Molecular Functionalization and Emergence of Long-range Spin-dependent Phenomena in Two-dimensional (2D) Carbon Nanotube Networks Rahman, Md. Wazedur Mañas Torres, María del Carmen Firouzeh, Seyedamin Cuerva Carvajal, Juan Manuel Álvarez Cienfuegos Rodríguez, Luis Pramanik, Sandipan Chirality-induced spin selectivity Carrier transport Carbon nanotube Peptides Spin−orbit coupling Molecular functionalization of CNTs is a routine procedure in the field of nanotechnology. However, whether and how these molecules affect the spin polarization of the charge carriers in CNTs are largely unknown. In this work we demonstrate that spin polarization can indeed be induced in twodimensional (2D) CNT networks by “certain” molecules and the spin signal routinely survives length scales significantly exceeding 1 μm. This result effectively connects the area of molecular spintronics with that of carbon-based 2D nanoelectronics. By using the versatility of peptide chemistry, we further demonstrate how spin polarization depends on molecular structural features such as chirality as well as molecule−nanotube interactions. A chiralityindependent effect was detected in addition to the more common chiralitydependent effect, and the overall spin signal was found to be a combination of both. Finally, the magnetic field dependence of the spin signals has been explored, and the “chirality-dependent” signal has been found to exist only in certain field angles. 2022-05-10T06:51:16Z 2022-05-10T06:51:16Z 2021-12-06 info:eu-repo/semantics/article ACS Nano 2021, 15, 20056−20066 http://hdl.handle.net/10481/74765 10.1021/acsnano.1c07739 eng http://creativecommons.org/licenses/by-nc-nd/3.0/ info:eu-repo/semantics/openAccess Creative Commons Attribution-NonCommercial-NoDerivs 3.0 License ACS