Theoretical investigation of silicon nanowires: Methodology, geometry, surface modification, and electrical conductivity using a multiscale approach Man-Fai Ng, 1 Liping Zhou, 1,2 Shuo-Wang Yang, 1, * Li Yun Sim, 1 Vincent B. C. Tan, 2 and Ping Wu 1 1 Institute of High Performance Computing, 1 Science Park Road, #01-01 The Capricorn, Singapore 117528, Singapore 2 Department of Mechanical Engineering, National University of Singapore, Singapore 117576, Singapore Received 23 April 2007; revised manuscript received 26 June 2007; published 29 October 2007 The structural and electronic properties of hydrogenated silicon nanowires SiNWsoriented in 100, 110, 111, and 112directions are investigated systematically using a multiscale approach: geometry optimization is done by a semiempirical method and electronic band structure is calculated by density-functional theory with Gaussian basis set. The calculated band gaps agree very well with the available experimental data. We propose that the multiscale approach is an accurate and effective way for calculating the structural and electronic properties of SiNWs with diameter up to 3 nm. Besides, we found that surface modification of the SiNWs using the hydroxyl and fluoro groups can strongly reduce the band gap by as much as 1 eV, and more interestingly, alter the gap nature. On the contrary, the 110SiNWs exhibiting different patterns at the cross section do not show significant difference in their band gaps 0.09 eV, indicating that the electronic struc- tures of SiNWs are much more sensitive to surface modification than the change of cross section. Moreover, SiNWs of different orientations exhibit different degrees of band gap reduction upon surface modification, in which the 110SiNW demonstrates the highest sensitivity. The result indicates that SiNWs oriented in 110 direction are the better candidate for sensor application. On the contrary, the 111SiNW is found to be very tight to structural change with diameter and the most reluctant to surface modification, showing that it is structurally stable and rather inert. In addition, from the I-V curves of the SiNWs with surfaces modified with hydroxyl groups, which are calculated by the nonequilibrium Green’s function theory, we found that the electrical conductivity of the SiNWs is highly chemical sensitive. Besides, the phenomenon of negative dif- ferential resistance is observed in the I-V curves. DOI: 10.1103/PhysRevB.76.155435 PACS numbers: 73.22.f I. INTRODUCTION The intrinsic characteristics of silicon nanowire SiNW such as one dimensionality, high surface-to-volume ratio, biocompatibility, as well as the tunable band gap make it a unique and special class of semiconductors. More impor- tantly, because of its interface compatibility with the existing silicon-based technology and the intensive pursuits of the miniaturization of silicon electronic, 1 the development of SiNW appears to be a natural choice. In fact, SiNWs have been successfully synthesized and have already been utilized in various applications such as field-effect transistors, 25 chemical and biological sensors, 6,7 complementary metal- oxide semiconductor devices, 8 as well as for developing op- tical and photonic devices. 9 Currently, most applications make use of SiNWs with diameters of few tens nanometer. However, SiNWs with diameters of few nanometer can be- come more important in application not only due to the size matter but also for the fact that small diameter SiNWs ex- hibit unique properties because of the growth orientation and the pronounced quantum confinement effect. SiNWs below 10 nm in diameter have been synthesized recently by various techniques. 1014 These SiNWs exhibit various diameter distributions and growth orientations. In particular, the solution techniques employed by Holmes et al. 11 produced SiNWs with 4 – 5 nm in diameter that oriented in 100and 110directions. Cui et al. 12 reported that SiNWs grown by a vapor-liquid-solid mechanism have a range of diameters from 6 to 31 nm with 110and 111 growth orientations. Ma et al. 13 adopted the oxide-assisted catalyst-free method, by which the 110and 112SiNWs are grown with diameters ranged from 1.3 to 7 nm. Wu et al. 14 obtained SiNWs with 110, 111, and 112growth orientations down to 3 nm in diameter by employing the chemical vapor deposition method using gold nanocluster as catalyst. Normally the synthesized SiNWs are coated with an oxide layer. Hydrogenated SiNWs can be obtained after re- moving the oxide layer by hydrofluoric acid treatment. It is noted from these experimental results that the 110SiNW is the most commonly produced by these “bottom-up” syn- thetic strategies with diameter as small as 3 nm. The occur- rence of the 111and 112SiNWs tends to be more tech- nique dependent. The 100SiNW is relatively less reported. Nevertheless, these experiments show that 110, 111, 112, and 100are the most important and the most com- mon growth orientations for small diameter SiNWs. Understanding the electronic properties of SiNW within the quantum confined regime 3 nm diametervia theoret- ical studies is important for two reasons: iit is still difficult for the experimentalists to synthesize SiNWs with such small diameters and thus their properties have only been partially determined by experiments, and iiSiNWs within this re- gime have larger band gaps that can extend their functional- ity and they are also more unique. For instance, the elec- tronic structures of SiNWs of different growth orientations within this regime are more differentiated. The calculated results can thus provide more guidelines for the band gap engineering purposes. In fact, the electronic properties of SiNWs have been extensively investigated theoretically with respect to diameters, growth orientations, morphologies, sur- face modifications, and doping effects. 1526 Moreover, the optical properties, 2729 structural stability, 3034 and electrical properties 35 have also been reported. PHYSICAL REVIEW B 76, 155435 2007 1098-0121/2007/7615/15543511©2007 The American Physical Society 155435-1