PubMed İndeksli Yayınlar Koleksiyonu / PubMed Indexed Publications Collection
Permanent URI for this collectionhttps://hdl.handle.net/11147/7645
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Article Citation - WoS: 32Citation - Scopus: 31Wien Effect in Interfacial Water Dissociation Through Proton-Permeable Graphene Electrodes(Nature Research, 2022) Cai, Junhao; Griffin, Eoin; Guarochico-Moreira, Victor H.; Barry, D.; Xin, B.; Yağmurcukardeş, Mehmet; Zhang, Sheng; Geim, Andre K.; Peeters, François M.; Lozada-Hidalgo, MarceloStrong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 107 V m−1, sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O ⇆ H+ + OH−) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 108 V m−1. The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager’s theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport.Article Citation - WoS: 40Citation - Scopus: 38Gas Permeation Through Graphdiyne-Based Nanoporous Membranes(Nature Research, 2022) Zhou, Zhihua; Tan, Yongtao; Yang, Qian; Bera, Achintya; Xiong, Zecheng; Yağmurcukardeş, Mehmet; Kim, MinsooNanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeance. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of ∼0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale.Article Citation - WoS: 6Citation - Scopus: 7Interface-Dependent Phononic and Optical Properties of Geo/Moso Heterostructures(Royal Society of Chemistry, 2022) Yağmurcukardeş, Mehmet; Sözen, Yiğit; Başkurt, Mehmet; Peeters, François M.; Şahin, HasanThe interface-dependent electronic, vibrational, piezoelectric, and optical properties of van der Waals heterobilayers, formed by buckled GeO (b-GeO) and Janus MoSO structures, are investigated by means of first-principles calculations. The electronic band dispersions show that O/Ge and S/O interface formations result in a type-II band alignment with direct and indirect band gaps, respectively. In contrast, O/O and S/Ge interfaces give rise to the formation of a type-I band alignment with an indirect band gap. By considering the Bethe-Salpeter equation (BSE) on top of G0W0 approximation, it is shown that different interfaces can be distinguished from each other by means of the optical absorption spectra as a consequence of the band alignments. Additionally, the low-and high-frequency regimes of the Raman spectra are also different for each interface type. The alignment of the individual dipoles, which is interface-dependent, either weakens or strengthens the net dipole of the heterobilayers and results in tunable piezoelectric coefficients. The results indicate that the possible heterobilayers of b-GeO/MoSO asymmetric structures possess various electronic, optical, and piezoelectric properties arising from the different interface formations and can be distinguished by means of various spectroscopic techniques.Article Citation - WoS: 62Citation - Scopus: 59Exponentially Selective Molecular Sieving Through Angstrom Pores(Nature Publishing Group, 2021) Sun, Pengzhan; Yağmurcukardeş, Mehmet; Zhang, R.; Kuang, Wenjun; Lozada-Hidalgo, Marcelo; Liu, B. L.; Geim, Andre K.Two-dimensional crystals with angstrom-scale pores are widely considered as candidates for a next generation of molecular separation technologies aiming to provide extreme, exponentially large selectivity combined with high flow rates. No such pores have been demonstrated experimentally. Here we study gas transport through individual graphene pores created by low intensity exposure to low kV electrons. Helium and hydrogen permeate easily through these pores whereas larger species such as xenon and methane are practically blocked. Permeating gases experience activation barriers that increase quadratically with molecules’ kinetic diameter, and the effective diameter of the created pores is estimated as ∼2 angstroms, about one missing carbon ring. Our work reveals stringent conditions for achieving the long sought-after exponential selectivity using porous two-dimensional membranes and suggests limits on their possible performance.Article Citation - WoS: 35Citation - Scopus: 40Two-Dimensional Covalent Crystals by Chemical Conversion of Thin Van Der Waals Materials(American Chemical Society, 2019) Sreepal, Vishnu; Yağmurcukardeş, Mehmet; Vasu, Kalangi S.; Kelly, Daniel J.; Taylor, Sarah F. R.; Şahin, Hasan; Kravets, Vasyl G.; Nair, Rahul R.Most of the studied two-dimensional (2D) materials have been obtained by exfoliation of van der Waals crystals. Recently, there has been growing interest in fabricating synthetic 2D crystals which have no layered bulk analogues. These efforts have been focused mainly on the surface growth of molecules in high vacuum. Here, we report an approach to making 2D crystals of covalent solids by chemical conversion of van der Waals layers. As an example, we used 2D indium selenide (InSe) obtained by exfoliation and converted it by direct fluorination into indium fluoride (InF3), which has a nonlayered, rhombohedral structure and therefore cannot possibly be obtained by exfoliation. The conversion of InSe into InF3 is found to be feasible for thicknesses down to three layers of InSe, and the obtained stable InF3 layers are doped with selenium. We study this new 2D material by optical, electron transport, and Raman measurements and show that it is a semiconductor with a direct bandgap of 2.2 eV, exhibiting high optical transparency across the visible and infrared spectral ranges. We also demonstrate the scalability of our approach by chemical conversion of large-area, thin InSe laminates obtained by liquid exfoliation, into InF3 films. The concept of chemical conversion of cleavable thin van der Waals crystals into covalently bonded noncleavable ones opens exciting prospects for synthesizing a wide variety of novel atomically thin covalent crystals.