Third Crystalline Form of P(NDI2OD-T2) with Pronounced End-on Texture

Đoán, Vũ Văn; Tan, Wen Liang; He, Lu; Ehm, Alexander; Zahn, Dietrich R. T.; McNeill, Christopher R.

doi:10.1021/acsmacrolett.2c00402

Cited by 3 publications

(14 citation statements)

References 41 publications

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“…In contrast, form II is characterized by an alternating packing of NDI and T2 units, with NDI units associating with T2 units on adjacent chains and vice versa. This c /2 shift in adjacent chains along the backbone direction results in a very weak (001) reflection and dominant (002) backbone reflection. , Form II is also characterized by the appearance of mixed index peaks such (101), (201), and (302). , Recently, we reported the discovery of a third crystalline form of P(NDI2OD-T2), form III, distinguished from forms I and II by a doubling of the length of the c -axis, corresponding to an accommodation of two monomer units in the unit cell along the backbone direction . Curiously, this new form III polymorph was also found to exhibit a strong end-on texture with backbones oriented vertically with respect to the substrate, a texture that is generally difficult to achieve.…”

Section: Introductionmentioning

confidence: 99%

“…25,26 Form II is also characterized by the appearance of mixed index peaks such (101), (201), and (302). 25,26 Recently, we reported the discovery of a third crystalline form of P(NDI2OD-T2), form III, distinguished from forms I and II by a doubling of the length of the c-axis, corresponding to an accommodation of two monomer units in the unit cell along the backbone direction. 26 Curiously, this new form III polymorph was also found to exhibit a strong end-on texture with backbones oriented vertically with respect to the substrate, a texture that is generally difficult to achieve.…”

Section: ■ Introductionmentioning

confidence: 99%

“…25,26 Recently, we reported the discovery of a third crystalline form of P(NDI2OD-T2), form III, distinguished from forms I and II by a doubling of the length of the c-axis, corresponding to an accommodation of two monomer units in the unit cell along the backbone direction. 26 Curiously, this new form III polymorph was also found to exhibit a strong end-on texture with backbones oriented vertically with respect to the substrate, a texture that is generally difficult to achieve. Figure 1 presents a schematic of the characteristic GIWAXS patterns of forms I, II, and III, with each form shown in its dominant molecular orientation (texture).…”

Section: ■ Introductionmentioning

confidence: 99%

“…Similar to form II, form III was produced by annealing to high temperature (specifically 340 °C) followed by a slow cooling. 26 However, the fact that form III had not been discovered until very recently suggests that the formation of form III requires more stringent control of processing parameters. The observation that melt annealing and slow cooling can lead to either an edge-on 28 or end-on orientation 26 is also intriguing.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Unlike for form I and form II, the factors that lead to the formation of form III are not well understood. Similar to form II, form III was produced by annealing to high temperature (specifically 340 °C) followed by a slow cooling . However, the fact that form III had not been discovered until very recently suggests that the formation of form III requires more stringent control of processing parameters.…”

Section: Introductionmentioning

confidence: 99%

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Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

et al. 2023

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The molecular packing and orientation of conjugated polymer chains in thin films have considerable influence on the charge transport properties and performance of polymer-based optoelectronic devices. Understanding and controlling the formation of different packing geometries and textures are important for understanding structure–function relationships and the purposeful optimization of device performance. Here, we extensively study the origin of a recently discovered third crystalline form (“form III”) of the well-studied electron transporting polymer P(NDI2OD-T2) that also exhibits pronounced end-on orientation. The effects of various processing conditions on the thin-film microstructure are studied with grazing-incidence wide-angle X-ray scattering. We find that end-on oriented form III crystallites directly evolve from face-on oriented form I crystallites upon melting under the specific conditions of high molecular weight, optimum annealing temperature, and optimum film thickness. Furthermore, by studying the charge transport properties of P(NDI2OD-T2) thin films in electron-only diodes and field-effect transistors, we find that films with end-on oriented form III crystallites demonstrate a 5-fold increase in carrier mobility in diodes (vertical transport direction) and a 1.5-fold increase in electron mobility in transistors (horizontal transport direction) compared to films with either face-on form I crystallites or edge-on form II crystallites.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

et al. 2023

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Design Principles of Diketopyrrolopyrrole‐Thienopyrrolodione Acceptor₁–Acceptor₂ Copolymers

Erhardt,

Hungenberg,

Chantler

et al. 2024

Adv Funct Materials

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The design principles of acceptor1–acceptor2 copolymers featuring alternating diketopyrrolopyrrole (DPP) and thienopyrrolodione (TPD) moieties are investigated. The investigated series of polymers is obtained by varying the aromatic linker between the two acceptor motifs between thiophene, thiazole, pyridine, and benzene. High electron affinities between 3.96 and 4.42 eV, facilitated by the synergy of the acceptor motifs are determined with optical gaps between 1.37 and 2.02 eV. Grazing incidence wide‐angle X‐ray scattering studies reveal a range of film morphologies after thermal annealing, including face‐on, end‐on and superstructure edge‐on‐like crystallites. Conversely, all materials form thin edge‐on layers on the polymer–air interface, as demonstrated by multi‐elemental near‐edge X‐ray absorption fine‐structure spectroscopy. The benefit of the electron‐deficient linkers thiazole and pyridine is evident: In organic field effect transistors, electron mobilities of up to 4.6 × 10−2 cm2 V−1 s−1 are obtained with outstanding on/off current ratios of 5 × 105, facilitated by the absence of detectable hole transport in these materials. Viability for all‐polymer solar cells is assessed in active layer blends with the donor polymer PM6, yielding a maximum average power conversion efficiency of 4.8% and an open circuit voltage above 1 V.

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Nanoconfinement Dominates the Formation of Edge-On Lamellar Crystals in Ultrathin Poly(l-lactide) Films

Lin,

Wei,

Wei

et al. 2024

Macromolecules

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The crystallization morphologies and orientations of poly(L-lactide) (PLLA) in ultrathin films supported on hydroxylation-modified gold-coated substrates with molecular weights (M w ) between 71 and 2100 kg/mol were investigated by atomic force microscopy and infrared reflection absorption spectroscopy. The results show that the predominant orientation of the crystals in the ultrathin PLLA films varies from flat-on to edge-on with increasing M w or decreasing film thickness (h). These phenomena were mainly attributed to the difference in chain conformation for various M w and h, which was caused by nanoconfinement. With the enhancement of the nanoconfinement, the molecular chains prefer to line up parallel to the substrate as prepared by spin-coating and have a stronger memory effect to resist the variation of chain conformation during annealing. Therefore, the crystals with kinetically favored edge-on orientation were easier to be formed. These results provide a new insight into controlling the lamellar orientation in thin crystalline polymer films.

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Third Crystalline Form of P(NDI2OD-T2) with Pronounced End-on Texture

Cited by 3 publications

References 41 publications

Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

Design Principles of Diketopyrrolopyrrole‐Thienopyrrolodione Acceptor₁–Acceptor₂ Copolymers

Nanoconfinement Dominates the Formation of Edge-On Lamellar Crystals in Ultrathin Poly(l-lactide) Films

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Third Crystalline Form of P(NDI2OD-T2) with Pronounced End-on Texture

Cited by 3 publications

References 41 publications

Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

Formation and Charge Transport Properties of P(NDI2OD-T2) Thin Films with End-on Oriented Form III Crystallites

Design Principles of Diketopyrrolopyrrole‐Thienopyrrolodione Acceptor1–Acceptor2 Copolymers

Nanoconfinement Dominates the Formation of Edge-On Lamellar Crystals in Ultrathin Poly(l-lactide) Films

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Product

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Design Principles of Diketopyrrolopyrrole‐Thienopyrrolodione Acceptor₁–Acceptor₂ Copolymers