Soonil Hong

Electrostatically Self‐Assembled Nonconjugated Polyelectrolytes as an Ideal Interfacial Layer for Inverted Polymer Solar Cells

Polymer solar cells (PSCs) based on the bulk heterojunction (BHJ) blend of a conjugated polymer donor and a fullerene acceptor have gained considerable attention as a cost-effi cient, fl exible, and portable energy source. [ 1–3 ] Considering the practical aspects of its commercialization, the inverted device structure of PSCs (I-PSCs), consisting of a BHJ photoactive layer between indium tin oxide (ITO) as a bottom cathode and a high work function (WF) metal (Ag or Au) as a top anode, is an advantageous approach due to its superior long-term stability and printability. [ 4–6 ] In this type of inverted device structure, an additional interfacial layer between the active layer and ITO electrode must be introduced to establish the device concept. The high WF of the bottom ITO cathode (approximately 4.8 eV) hampers the formation of an ohmic contact with the lowest unoccupied molecular orbital (LUMO) level of fullerene and makes the creation of a high built-in fi eld used to break the electrical symmetry of the device diffi cult. Thus, many researchers explored a variety of interfacial materials to shift and modify the energy level of the ITO cathode. [ 4–16 ]

A series connection architecture for large-area organic photovoltaic modules with a 7.5% module efficiency

The fabrication of organic photovoltaic modules via printing techniques has been the greatest challenge for their commercial manufacture. Current module architecture, which is based on a monolithic geometry consisting of serially interconnecting stripe-patterned subcells with finite widths, requires highly sophisticated patterning processes that significantly increase the complexity of printing production lines and cause serious reductions in module efficiency due to so-called aperture loss in series connection regions. Herein we demonstrate an innovative module structure that can simultaneously reduce both patterning processes and aperture loss. By using a charge recombination feature that occurs at contacts between electron- and hole-transport layers, we devise a series connection method that facilitates module fabrication without patterning the charge transport layers. With the successive deposition of component layers using slot-die and doctor-blade printing techniques, we achieve a high module efficiency reaching 7.5% with area of 4.15 cm2.

Achieving Large‐Area Planar Perovskite Solar Cells by Introducing an Interfacial Compatibilizer

Despite the recent unprecedented increase in the power conversion efficiencies (PCEs) of small-area devices (≤0.1 cm2 ), the PCEs deteriorate drastically for PSCs of larger areas because of the incomplete film coverage caused by the dewetting of the hydrophilic perovskite precursor solutions on the hydrophobic organic charge-transport layers (CTLs). Here, an innovative method of fabricating scalable PSCs on all types of organic CTLs is reported. By introducing an amphiphilic conjugated polyelectrolyte as an interfacial compatibilizer, fabricating uniform perovskite films on large-area substrates (18.4 cm2 ) and PSCs with the total active area of 6 cm2 (1 cm2 × 6 unit cells) via a single-turn solution process is successfully demonstrated. All of the unit cells exhibit highly uniform PCEs of 16.1 ± 0.9% (best PCE of 17%), which is the highest value for printable PSCs with a total active area larger than 1 cm2 .

Highly Stretchable and Highly Conductive PEDOT:PSS/Ionic Liquid Composite Transparent Electrodes for Solution-Processed Stretchable Electronics

Stretchable conductive materials have received great attention owing to their potential for realizing next-generation stretchable electronics. However, the simultaneous achievement of excellent mechanical stretchability and high electrical conductivity as well as cost-effective fabrication has been a significant challenge. Here, we report a highly stretchable and highly conducting polymer that was obtained by incorporating an ionic liquid. When 1-ethyl-3-methylimidazolium tetracyanoborate (EMIM TCB) was added to an aqueous conducting polymer solution of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), it was found that EMIM TCB acts not only as a secondary dopant but also as a plasticizer for PEDOT:PSS, resulting in a high conductivity of >1000 S cm-1 with stable performance at tensile strains up to 50% and even up to 180% in combination with the prestrained substrate technique. Consequently, by exploiting the additional benefits of high transparency and solution-processability of PEDOT:PSS, we were able to fabricate a highly stretchable, semitransparent, and wholly solution-processed alternating current electroluminescent device with unimpaired performance at 50% strain by using PEDOT:PSS/EMIM TCB composite films as both bottom and top electrodes.

Long-Term Stable Recombination Layer for Tandem Polymer Solar Cells Using Self-Doped Conducting Polymers.

UNLABELLED Recently, the most efficient tandem polymer solar cells (PSCs) have used poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) ( PEDOT PSS) as a p-type component of recombination layer (RL). However, its undesirable acidic nature, originating from insulating PSS, of PEDOT PSS drastically reduces the lifetime of PSCs. Here, we demonstrate the efficient and stable tandem PSCs by introducing acid-free self-doped conducting polymer (SCP), combined with zinc oxide nanoparticles (ZnO NPs), as RL for PEDOT PSS-free tandem PSCs. Moreover, we introduce an innovative and versatile nanocomposite system containing photoactive and p-type conjugated polyelectrolyte (p-CPE) into the tandem fabrication of an ideal self-organized recombination layer. In our new RL, highly conductive SCP facilitates charge transport and recombination process, and p-CPE helps to achieve nearly loss-free charge collection by increasing effective work function of indium tin oxide (ITO) and SCP. Because of the synergistic effect of extremely low electrical resistance, ohmic contact, and pH neutrality, tandem devices with our novel RL performed well, exhibiting a high power conversion efficiency of 10.2% and a prolonged lifetime. These findings provide a new insight for strategic design of RLs using SCPs to achieve efficient and stable tandem PSCs and enable us to review and extend the usefulness of SCPs in various electronics research fields.

A New Architecture for Printable Photovoltaics Overcoming Conventional Module Limits

A new architecture for manufacturing large-area polymer solar cells that does not produce concomitant aperture and Ohmic losses is presented. By introducing the innovative concept of metal-filamentary nanoelectrodes, which are vertically formed inside the main active layers, loss-free, widely expandable solar cells with the highest relative power conversion efficiency (ca. 90%) in organic photovoltaic systems are demonstrated.

Highly Deformable and See‐Through Polymer Light‐Emitting Diodes with All‐Conducting‐Polymer Electrodes

Despite the high expectation of deformable and see-through displays for future ubiquitous society, current light-emitting diodes (LEDs) fail to meet the desired mechanical and optical properties, mainly because of the fragile transparent conducting oxides and opaque metal electrodes. Here, by introducing a highly conductive nanofibrillated conducting polymer (CP) as both deformable transparent anode and cathode, ultraflexible and see-through polymer LEDs (PLEDs) are demonstrated. The CP-based PLEDs exhibit outstanding dual-side light-outcoupling performance with a high optical transmittance of 75% at a wavelength of 550 nm and with an excellent mechanical durability of 9% bending strain. Moreover, the CP-based PLEDs fabricated on 4 µm thick plastic foils with all-solution processing have extremely deformable and foldable light-emitting functionality. This approach is expected to open a new avenue for developing wearable and attachable transparent displays.

High-efficiency large-area perovskite photovoltaic modules achieved via electrochemically assembled metal-filamentary nanoelectrodes

We devised an electrochemical patterning process for large-area perovskite photovoltaic modules. Realizing industrial-scale, large-area photovoltaic modules without any considerable performance losses compared with the performance of laboratory-scale, small-area perovskite solar cells (PSCs) has been a challenge for practical applications of PSCs. Highly sophisticated patterning processes for achieving series connections, typically fabricated using printing or laser-scribing techniques, cause unexpected efficiency drops and require complicated manufacturing processes. We successfully fabricated high-efficiency, large-area PSC modules using a new electrochemical patterning process. The intrinsic ion-conducting features of perovskites enabled us to create metal-filamentary nanoelectrodes to facilitate the monolithic serial interconnections of PSC modules. By fabricating planar-type PSC modules through low-temperature annealing and all-solution processing, we demonstrated a notably high module efficiency of 14.0% for a total area of 9.06 cm2 with a high geometric fill factor of 94.1%.

Introducing paired electric dipole layers for efficient and reproducible perovskite solar cells

Elimination of charge trapping at defects is highly challenging for poly-crystalline organometal halide perovskites. Here, we report a new architecture for reinforcing the built-in electric field (Ein) across the photoactive layer with a pair of strong electric dipole layers (EDLs). The paired EDLs significantly intensify the Ein across the perovskite layer, resulting in suppressed charge trapping of photogenerated charges. As a result, our low-temperature processed P–I–N planar PeSC devices using the paired EDLs exhibit a higher power conversion efficiency (ηmax ∼ 19.4%) and a smaller device-to-device variation with a standard deviation (S.D.) of 0.70%, which far surpass those (ηmax ∼ 17.8%, S.D. ∼ 1.1%) of the devices with typical charge transport layers.

Interface engineering for large-area planar perovskite solar cells (Conference Presentation)

The formation of pinhole-free perovskite photoactive films with full surface coverage has been a tremendous challenge for up-scaling planar perovskite solar cells (PSCs) while maintaining their high power conversion efficiencies (PCEs). Particularly, a significant mismatch between the surface energies of a hydrophilic perovskite precursor solution and a hydrophobic organic charge transport layer (CTL) has been a major cause for the poor and random surface coverage of perovskite photoactive films, which drastically reduces the scalability and reproducibility of PSCs. Here, we report a universal method to create extremely compact perovskite photoactive films on a variety of hydrophobic CTLs. By introducing an amphiphilic conjugated polyelectrolyte as an interfacial compatibilizer, we succeed in improving the wettability of perovskite precursor solutions on hydrophobic CTLs and fabricating perovskite photoactive films over large areas. Our approach enables the scalable fabrication of planar PSCs with large areas (1 cm2, PCE of 17%) while preserving nearly 90% of the PCEs of the corresponding small-area devices (PCE of 19%).