The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the corr...The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the correlation between the exposure of passivating groups on the surface and device performance remains unexplored.Herein,we introduce two newly designed SAM molecules,Cbz2S and Cbz2SMe,incorporating cyclic disulfide or two flanking thiomethyls by modifying the 4,5-position of carbazole to adjust the Lewis basicity of the SAM-modified surface.Despite possessing suitable energetic alignment,Cbz2S with more-exposed sulfur atoms exhibited inferior device performance due to excessive reactivity,leading to an overpopulation of PbI2 crystallites at the buried perovskite interface.In contrast,the screening effect from the methyl groups of Cbz2SMe optimized SAM reactivity,exquisitely integrating buried interface passivation and hole selection together.Consequently,the champion inverted perovskite solar cell(PSC)employing Cbz2SMe achieved an impressive power conversion efficiency of 24.42%,accompanied by prolonged stability.This work demonstrates the feasibility of incorporating Lewis-basic passivation groups into SAM molecules and elucidates the relationship between the reactivity of SAM passivation groups and device performance.These findings provide valuable insights for the design of novel multifunctional SAM molecules,further advancing the performance of PSCs.展开更多
Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport vi...Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport via intramolecular coupling remains challenging.Herein,we demonstrate the transition of the intramolecular through-bond and through-space coupling in a single-molecule junction with a family of diketopyrrolopyrrole(DPP)derivative by varying intramolecular donor–acceptor(D–A)interactions.The transition is accomplished by regulating D–A interactions by inserting different aromatic rings inside,leading to two orders of magnitude difference of the single-molecule conductance.The flicker noise analysis demonstrates that the conductance difference arises from the control of the contribution between through-bond and through-space coupling.These findings are further supported by the calculation that the intramolecular coupling among molecular building blocks correlates with the D–A interaction,providing a promising way to regulate the contribution between through-bond and through-space coupling in the charge transport through molecular materials and devices.展开更多
Photoresists are essential for the fabrication of flexible electronics through all-photolithographic processes.Single component semiconducting photoresist exhibits both semiconducting and photo-patterning properties,a...Photoresists are essential for the fabrication of flexible electronics through all-photolithographic processes.Single component semiconducting photoresist exhibits both semiconducting and photo-patterning properties,and as a result,the device fabrication process can be simplified.However,the design of semiconducting polymeric photoresist with ambipolar semiconducting property remains challenging.In this paper,we report a single component semiconducting photoresist(PFDPPF4T-N_(3))by incorporating azide groups and noncovalent conformation locks into the side alkyl chains and conjugated backbones of a diketopyrrolopyrrole-based conjugated polymer,respectively.The results reveal that PFDPP4FT-N_(3) exhibits ambipolar semiconducting property with hole and electron mobilities up to 1.12 and 1.17 cm^(2) V^(−1) s^(−1),respectively.Moreover,field effect transistors with the individual photo-patterned thin films of PFDPP4FT-N_(3) also show ambipolar semiconducting behavior with hole and electron mobilities up to 0.66 and 0.80 cm^(2) V^(−1) s^(−1),respectively.These results offer a simple yet effective design strategy for high-performance single component semiconducting photoresists,which hold great potential for flexible electronics processed by all-photolithography.展开更多
基金support from the CityU Infrastructure Support from Central (APRCgrant nos.9380086,9610419,9610492,and 9610508)of the City University of Hong Kong+5 种基金the Guangdong-Hong Kong Technology Cooperation Funding Scheme (TCFS,grant no.GHP/018/20SZ)Midstream Research Programme for Universities (MRP)Grant (grant no.MRP/040/21X)from the Innovation and Technology Commission of Hong Kongthe Green Tech Fund (grant no.202020164)from the Environment and Ecology Bureau of Hong Kongthe General Research Fund (GRF,grant nos.11307621 and 11316422)from the Research Grants Council of Hong KongShenzhen Science and Technology Program (grant no.SGDX20201103095412040)Guangdong Major Project of Basic and Applied Basic Research (grant no.2019B030302007).
文摘The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the correlation between the exposure of passivating groups on the surface and device performance remains unexplored.Herein,we introduce two newly designed SAM molecules,Cbz2S and Cbz2SMe,incorporating cyclic disulfide or two flanking thiomethyls by modifying the 4,5-position of carbazole to adjust the Lewis basicity of the SAM-modified surface.Despite possessing suitable energetic alignment,Cbz2S with more-exposed sulfur atoms exhibited inferior device performance due to excessive reactivity,leading to an overpopulation of PbI2 crystallites at the buried perovskite interface.In contrast,the screening effect from the methyl groups of Cbz2SMe optimized SAM reactivity,exquisitely integrating buried interface passivation and hole selection together.Consequently,the champion inverted perovskite solar cell(PSC)employing Cbz2SMe achieved an impressive power conversion efficiency of 24.42%,accompanied by prolonged stability.This work demonstrates the feasibility of incorporating Lewis-basic passivation groups into SAM molecules and elucidates the relationship between the reactivity of SAM passivation groups and device performance.These findings provide valuable insights for the design of novel multifunctional SAM molecules,further advancing the performance of PSCs.
基金supported by Natural Science Foundation of China(nos.21722305,21673195,21703188,51733004,and 51525303)the National Key R&D Program of China(nos.2017YFA0204902 and 2017YFA0204903)+1 种基金the Beijing National Laboratory for Molecular Sciences(no.BNLMS202005)the China Postdoctoral Science Foundation(no.2017M622060).
文摘Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport via intramolecular coupling remains challenging.Herein,we demonstrate the transition of the intramolecular through-bond and through-space coupling in a single-molecule junction with a family of diketopyrrolopyrrole(DPP)derivative by varying intramolecular donor–acceptor(D–A)interactions.The transition is accomplished by regulating D–A interactions by inserting different aromatic rings inside,leading to two orders of magnitude difference of the single-molecule conductance.The flicker noise analysis demonstrates that the conductance difference arises from the control of the contribution between through-bond and through-space coupling.These findings are further supported by the calculation that the intramolecular coupling among molecular building blocks correlates with the D–A interaction,providing a promising way to regulate the contribution between through-bond and through-space coupling in the charge transport through molecular materials and devices.
基金supported by the National Key R&D Program of China(2018YFE0200700)the National Natural Science Foundation of China(22175081,21790363,61890943,22021002,22090021,22075293)+3 种基金the Key Research Program of the Chinese Academy of Sciences(XDPB13)the CAS-Croucher Funding Scheme for Joint LaboratoriesBeijing National Laboratory for Molecular Sciences(BNLM202010)Guangdong Provincial Key Laboratory of Catalysis(20210701)。
文摘Photoresists are essential for the fabrication of flexible electronics through all-photolithographic processes.Single component semiconducting photoresist exhibits both semiconducting and photo-patterning properties,and as a result,the device fabrication process can be simplified.However,the design of semiconducting polymeric photoresist with ambipolar semiconducting property remains challenging.In this paper,we report a single component semiconducting photoresist(PFDPPF4T-N_(3))by incorporating azide groups and noncovalent conformation locks into the side alkyl chains and conjugated backbones of a diketopyrrolopyrrole-based conjugated polymer,respectively.The results reveal that PFDPP4FT-N_(3) exhibits ambipolar semiconducting property with hole and electron mobilities up to 1.12 and 1.17 cm^(2) V^(−1) s^(−1),respectively.Moreover,field effect transistors with the individual photo-patterned thin films of PFDPP4FT-N_(3) also show ambipolar semiconducting behavior with hole and electron mobilities up to 0.66 and 0.80 cm^(2) V^(−1) s^(−1),respectively.These results offer a simple yet effective design strategy for high-performance single component semiconducting photoresists,which hold great potential for flexible electronics processed by all-photolithography.
