Ultra-low dielectric constant polyimides: Combined efforts of fluorination and micro-branched crosslink structure

Han, Shuhao; Li, Yinong; Hao, Fuyao; Zhou, Han; Qi, Shengli; Tian, Guofeng; Wu, Dezhen

doi:10.1016/j.eurpolymj.2020.110206

Cited by 78 publications

(47 citation statements)

References 23 publications

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“…As shown in Figure 6a, the storage modulus of PIs reduces gradually with rising temperature and drops sharply near the T g . In Figure 6b, the T g of PIs increases from 272.9 to 283.5 °C with the content of TAPB increasing due to the crosslinked network hindering the movement of molecular chains, resulting in the improvement of the heat resistance [12]. Figure 7 shows the variation of tensile strength and elongation at the break of PI films with TAPB content increasing.…”

Section: Resultsmentioning

confidence: 99%

“…It indicates that the micro-branched structure widens the distance between molecules and reduces the aggregation of molecular chains, resulting in the reduction of the dielectric permittivity. Meanwhile, the formation of the slight crosslinked network structure will restrict the orientation of dipoles effectively to reduce molecular polarizability, which also leads to the reduction of dielectric permittivity [12]. When the content of TAPB exceeded 0.2 mmol, the dielectric permittivity and loss started to increase due to the excess TAPB content, which can diminish the distance between molecular chains via the crosslinking effect.…”

Section: Resultsmentioning

confidence: 99%

“…the PI/TAPOB hybrid film was decreased from 3.42 to 3.12 (10 MHz) as compared to that of neat PI due to the induced micro-branched crosslink structure could bring in a higher free volume of the molecular chain. In addition, the presence of micro-branched structures in PIs could also increase the rigidity of the PI chains to improve the resistance to deformation of PI films simultaneously [12]. Song et al [13] found the contact angle values of PI films increased, indicating that the surface of PI films became more hydrophobic due to the existence of crosslinked networks.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Construction of micro-branched crosslink fluorinated polyimide with ultra-low dielectric permittivity and enhanced mechanical properties

Zhao¹,

Cao²,

Huang³

et al. 2022

Express Polym. Lett.

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There is a great demand for low dielectric materials as insulating interlayers in large-scale integrated circuit development. However, it is still a huge challenge to reduce the dielectric permittivity of polymers while maintaining excellent thermal stability and mechanical properties. In this work, the fluorinated polyimides (PIs) in combination with a micro-branched crosslinking structure were prepared successfully by introducing different amounts of 1,3,5-tris(4-aminophenyl) benzene (TAPB) to obtain ultra-low dielectric permittivity. The results revealed that PI film containing 2 mmol TAPB had the lowest dielectric permittivity (2.47) and dielectric loss (0.008) at 1 MHz due to the fluorine atoms and the micro-branched crosslink structure, which not only decreased the molecular polarizability but also increased the free fractional volume. In addition, PI film containing 2 mmol TAPB had the highest tensile strength of 106.02 MPa with an elongation at a break of 15.1% because the presence of TAPB effectively promoted the connection between PI molecular chains, resulting in the inhibition of the molecular mobility. The incorporation of TAPB also enhanced the thermal stability and ultraviolet light-shielding performance of PI films. This method paves the way for the development of PIs with ultra-low dielectric permittivity for the electronic industry.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Construction of micro-branched crosslink fluorinated polyimide with ultra-low dielectric permittivity and enhanced mechanical properties

Zhao¹,

Cao²,

Huang³

et al. 2022

Express Polym. Lett.

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“…针对化学交联法调控聚酰亚胺薄膜面内热膨胀的研究报道已有很多，例如通过引入三官能团单体、炔基、苯并环丁烯或金属离子配位基团等方式，可获得具有不同交联程度的聚酰亚胺薄膜，有效降低薄膜的面内热膨胀系数 [52][53][54][55][56][57] . 从分子结构设计角度而言， Liou 等 [25] 将马来酸酐或苯乙炔基封端的可交联低聚物，分别与 PMDA/ODA、BPDA/PDA 的商品化前驱体溶液共混，制备了厚度为 10 μm 的交联型聚酰亚胺薄膜.…”

Section: 化学交联结构unclassified

Research progress in thermal expansion behavior of polyimide films

Wang¹,

Zhai²,

Gao³

et al. 2022

Sci. Sin.-Chim

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As one of the most important flexible substrates and interlayer dielectric materials, the thermal expansion performance of polyimide films has always attracted great interest. Especially with the development of advanced electronic and microelectronic devices, the linear and volumetric thermal expansion of polyimide films are facing more and more stringent requirements. In order to explore new generation polyimide films with low thermal expansion, it is necessary to clarify the thermal expansion behaviors and influence mechanism. For polymer films, the thermal expansion actually includes in-plane and out-of-plane linear as well as volumetric thermal expansion. Most researches on thermal expansion of polyimide films are focused on the in-plane thermal expansion, but there are few studies on the out-of-plane and volume thermal expansion of films. There is no systematic understanding of comprehensive and anisotropic of thermal expansion of films. The research on linear and volume thermal expansion behavior of polyimide films were firstly summarized in this paper. The testing methods were introduced in detail, including thermomechanical analysis (TMA), variable temperature wide-angle X-ray diffraction (VT-WAXD), capacitance technique, optical interferometry, etc. The influencing factors of thermal expansion behavior of polyimide films were discussed, such as molecular backbone structures, local molecular motions, chemical crosslinking, aggregation structures and film preparation process. The relationship between structures and processes on in-plane, out-of-plane linear and volumetric thermal expansion behavior of polyimide films was clarified. The problems and challenges in the future research on thermal expansion were prospected. This review can provide a necessary guidance for the development of high-performance polyimide films with low thermal expansion during wide temperature range.

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“…Unfortunately, owing to the poor polarization of their rigid backbone, the dielectric constant of commercial PIs (k = ~3.5 at 1 kHz) is too high for increasing the data transmission speed of electronic devices [ 7 , 8 , 9 ]. Typical synthetic routes of porous PIs include: (i) modification of chemical backbone structure (e.g., fluorination, or side-chain substitution) [ 10 , 11 , 12 ], (ii) incorporation of high-volume air pockets with k = ~1 into the matrix [ 13 , 14 ], and organic–inorganic hybridization [ 15 ].…”

Section: Introductionmentioning

confidence: 99%

Polymer Concentration and Liquid—Liquid Demixing Time Correlation with Porous Structure of Low Dielectric Polyimide in Diffusion-Driven Phase Separation

et al. 2022

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Porous polyimide (PI) films are a promising low-k dielectric material for high-frequency data transmission with low signal attenuation. Pores are generated by non-solvent induced phase separation (NIPS) during phase inversion of polymer solution via non-solvent accumulation and solvent diffusion. In this study, aromatic PI was employed as a matrix for NIPS, and the influence of polymer concentration and liquid—liquid demixing time on the morphology of pores in the PI films was investigated. This ensured control over the porous structure of the PI film and provided desirable dielectric properties in a broad frequency range of 100 Hz–30 MHz (1.99 at 30 MHz) and thermal stability (Td5% > 576 °C, Tg > 391 °C). This study addresses the effect of polymer concentration and coagulation time on the morphology and physical properties of PI sponge films and provides guidance on the design and optimization of architectures for polymeric materials requiring pore modification.

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Ultra-low dielectric constant polyimides: Combined efforts of fluorination and micro-branched crosslink structure

Cited by 78 publications

References 23 publications

Construction of micro-branched crosslink fluorinated polyimide with ultra-low dielectric permittivity and enhanced mechanical properties

Construction of micro-branched crosslink fluorinated polyimide with ultra-low dielectric permittivity and enhanced mechanical properties

Research progress in thermal expansion behavior of polyimide films

Polymer Concentration and Liquid—Liquid Demixing Time Correlation with Porous Structure of Low Dielectric Polyimide in Diffusion-Driven Phase Separation

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