A tool box to ascertain the nature of doping and photoresponse in single-walled carbon nanotubes
6 Figuras. 3 Tablas. ; The effect of doping on the electronic properties in bulk single-walled carbon nanotube (SWCNT) samples is studied for the first time using a new in situ Raman spectroelectrochemical method, and further verified by DFT calculations and photoresponse. We use p-/n-doped SWCNTs prepared by diazonium reactions as a versatile chemical strategy to control the SWCNT behavior. The measured and calculated data testify an acceptor effect of 4-aminobenzenesulfonic acid (p-doping), and a donor effect (n-doping) in the case of benzyl alcohol. In addition, pristine and covalently functionalized SWCNTs were used for the preparation of photoactive film electrodes. The photocathodic current in the photoelectrochemical cell is consistently modulated by the doping group. These results validate the in situ Raman spectroelectrochemistry as a unique tool box for predicting the electronic properties of functionalized SWCNTs in the form of thin films and their operational functionality in thin film devices for future optoelectronic applications. ; The authors acknowledge financial support from the European Union FP7 RADDEL programme (ITN Marie Curie Actions PEOPLE-2011-290023) and the MEYS Inter Excellence Project no. LTC18039 and H2020-MSCA RISE Agreement no. 734834 (INFUSION). This work at the Instituto de Carboquímica has been funded by the MINECO and the European Regional Development Fund (ENE 2016-79282-C5-1-R), the Government of Aragon (T03-17R), and the European Commission (H2020-MSCA-ITN-2014-ETN 642742 'Enabling Excellence'). The work in Mons is supported by the European Union H2020 iSwitch programme (H2020-MSCA-ITN-2014-ETN 642196). Computational resources in Mons were provided by the Consortium des Équipements de Calcul Intensif (CÉCI) funded by the Belgian National Fund for Scientific Research (F.R.S.-FNRS) under Grant 2.5020.11. J. C. is an FNRS research director. The authors acknowledge the assistance provided by the Research Infrastructures NanoEnviCz (Project No. LM2015073) supported by the Ministry of Education, Youth and Sports of the Czech Republic and the project Pro-NanoEnviCz (Reg. no. CZ.02.1.01/0.0/0.0/16_013/0001821) supported by the Ministry of Education, Youth and Sports of the Czech Republic and the European Union – European Structural and Investments Funds in the frame of Operational Programme Research Development and Education. J. M. G.-D. is grateful to Spanish Ministry of Science, Innovation and Universities for his 'Juan de la Cierva – Incorporación' research grant. A. S. is grateful to Dr Sara Costa and Dr Johan Ek Weis for fruitful discussions and helpful comments. ; We also acknowledge institutional support from the Unit of Information Resources for Research at the "Consejo Superior de Investigaciones Científicas" (CSIC) for the article-processing charges contribution ; Peer reviewed