Kwon Hyejin, Furmanchuk Al'ona, Kim Mijin, Meany Brendan, Guo Yong, Schatz George C, Wang YuHuang
Department of Chemistry and Biochemistry, University of Maryland , College Park, Maryland 20742, United States.
Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States.
J Am Chem Soc. 2016 Jun 1;138(21):6878-85. doi: 10.1021/jacs.6b03618. Epub 2016 May 17.
We describe the chemical creation of molecularly tunable fluorescent quantum defects in semiconducting carbon nanotubes through covalently bonded surface functional groups that are themselves nonemitting. By variation of the surface functional groups, the same carbon nanotube crystal is chemically converted to create more than 30 distinct fluorescent nanostructures with unique near-infrared photoluminescence that is molecularly specific, systematically tunable, and significantly brighter than that of the parent semiconductor. This novel exciton-tailoring chemistry readily occurs in aqueous solution and creates functional defects on the sp(2) carbon lattice with highly predictable C-C bonding from virtually any iodine-containing hydrocarbon precursor. Our new ability to control nanostructure excitons through a single surface functional group opens up exciting possibilities for postsynthesis chemical engineering of carbon nanomaterials and suggests that the rational design and creation of a large variety of molecularly tunable quantum emitters-for applications ranging from in vivo bioimaging and chemical sensing to room-temperature single-photon sources-can now be anticipated.
我们描述了通过本身不发光的共价键合表面官能团在半导体碳纳米管中化学创建分子可调谐荧光量子缺陷的方法。通过改变表面官能团,同一碳纳米管晶体被化学转化,以创建30多种具有独特近红外光致发光的不同荧光纳米结构,这些光致发光具有分子特异性、系统可调性,并且比母体半导体的光致发光亮得多。这种新颖的激子剪裁化学很容易在水溶液中发生,并在sp(2)碳晶格上产生功能缺陷,这些缺陷具有来自几乎任何含碘烃前体的高度可预测的C-C键。我们通过单个表面官能团控制纳米结构激子的新能力为碳纳米材料的合成后化学工程开辟了令人兴奋的可能性,并表明现在可以预期合理设计和创建各种分子可调谐量子发射器,其应用范围从体内生物成像和化学传感到室温单光子源。