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Patterning Nanoroads and Quantum Dots on Fluorinated Graphene*

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Patterning Nanoroads and Quantum Dots on Fluorinated Graphene* Patterning Nanoroads and Quantum Dots on Fluorinated Graphene* Morgana A. Ribas1, Abhishek K. Singh1, 2, Pavel B. Sorokin1, and Boris I. Yakobson1# 1 Department of Mechanical Engineering and Materials Science and Department of Chemistry, Rice University, Houston, Texas 77005, USA 2 Materials Research Centre, Indian Institute of Science, Bangalore 560012, India #Corresponding author: [email protected] Using ab initio methods we have investigated the fluorination of graphene and find that different stoichiometric phases can be formed without a nucleation barrier, with the complete “2D-Teflon” CF phase being thermodynamically most stable. The fluorinated graphene is an insulator and turns out to be a perfect matrix-host for patterning nanoroads and quantum dots of pristine graphene. The electronic and magnetic properties of the nanoroads can be tuned by varying the edge orientation and width. The energy gaps between the highest occupied and lowest unoccupied molecular orbitals (HOMO–LUMO) of quantum dots are size-dependent and show a confinement typical of Dirac fermions. Furthermore, we study the effect of different basic coverage of F on graphene (with stoichiometries CF and C4F) on the band gaps, and show the suitability of these materials to host quantum dots of graphene with unique electronic properties. Keywords: Graphene, fluorinated graphene, fluorographene, nanoroads, quantum dots *Nano Research, 4 (2011) 143-152. http://www.springerlink.com/content/j6451747047qx668/ The original publication is available at www.springerlink.com. 1 1. Introduction as hydrogen storage materials, and has been experimentally observed [26, 27]. However, a After the first experimental evidence of graphene [1], nucleation barrier exists in the initial steps of research on its properties and applications has hydrogenation of graphene and it is desirable to find continued to grow with unprecedented pace. a similar or even more favorable element which can However, a great deal remains to be done to fully transform graphene into a semiconducting material. incorporate graphene’s unique properties into electronic devices. The rapid advances in fabrication Here we explore the functionalization of graphene methods [2–5] have now made it possible to produce by fluorine, which results in compositions similar to graphene on a large scale. The major obstacle to its Teflon -(CF2)n-, which in a 2-dimensional incarnation application in electronic devices is the lack of a corresponds to -(CF)n-. The biggest advantage of consistent method to open the zero band gap of fluorination of graphene comes from the shear graphene in a controlled fashion. availability of experimental and theoretical research that has been done on fluorinated graphite [28–39] The use of graphene nanoribbons has been and fluorinated carbon nanotubes [40–45]. This proposed as a way to tune graphene’s electronic knowledge base can help devise ways of controllable properties [6–9]. Depending upon their width and fluorination of graphene. Depending on the edge orientation, graphene nanoribbons can be either experimental conditions and reactant gases, different metallic or semiconducting [10–14]. Though there stoichiometries (e.g., (CF) [46], (C F) [29], and (C F) has been intensive research on nanoribbon n 2 n 4 n [47]) can be obtained. Therefore, unlike fabrication, it is still difficult to obtain ribbons with hydrogenation, fluorination can offer several well-defined edges (e.g., by chemical methods [9, 15, promising functionalized phases to serve as host 16]) or to scale up its production (e.g., by carbon materials for graphene nanoroads and quantum dots. nanotube unzipping [17, 18]). Even a bottom-up Thus, the wide range of possible chemical reactions approach [19] does not solve the challenge of involving fluorinated graphitic materials, in assembling graphene nanoribbons into functional combination with possibility of tunable electronic devices. properties of patterned graphene structures, opens A recently explored alternative way to tune the the door to a range of exciting applications. band gap is to use a fully hydrogenated graphene [20] Using ab initio methods, we have carried out a (also known as graphane [21]) as a matrix-host in comparative study of the formation of CF, C F, and which graphene nanoroads [22] or quantum dots [23] 2 C F (shown in Fig. 1) by chemisorption of F atoms on are patterned. As is the case for graphene 4 graphene. Based on the formation energies, CF is the nanoribbons, the electronic properties of such roads most favorable, and its formation does not have a and dots are width- and orientation-dependent. nucleation barrier, in contrast to the barrier observed However, their biggest advantage over nanoribbons for the formation of graphane. We further show that is that both semiconducting and metallic elements nanoroads and quantum dots of graphene can be can be patterned and interconnected on the same patterned on these substrates; these exhibit tunable graphene sheet, without compromising its electronic and magnetic properties, and offer a mechanical integrity. This new approach has already variety of applications. been attempted experimentally [24] and has potential to quickly rival graphene ribbons. 2. Calculation methods The nanoroads and quantum dots can be patterned on any insulating functionalized graphene, The calculations were carried out using ab initio e.g., graphane. The formation energy of graphane density functional theory (DFT), as implemented in lies within a favorable and reversible range [25]. This the Vienna ab initio package simulation (VASP) [48, reversibility is very important for applications such 49]. Spin polarized calculations were performed 2 using the projected augmented wave (PAW) method are analyzed here. Furthermore, we examine [50, 51] and Perdew–Burke–Ernzerhof (PBE) [52] structures of single-sided (Fig. 1(c)) and approximation for the exchange and correlation, double-sided fluorinated C4F [38, 47]. with plane wave kinetic energy cutoff of 400 eV. Considering the fluorination to occur through the Periodic boundary conditions were used, and the simple reaction x C + y/2 F2 CxFy, we calculate the system was considered optimized when the residual formation energies (Ef) of these four structures (Table forces were less than 0.005 eV/Å. The unit cells 1), where , is lengths of CxFy and nanoroads were fully optimized. the energy of CxFy, EC and are the energies of a The Brillouin zone integrations were carried out C atom on graphene and F , respectively, and x and y using a 15 x 15 x 1 Monkhorst–Pack k-grid for the 2 are the number of C and F atoms, respectively. The C F , 1 x 1 x 5 for the nanoroads, and at the Γ point x y formation of CF is more favorable than C F and C F. for the clusters. 2 4 The formation energy decreases with increasing F For the quantum dots, the total energies for n = coverage. For C2F, AB stacking is energetically more 1–384 were calculated using a density functional based tight-binding method (DF–TB) with the corresponding Slater–Koster parameters [53], as implemented in the DFTB+ code [54]. Initially we tested several non-equivalent geometries for the smallest dots (n < 7) and observed that the lowest energy structures were generally derived from n–1 structures. The DF–TB results were tested by comparing the formation energies of the smaller dots (n = 1–24) on a finite fully fluorinated graphene cluster (C54F72) by DFT calculations (as described above). To mimic an infinite sp3 CF, the edge C atoms of the cluster were passivated with two F atoms and kept constrained during the simulation of the dots. In all calculations sufficient vacuum space was kept between the periodic images to avoid spurious interactions. 3. Results and discussion 3.1 Structure and electronic properties The structure of the fluorinated graphite, based on X-ray diffraction results, has long been believed to consist of trans-linked cyclohexane chairs of fluoridated sp3 carbon [28, 29, 36, 37]. Such a structure was later confirmed by DFT calculations [55], and it is the one used here to represent CF (Fig. 1(a)). There are two possible stacking sequences for Figure 1 The atomic structures (darker atoms are closer; red dashed lines mark the unit cells) of (a) CF, (b) C2F for AB (C2F)n: AB/A′B′ and AA′/AA′ [29, 33], where the stacking, and (c) C F for double-sided fluorination, and (d)–(f) prime and slash indicate a mirror symmetry and the 4 the corresponding electronic band structures. CF and C2F AB presence of covalently bonded fluorine atoms, have a direct band gap at the Γ-point, 3.12 eV and 3.99 eV, respectively. Both AB (Fig. 1(b)), and AA′ (not shown) respectively, whereas C4F has an indirect band gap of 2.94 eV. 3 favorable than AA′. The formation energies for C4F Graphene’s gapless electronic structure changes with single- and double-sided fluorination are very completely after fluorination. A finite gap appears in similar, within the error of the calculation. the electronic band structure of CF, C2F, and C 4F (Figs. The length of the C–F bond in molecular species is 1(d)–1(f), respectively), transforming them into wide 1.47 Å, and the C-F bond strength is partially band gap semiconductors. The electronic band attributed to its highly polarized nature. As a result, structure of CF shows a 3.12 eV direct band gap at fluorocarbons have been widely explored in organic the Γ point, agreeing well with previously reported chemistry for a variety of applications [32, 56–58]. values [47, 55, 60]. The band gaps of C2F for both stacking sequences are very similar, which is as The calculated C–F bond lengths in CF and C2F are 1.38 Å in each case and agree well with both expected due to the similarities in their structures. experimental (1.41 Å) [33, 37] and theoretical (1.37 Å) Recent experiments on graphene fluorination yielded an optically transparent C F with a 2.93 eV [55] values.
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