Unveiling the Multiradical Character of the Biphenylene Network and Its Anisotropic Charge Transport

被引:28
作者
Alcon, Isaac [3 ,4 ,8 ]
Calogero, Gaetano [1 ]
Papior, Nick [2 ]
Antidormi, Aleandro [3 ,4 ]
Song, Kenan [5 ]
Cummings, Aron W. [3 ,4 ]
Brandbyge, Mads [6 ,7 ]
Roche, Stephan [3 ,4 ,9 ]
机构
[1] CNR Inst Microelect & Microsyst CNR IMM, I-95121 Catania, Italy
[2] Tech Univ Denmark, Comp Ctr, DK-2800 Lyngby, Denmark
[3] Catalan Inst Nanosci & Nanotechnol ICN2, CSIC, Barcelona 08193, Spain
[4] BIST, Barcelona 08193, Spain
[5] King Abdullah Univ Sci & Technol KAUST, Phys Sci & Engn Div, Thuwal 23955, Saudi Arabia
[6] Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark
[7] Ctr Nanostruct Graphene CNG, DK-2800 Lyngby, Denmark
[8] Free Univ Berlin, Inst Chem & Biochem Phys & Theoret Chem, D-14195 Berlin, Germany
[9] ICREA Inst Catalana Recerca & Estudis Avancats, Barcelona 08070, Spain
基金
新加坡国家研究基金会;
关键词
ELECTRONIC-PROPERTIES; CARBON; GRAPHENE; GRAPHYNE; POLYMER; RINGS;
D O I
10.1021/jacs.2c02178
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Recent progress in the on-surface synthesis and characterization of nanomaterials is facilitating the realization of new carbon allotropes, such as nanoporous graphenes, graphynes, and 2D pi-conjugated polymers. One of the latest examples is the biphenylene network (BPN), which was recently fabricated on gold and characterized with atomic precision. This gapless 2D organic material presents uncommon metallic conduction, which could help develop innovative carbon-based electronics. Here, using first principles calculations and quantum transport simulations, we provide new insights into some fundamental properties of BPN, which are key for its further technological exploitation. We predict that BPN hosts an unprecedented spin-polarized multiradical ground state, which has important implications for the chemical reactivity of the 2D material under practical use conditions. The associated electronic band gap is highly sensitive to perturbations, as seen in finite temperature (300 K) molecular dynamics simulations, but the multiradical character remains stable. Furthermore, BPN is found to host in-plane anisotropic (spin-polarized) electrical transport, rooted in its intrinsic structural features, which suggests potential device functionality of interest for both nanoelectronics and spintronics.
引用
收藏
页码:8278 / 8285
页数:8
相关论文
共 72 条
[1]   Toward reliable density functional methods without adjustable parameters: The PBE0 model [J].
Adamo, C ;
Barone, V .
JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (13) :6158-6170
[2]   The electronic and transport properties of two-dimensional conjugated polymer networks including disorder [J].
Adjizian, Jean-Joseph ;
Lherbier, Aurelien ;
Dubois, Simon M. -M. ;
Botello-Mendez, Andres Rafael ;
Charlier, Jean-Christophe .
NANOSCALE, 2016, 8 (03) :1642-1651
[3]   Dirac Cones in two-dimensional conjugated polymer networks [J].
Adjizian, Jean-Joseph ;
Briddon, Patrick ;
Humbert, Bernard ;
Duvail, Jean-Luc ;
Wagner, Philipp ;
Adda, Coline ;
Ewels, Christopher .
NATURE COMMUNICATIONS, 2014, 5
[4]  
Alcon I., J PHYS CHEM LETT, V2021, P11220
[5]   Electrochemical Control of Charge Current Flow in Nanoporous Graphene [J].
Alcon, Isaac ;
Calogero, Gaetano ;
Papior, Nick ;
Brandbyge, Mads .
ADVANCED FUNCTIONAL MATERIALS, 2021, 31 (40)
[6]   Conformational control over π-conjugated electron pairing in 1D organic polymers [J].
Alcon, Isaac ;
Shao, Jingjing ;
Tremblay, Jean Christophe ;
Paulus, Beate .
RSC ADVANCES, 2021, 11 (33) :20498-20506
[7]   Controlling pairing of π-conjugated electrons in 2D covalent organic radical frameworks via in-plane strain [J].
Alcon, Isaac ;
Santiago, Raul ;
Ribas-Arino, Jordi ;
Deumal, Merce ;
Moreira, Iberio de P. R. ;
Bromley, Stefan T. .
NATURE COMMUNICATIONS, 2021, 12 (01)
[8]   Existence of multi-radical and closed-shell semiconducting states in post-graphene organic Dirac materials [J].
Alcon, Isaac ;
Vines, Francesc ;
Moreira, Iberio de P. R. ;
Bromley, Stefan T. .
NATURE COMMUNICATIONS, 2017, 8
[9]   Design of multi-functional 2D open-shell organic networks with mechanically controllable properties [J].
Alcon, Isaac ;
Reta, Daniel ;
Moreira, Iberio de P. R. ;
Bromley, Stefan T. .
CHEMICAL SCIENCE, 2017, 8 (02) :1027-1039
[10]  
Amnon Yariv P.Y., 2002, Optical Waves in Crystals: Propagation and Control of Laser Radiation