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• W3200380859 abstract "Adding the chemical tunability of conjugated organic materials to organic/inorganic heterostructures with monolayer precision allows the properties to be tailored at the molecular level. Likewise, construction of an ordered organic layer on an inorganic layered surface constitutes an effective strategy to achieve atomically well-defined interfaces. Consequently, (opto)electronics with unique capabilities and multifunctionalities can be designed by making use of novel physical processes at hybrid interfaces and the combined advantages of different material classes. This review addresses the fundamentals of design strategies toward vdW organic/inorganic heterostructures in the 2D limit and the resulting interface interactions. Furthermore, we provide an overview of advanced electronics and optoelectronics as well as neuromorphic and other multifunctional devices based on these emergent heterostructures, with performance superior to what have been achieved with the individual material classes. Van der Waals organic/inorganic heterostructures in the two-dimensional (2D) limit with extensive structural tunability will advance the development of artificial solids with tailored functionalities. Recent breakthroughs in several types of 2D organic materials, including molecular monolayer films, 2D polymers, covalent-organic frameworks, and metal oxide frameworks, have greatly enriched the design possibilities of heterostructures with inorganic 2D materials. This review provides a timely summary of the latest advances in synthesis approaches toward advanced organic/inorganic heterostructures, answers the fundamental questions regarding the interfacial interactions in the 2D limit, and further highlights the uses of such organic/inorganic heterostructures in advanced transistors, optoelectronics, neuromorphic, and other multifunctional devices with unique capabilities. Van der Waals organic/inorganic heterostructures in the two-dimensional (2D) limit with extensive structural tunability will advance the development of artificial solids with tailored functionalities. Recent breakthroughs in several types of 2D organic materials, including molecular monolayer films, 2D polymers, covalent-organic frameworks, and metal oxide frameworks, have greatly enriched the design possibilities of heterostructures with inorganic 2D materials. This review provides a timely summary of the latest advances in synthesis approaches toward advanced organic/inorganic heterostructures, answers the fundamental questions regarding the interfacial interactions in the 2D limit, and further highlights the uses of such organic/inorganic heterostructures in advanced transistors, optoelectronics, neuromorphic, and other multifunctional devices with unique capabilities. IntroductionThe feasibility of combining materials with diverse characteristics that leads to intriguing behavior at the interfaces and a wide range of electronic and optical properties lies in the heart of modern electronics.1Britnell L. Ribeiro R.M. Eckmann A. Jalil R. Belle B.D. Mishchenko A. Kim Y.J. Gorbachev R.V. Georgiou T. Morozov S.V. et al.Strong light-matter interactions in heterostructures of atomically thin films.Science. 2013; 340: 1311-1314Crossref PubMed Scopus (1710) Google Scholar,2Geim A.K. Grigorieva I.V. Van der Waals heterostructures.Nature. 2013; 499: 419-425Crossref PubMed Scopus (6083) Google Scholar This is of paramount importance especially when imparting advanced properties to individual material class becomes increasingly difficult while the demands of multifunctionality in appropriate physical dimensions are growing fast.3Sun J. Choi Y. Choi Y.J. Kim S. Park J.H. Lee S. Cho J.H. 2D–organic hybrid heterostructures for optoelectronic applications.Adv. Mater. 2019; 31: e1803831https://doi.org/10.1002/adma.201803831Crossref PubMed Scopus (45) Google Scholar New material structures and technologies are urgently needed to enable further diversity and multifunctionality of future electronics. The successful isolation of a single atomic layer from graphite in 20044Novoselov K.S. Geim A.K. Morozov S.V. Jiang D. Zhang Y. Dubonos S.V. Grigorieva I.V. Firsov A.A. Electric field effect in atomically thin carbon films.Science. 2004; 306: 666-669Crossref PubMed Scopus (46860) Google Scholar and then other layered nanomaterials5Novoselov K.S. Jiang D. Schedin F. Booth T.J. Khotkevich V.V. Morozov S.V. Geim A.K. Two-dimensional atomic crystals.Proc. Natl. Acad. Sci. USA. 2005; 102: 10451-10453Crossref PubMed Scopus (0) Google Scholar has inspired vigorous research efforts devoted to two-dimensional (2D) van der Waals (vdW) materials and heterostructures.6Zhang H. Cheng H.M. Ye P. 2D nanomaterials: beyond graphene and transition metal dichalcogenides.Chem. Soc. Rev. 2018; 47: 6009-6012Crossref PubMed Google Scholar With the atomically thin nature and dangling-bond-free advantage of this material class, it is possible to overcome the scaling limitation of bulk-material-based traditional electronics, and more importantly, to allow further integration with other material classes for programmed functionality.7Liu C. Chen H. Wang S. Liu Q. Jiang Y.G. Zhang D.W. Liu M. Zhou P. Two-dimensional materials for next-generation computing technologies.Nat. Nanotechnol. 2020; 15: 545-557Crossref PubMed Scopus (97) Google Scholar, 8Wu F. Li Q. Wang P. Xia H. Wang Z. Wang Y. Luo M. Chen L. Chen F. Miao J. et al.High efficiency and fast van der Waals hetero-photodiodes with a unilateral depletion region.Nat. Commun. 2019; 10: 4663https://doi.org/10.1038/s41467-019-12707-3Crossref PubMed Scopus (86) Google Scholar, 9Zhang H. Abhiraman B. Zhang Q. Miao J. Jo K. Roccasecca S. Knight M.W. Davoyan A.R. Jariwala D. Hybrid exciton-plasmon-polaritons in van der Waals semiconductor gratings.Nat. Commun. 2020; 11: 3552Crossref PubMed Scopus (16) Google Scholar In addition, the atomically thin nature of these new materials renders them high mechanical flexibility and optical transparency, serving as ideal platforms for flexible or wearable (opto)electronics, sensors, and integrated systems.As the molecular analogs of 2D atomic materials, organic 2D materials, i.e., 2D molecular crystals10Yang F. Cheng S. Zhang X. Ren X. Li R. Dong H. Hu W. 2D organic materials for optoelectronic applications.Adv. Mater. 2018; 30: 1702415Crossref Scopus (58) Google Scholar and synthetic polymers11Colson J.W. Dichtel W.R. Rationally synthesized two-dimensional polymers.Nat. Chem. 2013; 5: 453-465Crossref PubMed Scopus (692) Google Scholar with molecular/monomer-unit thickness over a large area, well-defined in-plane periodicity, and saturated bonds in surface, have attracted considerable attention in the past decades. Coupled with well-designed interlinkage bonds, crystalline frameworks, including covalent-organic frameworks (COFs) and metal-organic frameworks (MOFs),12Zhao M. Huang Y. Peng Y. Huang Z. Ma Q. Zhang H. Two-dimensional metal-organic framework nanosheets: synthesis and applications.Chem. Soc. Rev. 2018; 47: 6267-6295Crossref PubMed Google Scholar can be formed with monolayer precision showing variable lattice topology. The resulting 2D polymers (2DPs) have their properties tunable at the molecular level by using different monomers and polymerization chemistries. Besides, these in-plane and bonded molecular tilings can be assembled further through vdW interaction into vertical heterostructures and superlattices in a layer-by-layer fashion.13Jing Y. Heine T. Making 2D topological polymers a reality.Nat. Mater. 2020; 19: 823-824Crossref PubMed Scopus (5) Google Scholar2D inorganic and organic materials, individually and unambiguously, have demonstrated superior properties relative to their bulk materials. The rich molecular and synthetic polymer library arguably has the potential for expanding a novel family of organic/inorganic heterostructures in the 2D limit, without impeding the unique properties in a reduced dimension, while simultaneously combining advantages of the two material classes and compensating for their weaknesses. In this regard, the synthesis or formation of high-quality organic films, with extensive tunability derived from their molecular building blocks, on the basal plane of layered inorganic materials will advance the development of novel heterostructures with designed functionalities.14Gobbi M. Orgiu E. Samorì P. When 2D materials meet molecules: opportunities and challenges of hybrid organic/inorganic van der Waals heterostructures.Adv. Mater. 2018; 30: e1706103https://doi.org/10.1002/adma.201706103Crossref PubMed Scopus (127) Google Scholar This vibrant research field has shown multiple advantages even though it is still in its infancy stage. First, adding the chemical tunability of the 2D organics to 2D atomic crystals will lead to novel structures designed precisely at the molecular level and further tuned by interface interactions.15Jariwala D. Marks T.J. Hersam M.C. Mixed-dimensional van der Waals heterostructures.Nat. Mater. 2017; 16: 170-181Crossref PubMed Scopus (769) Google Scholar Second, the vdW heterostructures in the 2D limit enable fundamental studies of a range of phase transitions and physical processes, including charge carriers and excitonic dynamics, at the heterointerface. Particularly, as both constituents of a heterostructure are excitonic, with their excitons described in terms of Frenkel or Wannier-Mott limits according to the degree of exciton spatial localization and the surrounding dielectric environment,16Sharma A. Zhang L. Tollerud J.O. Dong M. Zhu Y. Halbich R. Vogl T. Liang K. Nguyen H.T. Wang F. et al.Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.Light Sci. Appl. 2020; 9: 116Crossref PubMed Scopus (11) Google Scholar,17Tartakovskii A. Excitons in 2D heterostructures.Nat. Rev. Phys. 2020; 2: 8-9Crossref Scopus (20) Google Scholar a profound understanding toward 2D excitons at the heterointerface will greatly richen the theoretical foundations and guide the design for advanced functional devices. Third, superior device performance and multifunctionalities have been realized already using the emergent vdW organic/inorganic heterostructures in the 2D limit, which will be addressed explicitly below.It should be noted that organic/inorganic heterostructures cover a broad structural range. According to the nature of the interfacial interaction, the resulting organic/inorganic 2D heterostructures can be divided into “vdW-bound” heterostructures and “covalently bound” heterostructures. The latter category, often associated with defect sites or metallic phases,18Voiry D. Goswami A. Kappera R. e Silva Cde C. Kaplan D. Fujita T. Chen M. Asefa T. Chhowalla M. Covalent functionalization of monolayered transition metal dichalcogenides by phase engineering.Nat. Chem. 2015; 7: 45-49Crossref PubMed Scopus (467) Google Scholar has been well summarized previously19Huang Y.L. Zheng Y.J. Song Z. Chi D. Wee A.T.S. Quek S.Y. The organic-2D transition metal dichalcogenide heterointerface.Chem. Soc. Rev. 2018; 47: 3241-3264Crossref PubMed Google Scholar and, thus, will not be further addressed here. Another important material category is hybrid organic/inorganic perovskites, with remarkable performance demonstrated in solar cells already.20Brenner T.M. Egger D.A. Kronik L. Hodes G. Cahen D. Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties.Nat. Rev. Mater. 2016; 1: 15007https://doi.org/10.1038/natrevmats.2015.7Crossref Scopus (818) Google Scholar Consisting of bulky organic cations sitting in large interstices between inorganic octahedra formed by lead (or tin) halides, this class of materials also allows rational engineering of optoelectronic, ferroelectricity, and a diverse range of physical properties, as has been summarized in excellent reviews already.21Leng K. Li R. Lau S.P. Loh K.P. Ferroelectricity and Rashba effect in 2D organic–inorganic hybrid perovskites.Trends in Chemistry. 2021; 3: 716-732https://doi.org/10.1016/j.trechmAbstract Full Text Full Text PDF Scopus (0) Google Scholar,22Leng K. Fu W. Liu Y. Chhowalla M. Loh K.P. From bulk to molecularly thin hybrid perovskites.Nat. Rev. Mater. 2020; 5: 482-500Crossref Scopus (50) Google Scholar The focus here is on combinations involving 2D materials that are characterized by covalent, coordination bonds or intermolecular interactions within each layer and noncovalent bonds between the layers. Besides, crossover to the 2D regime occurs at a thickness below 10 nm. Other structures including solution-cast polymer films with a thickness of tens/hundreds of nanometers on 2D inorganics, often applicable in energy-harvesting devices,3Sun J. Choi Y. Choi Y.J. Kim S. Park J.H. Lee S. Cho J.H. 2D–organic hybrid heterostructures for optoelectronic applications.Adv. Mater. 2019; 31: e1803831https://doi.org/10.1002/adma.201803831Crossref PubMed Scopus (45) Google Scholar are out of the scope of 2D limit and, thus, will not be addressed in detail herein.Given the increasing importance and rapid advances in this emergent research field combining organic and inorganic vdW materials in the 2D limit, we present here a timely and comprehensive review of their controlled synthesis, interface interactions, and device applications. We start by introducing the structure of individual inorganic and organic components in the 2D limit and effective approaches to form organic/inorganic heterostructures, mainly addressing the controlled assembly of 2D molecular films and synthesis and stacking of 2D polymers on atomically flat inorganic layers. We then examine the electronic and optical properties at the organic/inorganic heterointerfaces, including ground-state electronic properties, excited-state, and optical properties. Subsequently, we highlight applications of such emergent heterostructures with particular emphasis on advanced (opto)electronic, neuromorphic, and multifunctional devices showing superior performance that cannot be achieved by any of the material class alone (Figure 1). Finally, a personal reflection on how these exquisite designs combined with processing techniques will bring new understanding and application possibilities, and the future perspectives of this field are given.Individual componentsGraphene consists of a single layer of carbon atoms arranged in a honeycomb structure (Figure 2A),4Novoselov K.S. Geim A.K. Morozov S.V. Jiang D. Zhang Y. Dubonos S.V. Grigorieva I.V. Firsov A.A. Electric field effect in atomically thin carbon films.Science. 2004; 306: 666-669Crossref PubMed Scopus (46860) Google Scholar with superior electrical conductivity contributed by highly mobile π electrons (Figure 2B), as well as notable optical properties and high mechanical strength.23Geim A.K. Novoselov K.S. The rise of graphene.Nat. Mater. 2007; 6: 183-191Crossref PubMed Scopus (31146) Google Scholar Hexagonal boron nitride (h-BN) has a layered structure similar to graphite, with boron (B) and nitrogen (N) atoms bonded via sp2 orbitals to form strong σ bonds within each layer (Figure 2C). Different from the semi-metallic nature of graphene, h-BN is an electrical insulator and an essential component in 2D electronics, which provides high-quality and weakly interacting interfaces that preserve the electronic properties of adjacent materials.24Dean C.R. Young A.F. Meric I. Lee C. Wang L. Sorgenfrei S. Watanabe K. Taniguchi T. Kim P. Shepard K.L. Hone J. Boron nitride substrates for high-quality graphene electronics.Nat. Nanotechnol. 2010; 5: 722-726Crossref PubMed Scopus (4603) Google Scholar Transition metal dichalcogenides (TMDs) represent another group of 2D layered materials that differ from the single-carbon atomic-thick layer graphene consisting of a transition metal atom layer (M; e.g., Mo and W) sandwiched between two chalcogen atom layers (X; e.g., S, Se, and Te)25Lv R. Robinson J.A. Schaak R.E. Sun D. Sun Y. Mallouk T.E. Terrones M. Transition metal dichalcogenides and beyond: synthesis, properties, and applications of single- and few-layer nanosheets.Acc. Chem. Res. 2015; 48: 56-64Crossref PubMed Scopus (803) Google Scholar (Figure 2D). The alteration in filling of the nonbonding d orbitals of transition metal atoms and the hybridization of these with pz orbitals on chalcogen atoms result in considerable variability of the electronic properties of TMDs, many of which being semiconductors with an energy gap in the visible range.26Chhowalla M. Shin H.S. Eda G. Li L.J. Loh K.P. Zhang H. The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets.Nat. Chem. 2013; 5: 263-275Crossref PubMed Scopus (6211) Google ScholarFigure 2Structure of several 2D materialsShow full caption(A) Crystal structure of graphene.(B) Schematic of the covalent bonding in graphene, with in-plane σ -orbitals and out-of-plane π-orbitals formed by hybridization of the respective atomic orbitals. The electronic properties of graphene are dictated by π orbitals.(C) Crystal structure of a single-layer h-BN.(D) Crystal structure of a monolayer transition metal dichalcogenide with the chemical formula MX2, where M is a group IV, V, or VI transition metal (typically Mo, W), and X is a chalcogen (S, Se, or Te).View Large Image Figure ViewerDownload Hi-res image Download (PPT)The above-mentioned 2D materials are, thus, characterized by covalent bonds within each layer and weak, noncovalent bonds between the layers. Mono- and few-layer sheets of graphene, h-BN, and TMDs can be obtained by top-down or bottom-up approaches, including peeling apart individual layers from parent bulk crystals, synthesizing by wet-chemistry methods, or by chemical vapor deposition (CVD).27Tan C. Cao X. Wu X.J. He Q. Yang J. Zhang X. Chen J. Zhao W. Han S. Nam G.-H. et al.Recent advances in ultrathin two-dimensional nanomaterials.Chem. Rev. 2017; 117: 6225-6331Crossref PubMed Scopus (2463) Google Scholar While the 2D material family is still growing, this review mainly focuses on organic/inorganic heterostructures with graphene, TMDs, and h-BN as inorganic 2D components in recognition of their leading role in low-dimensional (opto)electronics.On the organic side, 2D and quasi-2D molecular crystals and films formed by self-assembly with under 10-nm thickness over a large area, whose surface features saturated bonds, have attracted considerable attention in the past decades.10Yang F. Cheng S. Zhang X. Ren X. Li R. Dong H. Hu W. 2D organic materials for optoelectronic applications.Adv. Mater. 2018; 30: 1702415Crossref Scopus (58) Google Scholar Representative conjugated molecules involved in the following discussions are listed in Figure 3A. Thin molecular films having thickness uniformity over a large scale, lateral continuity, and long-range intermolecular order were initially produced on crystalline metal surfaces in ultrahigh vacuum.28Forrest S.R. Ultrathin organic films grown by organic molecular beam deposition and related techniques.Chem. Rev. 1997; 97: 1793-1896Crossref PubMed Google Scholar The accessibility to ultrathin organic films has then been expanded with the development of solution processing.29Jiang L. Dong H. Meng Q. Li H. He M. Wei Z. He Y. Hu W. Millimeter-sized molecular monolayer two-dimensional crystals.Adv. Mater. 2011; 23: 2059-2063Crossref PubMed Scopus (87) Google Scholar These 2D molecular films with lateral dimensions even up to a millimeter range are held together by noncovalent intermolecular forces, mainly the π-π interactions. On the other hand, the structural anisotropy resulting from molecular shapes, engineered intermolecular interactions, and tunable molecule-substrate interactions can greatly alter the properties of such 2D molecular films. For instance, in a 2D film of the rod-like p-sexiphenyl, the molecular orientation can be changed from “upright standing” to “flat lying” by modifying the interaction strength with substrates, and the orientation has profound consequences for the ionization energy and electron affinity of the film.30Duhm S. Heimel G. Salzmann I. Glowatzki H. Johnson R.L. Vollmer A. Rabe J.P. Koch N. Orientation-dependent ionization energies and interface dipoles in ordered molecular assemblies.Nat. Mater. 2008; 7: 326-332Crossref PubMed Scopus (404) Google ScholarFigure 3Structures of representative organic molecules and 2D polymersShow full caption(A) Chemical structures of the organic molecules discussed in this article.(B) Schematic synthesis of a 2D polymer through Schiff-base condensation reaction at an interface. The chemical structures of the monomer and the resulting 2D polymer (predicted by calculations) are shown. Reprinted with permission from Sahabudeen et al.31Sahabudeen H. Qi H. Glatz B.A. Tranca D. Dong R. Hou Y. Zhang T. Kuttner C. Lehnert T. Seifert G. et al.Wafer-sized multifunctional polyimine-based two-dimensional conjugated polymers with high mechanical stiffness.Nat. Commun. 2016; 7: 13461Crossref PubMed Scopus (177) Google Scholar Copyright 2016 Nature Publishing Group.(C) Schematic synthesis of C2P-5. The chemical structures of TP-based monomers and the 2D COF (idealized without chemical and topological defects) are shown. Reprinted with permission from Jhulki et al.32Jhulki S. Kim J. Hwang I.-C. Haider G. Park J. Park J.Y. Lee Y. Hwang W. Dar A.A. Dhara B. et al.Solution-processable, crystalline π-conjugated two-dimensional polymers with high charge carrier mobility.Chem. 2020; 6: 1-2Abstract Full Text Full Text PDF Scopus (1) Google Scholar Copyright 2020 Elsevier.View Large Image Figure ViewerDownload Hi-res image Download (PPT)Graphene can be considered as a structurally defined, π-conjugated 2D polymer obtained from nature. Due to its remarkable properties that are homogeneous over a large area, graphene has also triggered considerable research interests in the rational design of synthetic 2D polymers.33Sakamoto J. van Heijst J. Lukin O. Schlüter A.D. Two-dimensional polymers: just a dream of synthetic chemists?.Angew. Chem. Int. Ed. Engl. 2009; 48: 1030-1069Crossref PubMed Scopus (560) Google Scholar Conceptually, 2D polymers comprise free-standing, atom/monomer-unit thin, and planar and covalent networks with well-defined in-plane periodicity.34Dong R. Zhang T. Feng X. Interface-assisted synthesis of 2D materials: trend and challenges.Chem. Rev. 2018; 118: 6189-6235Crossref PubMed Scopus (269) Google Scholar Early examples meeting the above criteria were achieved in 2012 by exfoliation of a lamellar polymer single crystal35Kissel P. Erni R. Schweizer W.B. Rossell M.D. King B.T. Bauer T. Götzinger S. Schlüter A.D. Sakamoto J. A two-dimensional polymer prepared by organic synthesis.Nat. Chem. 2012; 4: 287-291Crossref PubMed Scopus (271) Google Scholar and also by Ullmann coupling of porphyrin monomers under ultrahigh vacuum conditions on single-crystal metal surfaces.36Lafferentz L. Eberhardt V. Dri C. Africh C. Comelli G. Esch F. Hecht S. Grill L. Controlling on-surface polymerization by hierarchical and substrate-directed growth.Nat. Chem. 2012; 4: 215-220Crossref PubMed Scopus (389) Google Scholar Later on, various 2D covalently bonded networks were synthesized via exfoliation or interfacial reactions.37Liu W. Luo X. Bao Y. Liu Y.P. Ning G.H. Abdelwahab I. Li L. Nai C.T. Hu Z.G. Zhao D. et al.A two-dimensional conjugated aromatic polymer via C-C coupling reaction.Nat. Chem. 2017; 9: 563-570Crossref PubMed Scopus (184) Google Scholar,38Liu K. Qi H. Dong R. Shivhare R. Addicoat M. Zhang T. Sahabudeen H. Heine T. Mannsfeld S. Kaiser U. et al.On-water surface synthesis of crystalline, few-layer two-dimensional polymers assisted by surfactant monolayers.Nat. Chem. 2019; 11: 994-1000Crossref PubMed Scopus (102) Google Scholar Particularly, the air-water interface method could, in principle, offer an unlimited lateral size. To name an example, the Schiff-base condensation reaction at an air-water interface yields a 4-inch wafer-scale 2D conjugated polymer (Figure 3B) with a layer thickness of ∼ 0.7 nm, demonstrating semiconducting property due to the effective conjugation.31Sahabudeen H. Qi H. Glatz B.A. Tranca D. Dong R. Hou Y. Zhang T. Kuttner C. Lehnert T. Seifert G. et al.Wafer-sized multifunctional polyimine-based two-dimensional conjugated polymers with high mechanical stiffness.Nat. Commun. 2016; 7: 13461Crossref PubMed Scopus (177) Google ScholarIn particular, COFs are a class of porous polymeric materials, with controlled covalent bonds between molecules, thus providing predictable structures and long-ranging order.39Côté A.P. Benin A.I. Ockwig N.W. O’Keeffe M. Matzger A.J. Yaghi O.M. Porous, crystalline, covalent organic frameworks.Science. 2005; 310: 1166-1170Crossref PubMed Scopus (3488) Google Scholar,40Diercks C.S. Yaghi O.M. The atom, the molecule, and the covalent organic framework.Science. 2017; 355: eaal1585https://doi.org/10.1126/science.aal1585Crossref PubMed Scopus (836) Google Scholar 2D COFs are organic crystalline materials with predesigned π-electronic skeletons and highly ordered topological structures, with their building blocks arranged into periodic planar networks and having atomic precision in the vertical direction.41Geng K. He T. Liu R. Dalapati S. Tan K.T. Li Z. Tao S. Gong Y. Jiang Q. Jiang D. Covalent organic frameworks: design, synthesis, and functions.Chem. Rev. 2020; 120: 8814-8933Crossref PubMed Scopus (432) Google Scholar The high structural definition endows the 2D COF ordered π-electronic systems with the ability for good charge carrier transport, suggesting potential applications in optoelectronics. Theoretical investigations have predicted very high carrier mobility in such systems, potentially reaching values higher than that in the best molecular crystal semiconductors (95 cm2 V−1 s−1).42Thomas S. Li H. Dasari R.R. Evans A.M. Castano I. Allen T.G. Reid O.G. Rumbles G. Dichtel W.R. Gianneschi N.C. et al.Design and synthesis of two-dimensional covalent organic frameworks with four-arm cores: prediction of remarkable ambipolar charge-transport properties.Mater. Horiz. 2019; 6: 1868-1876Crossref Google Scholar However, experimental investigation of electronic properties of those materials is still limited, mainly due to persistent challenges in obtaining high-quality thin films (most investigations so far were done on bulk crystals or pressed pellets of powders) with large grain sizes. Furthermore, steric hindrance on a substrate can result in limited in-plane π-conjugation. Very recently, fully π-conjugated, highly crystalline 2D COFs were realized via covalent stitching of triphenylene (TP) derivatives through the formation of pyrazine motif, without any aid of template or preorganization in solution (Figure 3C). The resulting long-range ordered structure of C2P-5 (“C2P” stands for “conjugated 2D polymer,” and 5 represents the number of aromatic units in each arm of the hexagonal lattice) allows reaching a hole mobility of 4.0 cm2 V−1 s−1, the highest value among all synthetic 2D polymers to date.32Jhulki S. Kim J. Hwang I.-C. Haider G. Park J. Park J.Y. Lee Y. Hwang W. Dar A.A. Dhara B. et al.Solution-processable, crystalline π-conjugated two-dimensional polymers with high charge carrier mobility.Chem. 2020; 6: 1-2Abstract Full Text Full Text PDF Scopus (1) Google ScholarGenerally, a 2D or quasi-2D nature of organic materials gives rise to unique properties including but not limited to the following aspects: (1) charges can exhibit band-like transport due to the long-range order if dipolar disorder and interfacial coupling can be minimized,43Zhang Y. Qiao J. Gao S. Hu F. He D. Wu B. Yang Z. Xu B. Li Y. Shi Y. et al.Probing carrier transport and structure-property relationship of highly ordered organic semiconductors at the two-dimensional limit.Phys. Rev. Lett. 2016; 116: 016602Crossref PubMed Scopus (0) Google Scholar (2) strong light-matter coupling with high absorption coefficients,44Hertzog M. Wang M. Mony J. Börjesson K. Strong light-matter interactions: a new direction within chemistry.Chem. Soc. Rev. 2019; 48: 937-961Crossref PubMed Google Scholar and (3) high sensitivity to external stimuli, including environmental molecular species by the direct exposure of conductive channel and a large surface-to-volume ratio.45Li C. Wu H. Zhang T. Liang Y. Zheng B. Xia J. Xu J. Miao Q. Functionalized π stacks of hexabenzoperylenes as a platform for chemical and biological sensing.Chem. 2018; 4: 1416-1426Abstract Full Text Full Text PDF Scopus (0) Google Scholar These unique features have allowed great feasibility in tuning electrical and optical properties when forming heterostructures with 2D inorganic materials via engineering the interface and the device structure as discussed further on.Formation of van der Waals heterostructuresSynthesizing two materials with disparate atomic arrangements and thermal stability in a single process is exceedingly challenging.46Wang Q.H. Hersam M.C. Room-temperature molecular-resolution characterization of self-assembled organic monolayers on epitaxial graphene.Nat. Chem. 2009; 1: 206-211Crossref PubMed Scopus (373) Google Scholar Therefore, organic/inorganic 2D heterostructures are mostly formed by depositing or synthesizing the organic components on the already prepared 2D substrates that are usually chemically and thermally more stable. A less commonly utilized approach is to physically transfer organic crystals using a micromanipulator and stacking it on top of a 2D substrate.47Park C.-J. Seo C. Kim J. Joo J. Variation of photoluminescence of organic semiconducting-rubrene microplate depending" @default.
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• W3200380859 title "Van der Waals organic/inorganic heterostructures in the two-dimensional limit" @default.
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