up to 11.2%, higher than that of the control devices based on FTAZ: IHIC2 (7.45%). Furthermore, by using 0.2% 1,8‐diiodooctane as the processing additive, a PCE of 12.3% is achieved from the FTAZ:IOIC2 ‐ based devices, higher than that of the FTAZ:IHIC2 ‐ based devices (7.31%). These results indicate that incorporating extended conjugation into the electron‐donating fused‐ring units in nonfullerene acceptors is a promising strategy for designing high‐performance electron acceptors.

Zhu, Jingshuai↗
DOE OSTI2018

Bandgap Engineering of Stable Lead‐Free Oxide Double Perovskites for Photovoltaics

Abstract Despite the rapid progress in solar power conversion efficiency of archetype organic–inorganic hybrid perovskite CH 3 NH 3 PbI 3 ‐based solar cells, the long‐term stability and toxicity of Pb remain the main challenges for the industrial deployment, leading to more uncertainties for global commercialization. The poor stabilities of CH 3 NH 3 PbI 3 ‐based solar cells may not only be attributed to the organic molecules but also the halides themself, most of which exhibit intrinsic instability under moisture and light. As an alternative, the possibility of oxide perovskites for photovoltaic applications is explored here. The class of lead‐free stable oxide double perovskites A 2 M(III)M(V)O 6 (A = Ca, Sr, Ba; M(III) = Sb 3+ or Bi 3+ ; M(V) = V 5+ , Nb 5+ , or Ta 5+ ) is comprehensively explored with regard to their stability and their electronic and optical properties. Apart from the strong stability, this class of double perovskites exhibits direct bandgaps ranging from 0.3 to 3.8 eV. With proper B site alloying, the bandgap can be tuned within the range of 1.0–1.6 eV with optical absorptions as strong as CH 3 NH 3 PbI 3 , making them suitable for efficient single‐junction thin‐film solar cell application.

Sun, Qingde↗
DOE OSTI2018

Fused Tris(thienothiophene)‐Based Electron Acceptor with Strong Near‐Infrared Absorption for High‐Performance As‐Cast Solar Cells

Abstract A fused tris(thienothiophene) (3TT) building block is designed and synthesized with strong electron‐donating and molecular packing properties, where three thienothiophene units are condensed with two cyclopentadienyl rings. Based on 3TT, a fused octacylic electron acceptor (FOIC) is designed and synthesized, using strong electron‐withdrawing 2‐(5/6‐fluoro‐3‐oxo‐2,3‐dihydro‐1H‐inden‐1‐ylidene)‐malononitrile as end groups. FOIC exhibits absorption in 600–950 nm region peaked at 836 nm with extinction coefficient of up to 2 × 10 5 m –1 cm –1 , low bandgap of 1.32 eV, and high electron mobility of 1.2 × 10 –3 cm 2 V –1 s –1 . Compared with its counterpart ITIC3 based on indacenothienothiophene core, FOIC exhibits significantly upshifted highest occupied molecular orbital level, slightly downshifted lowest unoccupied molecular orbital level, significantly redshifted absorption, and higher mobility. The as‐cast organic solar cells (OSCs) based on blends of PTB7‐Th donor and FOIC acceptor without additional treatments exhibit power conversion efficiencies (PCEs) as high as 12.0%, which is much higher than that of PTB7‐Th: ITIC3 (8.09%). The as‐cast semitransparent OSCs based on the same blends show PCEs of up to 10.3% with an average visible transmittance of 37.4%.

Li, Tengfei↗
DOE OSTI2018

Phase Transition Control for High Performance Ruddlesden-Popper Perovskite Solar Cells

Ruddlesden–Popper reduced-dimensional hybrid perovskite (RDP) semiconductors have attracted significant attention recently due to their promising stability and excellent optoelectronic properties. Here, the RDP crystallization mechanism in real time from liquid precursors to the solid film is investigated, and how the phase transition kinetics influences phase purity, quantum well orientation, and photovoltaic performance is revealed. An important template-induced nucleation and growth of the desired (BA) 2 (MA) 3 Pb 4 I 13 phase, which is achieved only via direct crystallization without formation of intermediate phases, is observed. As such, the thermodynamically preferred perpendicular crystal orientation and high phase purity are obtained. At low temperature, the formation of intermediate phases, including PbI 2 crystals and solvate complexes, slows down intercalation of ions and increases nucleation barrier, leading to formation of multiple RDP phases and orientation randomness. These insights enable to obtain high quality (BA) 2 (MA) 3 Pb 4 I 13 films with preferentially perpendicular quantum well orientation, high phase purity, smooth film surface, and improved optoelectronic properties. The resulting devices exhibit high power conversion efficiency of 12.17%. This work should help guide the perovskite community to better control Ruddlesden–Popper perovskite structure and further improve optoelectronic and solar cell devices.

14 SOLAR ENERGY↗
DOE OSTI2018

Ultrafast Spin-to-Charge Conversion at the Surface of Topological Insulator Thin Films

Strong spin–orbit coupling, resulting in the formation of spin–momentum–locked surface states, endows topological insulators with superior spin–to–charge conversion characteristics, though the dynamics that govern it have remained elusive. Here, an all–optical method is presented, which enables unprecedented tracking of the ultrafast dynamics of spin–to–charge conversion in a prototypical topological insulator Bi 2 Se 3 /ferromagnetic Co heterostructure, down to the sub–picosecond timescale. Compared to pure Bi 2 Se 3 or Co, a giant terahertz emission is observed in the heterostructure that originates from spin–to–charge conversion, in which the topological surface states play a crucial role. A 0.12 ps timescale is identified that sets a technological speed limit of spin–to–charge conversion processes in topological insulators. Additionally, it is shown that the spin–to–charge conversion efficiency is temperature independent in Bi 2 Se 3 as expected from the nature of the surface states, paving the way for designing next–generation high–speed optospintronic devices based on topological insulators at room temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2019

From Lead Halide Perovskites to Lead‐Free Metal Halide Perovskites and Perovskite Derivatives

Abstract Despite the exciting progress on power conversion efficiencies, the commercialization of the emerging lead (Pb) halide perovskite solar cell technology still faces significant challenges, one of which is the inclusion of toxic Pb. Searching for Pb‐free perovskite solar cell absorbers is currently an attractive research direction. The approaches used for and the consequences of Pb replacement are reviewed herein. Reviews on the theoretical understanding of the electronic, optical, and defect properties of Pb and Pb‐free halide perovskites and perovskite derivatives are provided, as well as the experimental results available in the literature. The theoretical understanding explains well why Pb halide perovskites exhibit superior photovoltaic properties, but Pb‐free perovskites and perovskite derivatives do not.

Xiao, Zewen↗
DOE OSTI2018

Achieving Balanced Crystallinity of Donor and Acceptor by Combining Blade‐Coating and Ternary Strategies in Organic Solar Cells

Abstract As a prototype tool for slot‐die coating, blade‐coating exhibits excellent compatibility with large‐area roll‐to‐roll coating. A ternary organic solar cell based on PBDB‐T:PTB7‐Th:FOIC blends is fabricated by blade‐coating and exhibits a power conversion efficiency of 12.02%, which is one of the highest values for the printed organic solar cells in ambient environment. It is demonstrated that blade‐coating can enhance crystallization of these three materials, but the degree of induction is different (FOIC > PBDB‐T > PTB7‐Th). Thus, the blade‐coated PBDB‐T:FOIC device presents much higher electron mobility than hole mobility due to the very high crystallinity of FOIC. Upon the addition of PTB7‐Th into the blade‐coated PBDB‐T:FOIC blends, the crystallinity of FOIC decreases together with the corresponding electron mobility, due to the better miscibility between PTB7‐Th and FOIC. The ternary strategy not only maintains the well‐matched crystallinity and mobilities, but also increases the photocurrent with complementary light absorption as well as the Förster resonant energy transfer. Furthermore, small domains with homogeneously distributed nanofibers are observed in favor of the exciton dissociation and charge transport. This combination of blade‐coating and ternary strategies exhibits excellent synergistic effect in optimizing morphology, showing great potential in the large‐area fabrication of highly efficient organic solar cells.

Zhang, Lin↗
DOE OSTI2019

Surface and Interface Properties in Thin‐Film Solar Cells: Using Soft X‐rays and Electrons to Unravel the Electronic and Chemical Structure

Abstract Thin‐film solar cells have great potential to overtake the currently dominant silicon‐based solar cell technologies in a strongly growing market. Such thin‐film devices consist of a multilayer structure, for which charge‐carrier transport across interfaces plays a crucial role in minimizing the associated recombination losses and achieving high solar conversion efficiencies. Further development can strongly profit from a high‐level characterization that gives a local, electronic, and chemical picture of the interface properties, which allows for an insight‐driven optimization. Herein, the authors' recent progress of applying a “toolbox” of high‐level laboratory‐ and synchrotron‐based electron and soft X‐ray spectroscopies to characterize the chemical and electronic properties of such applied interfaces is provided. With this toolbox in hand, the activities are paired with those of experts in thin‐film solar cell preparation at the cutting edge of current developments to obtain a deeper understanding of the recent improvements in the field, e.g., by studying the influence of so‐called “post‐deposition treatments”, as well as characterizing the properties of interfaces with alternative buffer layer materials that give superior efficiencies on large, module‐sized areas.

Weinhardt, Lothar↗
DOE OSTI2019

In Situ Back‐Contact Passivation Improves Photovoltage and Fill Factor in Perovskite Solar Cells

Abstract Organic–inorganic hybrid perovskite solar cells (PSCs) have seen a rapid rise in power conversion efficiencies in recent years; however, they still suffer from interfacial recombination and charge extraction losses at interfaces between the perovskite absorber and the charge–transport layers. Here, in situ back‐contact passivation (BCP) that reduces interfacial and extraction losses between the perovskite absorber and the hole transport layer (HTL) is reported. A thin layer of nondoped semiconducting polymer at the perovskite/HTL interface is introduced and it is shown that the use of the semiconductor polymer permits—in contrast with previously studied insulator‐based passivants—the use of a relatively thick passivating layer. It is shown that a flat‐band alignment between the perovskite and polymer passivation layers achieves a high photovoltage and fill factor: the resultant BCP enables a photovoltage of 1.15 V and a fill factor of 83% in 1.53 eV bandgap PSCs, leading to an efficiency of 21.6% in planar solar cells.

Tan, Furui↗
DOE OSTI2019

Bamboo–Like Nitrogen–Doped Carbon Nanotube Forests as Durable Metal–Free Catalysts for Self–Powered Flexible Li–CO 2 Batteries

The Li-CO 2 battery is a promising energy storage device for wearable electronics due to its long discharge plateau, high energy density, and environmental friendliness. Furthermore, its utilization is largely hindered by poor cyclability and mechanical rigidity due to the lack of a flexible and durable catalyst electrode. Herein, flexible fiber-shaped Li-CO 2 batteries with ultralong cycle-life, high rate capability, and large specific capacity are fabricated, employing bamboo-like N-doped carbon nanotube fiber (B-NCNT) as flexible, durable metal-free catalysts for both CO 2 reduction and evolution reactions. Benefiting from high N-doping with abundant pyridinic groups, rich defects, and active sites of the periodic bamboo-like nodes, the fabricated Li-CO 2 battery shows outstanding electrochemical performance with high full-discharge capacity of 23328 mAh g -1 , high rate capability with a low potential gap up to 1.96 V at a current density of 1000 mA g -1 , stability over 360 cycles, and good flexibility. Meanwhile, the bifunctional B-NCNT is used as the counter electrode for a fiber-shaped dye-sensitized solar cell to fabricate a self-powered fiber-shaped Li-CO 2 battery with overall photochemical-electric energy conversion efficiency of up to 4.6%. Along with a stable voltage output, this design demonstrates great adaptability and application potentiality in wearable electronics with a breath monitor as an example.

25 ENERGY STORAGE↗
DOE OSTI2020

Choose Your Own Adventure: Fabrication of Monolithic All-Perovskite Tandem Photovoltaics

Metal halide perovskites (MHPs) have transfixed the photovoltaic (PV) community due to their outstanding and tunable optoelectronic properties coupled to demonstrations of high-power conversion efficiencies (PCE) at a range of bandgaps. This has motivated the field to push perovskites to reach the highest possible performance. One way to increase the efficiency is by fabricating multijunction solar cells, which can split the solar spectrum, reducing thermalization loss. Low-cost all-perovskite tandems have a real chance to soon exceed 30% PCE, which could transform the PV industry. Achieving this goal requires the identification of perovskite sub-cells that are both highly efficient and can be effectively integrated. In this review, it is discussed how to navigate the multiple-choice adventure in choosing between the myriad of options and considerations present when deciding what perovskite materials, contact layers, and processing tools to use. Some of the potential fabrication pitfalls often encountered in MHP based tandem PVs are highlighted, so that they can hopefully be avoided in the future.

14 SOLAR ENERGY↗
DOE OSTI2020

The Role of Demixing and Crystallization Kinetics on the Stability of Non‐Fullerene Organic Solar Cells

Abstract With power conversion efficiency now over 17%, a long operational lifetime is essential for the successful application of organic solar cells. However, most non‐fullerene acceptors can crystallize and destroy devices, yet the fundamental underlying thermodynamic and kinetic aspects of acceptor crystallization have received limited attention. Here, room‐temperature (RT) diffusion coefficients of 3.4 × 10 −23 and 2.0 × 10 −22 are measured for ITIC‐2Cl and ITIC‐2F, two state‐of‐the‐art non‐fullerene acceptors. The low coefficients are enough to provide for kinetic stabilization of the morphology against demixing at RT. Additionally profound differences in crystallization characteristics are discovered between ITIC‐2F and ITIC‐2Cl. The differences as observed by secondary‐ion mass spectrometry, differential scanning calorimetry (DSC), grazing‐incidence wide‐angle X‐ray scattering, and microscopy can be related directly to device degradation and are attributed to the significantly different nucleation and growth rates, with a difference in the growth rate of a factor of 12 at RT. ITIC‐4F and ITIC‐4Cl exhibit similar characteristics. The results reveal the importance of diffusion coefficients and melting enthalpies in controlling the growth rates, and that differences in halogenation can drastically change crystallization kinetics and device stability. It is furthermore delineated how low nucleation density and large growth rates can be inferred from DSC and microscopy experiments which could be used to guide molecular design for stability.

Hu, Huawei↗
DOE OSTI2020

Thermodynamic Properties and Molecular Packing Explain Performance and Processing Procedures of Three D18:NFA Organic Solar Cells

Abstract Organic solar cells (OSCs) based on D18:Y6 have recently exhibited a record power conversion efficiency of over 18%. The initial work is extended and the device performance of D18‐based OSCs is compared with three non‐fullerene acceptors, Y6, IT‐4F, and IEICO‐4Cl, and their molecular packing characteristics and miscibility are studied. The D18 polymer shows unusually strong chain extension and excellent backbone ordering in all films, which likely contributes to the excellent hole‐transporting properties. Thermodynamic characterization indicates a room‐temperature miscibility for D18:Y6 and D18:IT‐4F near the percolation threshold. This corresponds to an ideal quench depth and explains the use of solvent vapor annealing rather than thermal annealing. In contrast, D18:IEICO‐4Cl is a low‐miscibility system with a deep quench depth during casting and poor morphology control and low performance. A failure of ternary blends with PC 71 BM is likely due to the near‐ideal miscibility of Y6 to begin with and indicates that strategies for developing successful ternary or quaternary solar cells are likely very different for D18 than for other high‐performing donors. This work reveals several unique property–performance relations of D18‐based photovoltaic devices and helps guide design or fabrication of yet higher efficiency OSCs.

Wang, Zhen↗