J. A. Golovchenko

Harvard University, Cambridge, MA, United States

Are you J. A. Golovchenko?

Claim your profile

Publications (148)946.79 Total impact

  • [Show abstract] [Hide abstract]
    ABSTRACT: We fabricate a nanopore in a suspended single-layer graphene membrane, which serves as a barrier between two aqueous DNA reservoirs. This nanopore device can detect the electrophoretic passage of single or double stranded DNA through transient ionic current blockades caused by DNA obstruction of the pore. Furthermore, a graphene pore, which has atomic thickness, should allow discrimination of different DNA base pairs by ionic current measurements alone. This base discrimination can become the basis of a single-molecule, ultrafast DNA sequencing scheme. We demonstrate the fabrication and evaluate the performance of these graphene nanopore devices.
    03/2013;
  • Source
    Jules A Gardener, J A Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: We demonstrate that a low energy focused electron beam can locally pattern graphene coated with a thin ice layer. The irradiated ice plays a crucial role in the process by providing activated species that locally remove graphene from a silicon dioxide substrate. After patterning the graphene, the ice resist is easily removed by sublimation to leave behind a clean surface with no further processing. More generally, our findings demonstrate that ice-assisted e-beam lithography can be used to pattern very thin materials deposited on substrate surfaces. The procedure is performed in situ in a modified scanning electron microscope. Desirable structures such as nanoribbons are created using the method. Defects in graphene from electrons backscattered from the bulk substrate are identified. They extend several microns from the e-beam writing location. We demonstrate that these defects can be greatly reduced and localized by using thinner substrates and/or gentle thermal annealing.
    Nanotechnology 04/2012; 23(18):185302. · 3.84 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We report the use of MeV ion-irradiation-induced plastic deformation of amorphous materials to fabricate electrodes with nanometer-sized gaps. Plastic deformation of the amorphous metal Pd(80)Si(20) is induced by 4.64 MeV O(2+) ion irradiation, allowing the complete closing of a sub-micrometer gap. We measure the evolving gap size in situ by monitoring the field emission current-voltage (I-V) characteristics between electrodes. The I-V behavior is consistent with Fowler-Nordheim tunneling. We show that using feedback control on this signal permits gap size fabrication with atomic-scale precision. We expect this approach to nanogap fabrication will enable the practical realization of single molecule controlled devices and sensors.
    Applied Physics Letters 04/2012; 100(15):153108-1531083. · 3.79 Impact Factor
  • Source
    Christopher J Russo, J A Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: Graphene is an ideal thin membrane substrate for creating molecule-scale devices. Here we demonstrate a scalable method for creating extremely small structures in graphene with atomic precision. It consists of inducing defect nucleation centers with energetic ions, followed by edge-selective electron recoil sputtering. As a first application, we create graphene nanopores with radii as small as 3 Å, which corresponds to 10 atoms removed. We observe carbon atom removal from the nanopore edge in situ using an aberration-corrected electron microscope, measure the cross-section for the process, and obtain a mean edge atom displacement energy of 14.1 ± 0.1 eV. This approach does not require focused beams and allows scalable production of single nanopores and arrays of monodisperse nanopores for atomic-scale selectively permeable membranes.
    Proceedings of the National Academy of Sciences 04/2012; 109(16):5953-7. · 9.81 Impact Factor
  • Source
    Anpan Han, Aaron Kuan, Jene Golovchenko, Daniel Branton
    [Show abstract] [Hide abstract]
    ABSTRACT: Electron beam (e-beam) lithography using polymer resists is an important technology that provides the spatial resolution needed for nanodevice fabrication. But it is often desirable to pattern nonplanar structures on which polymeric resists cannot be reliably applied. Furthermore, fragile substrates, such as free-standing nanotubes or thin films, cannot tolerate the vigorous mechanical scrubbing procedures required to remove all residual traces of the polymer resist. Here we demonstrate several examples where e-beam lithography using an amorphous ice resist eliminates both of these difficulties and enables the fabrication of unique nanoscale device structures in a process we call ice lithography. (1, 2) We demonstrate the fabrication of micro- and nanostructures on the tip of atomic force microscope probes, microcantilevers, transmission electron microscopy grids, and suspended single-walled carbon nanotubes. Our results show that by using amorphous water ice as an e-beam resist, a new generation of nanodevice structures can be fabricated on nonplanar or fragile substrates.
    Nano Letters 02/2012; 12(2):1018-21. · 13.03 Impact Factor
  • Source
    A. Han, A. Kuan, J. Golovchenko, D. Branton
    [Show abstract] [Hide abstract]
    ABSTRACT: Electron beam (e-beam) lithography using polymer resists is an important technology that provides the spatial resolution needed for nanodevice fabrication. But it is often desirable to pattern nonplanar structures on which polymeric resists cannot be reliably applied. Furthermore, fragile substrates, such as free-standing nanotubes or thin films, cannot tolerate the vigorous mechanical scrubbing procedures required to remove all residual traces of the polymer resist. Here we demonstrate several examples where e-beam lithography using an amorphous ice resist eliminates both of these difficulties and enables the fabrication of unique nanoscale device structures in a process we call ice lithography.(1, 2) We demonstrate the fabrication of micro- and nanostructures on the tip of atomic force microscope probes, microcantilevers, transmission electron microscopy grids, and suspended single-walled carbon nanotubes. Our results show that by using amorphous water ice as an e-beam resist, a new generation of nanodevice structures can be fabricated on nonplanar or fragile substrates.
    Nano Letters 01/2012; 12(2):1018-1021. · 13.03 Impact Factor
  • Source
    A. Han, A. Kuan, J. Golovchenko, D. Branton
    Nano Letters 01/2012; 12:1018-1021. · 13.03 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: A fabrication method for positioning and embedding a single-walled carbon nanotube (SWNT) across the diameter of a solid state nanopore is presented. Chemical vapor deposition (CVD) is used to grow SWNTs over arrays of focused ion beam (FIB) milled pores in a thin silicon nitride membrane. This typically yields at least one pore whose diameter is centrally crossed by a SWNT. The final diameter of the FIB pore is adjusted to create a nanopore of any desired diameter by atomic layer deposition (ALD), simultaneously embedding and insulating the SWNT everywhere but in the region that crosses the diameter of the final nanopore, where it remains pristine and bare. This nanotube-articulated nanopore is an important step towards the realization of a new type of detector for biomolecule sensing and electronic characterization, including DNA sequencing.
    Journal of vacuum science & technology. B, Microelectronics and nanometer structures: processing, measurement, and phenomena: an official journal of the American Vacuum Society 09/2011; 29(5):053001. · 1.36 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We describe the design of an instrument that can fully implement a new nanopatterning method called ice lithography, where ice is used as the resist. Water vapor is introduced into a scanning electron microscope (SEM) vacuum chamber above a sample cooled down to 110 K. The vapor condenses, covering the sample with an amorphous layer of ice. To form a lift-off mask, ice is removed by the SEM electron beam (e-beam) guided by an e-beam lithography system. Without breaking vacuum, the sample with the ice mask is then transferred into a metal deposition chamber where metals are deposited by sputtering. The cold sample is then unloaded from the vacuum system and immersed in isopropanol at room temperature. As the ice melts, metal deposited on the ice disperses while the metals deposited on the sample where the ice had been removed by the e-beam remains. The instrument combines a high beam-current thermal field emission SEM fitted with an e-beam lithography system, cryogenic systems, and a high vacuum metal deposition system in a design that optimizes ice lithography for high throughput nanodevice fabrication. The nanoscale capability of the instrument is demonstrated with the fabrication of nanoscale metal lines.
    The Review of scientific instruments 06/2011; 82(6):065110. · 1.52 Impact Factor
  • Source
    Slaven Garaj, William Hubbard, J A Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: We demonstrate an ion implantation method for large-scale synthesis of high quality graphene films with controllable thickness. Thermally annealing polycrystalline nickel substrates that have been ion implanted with carbon atoms results in the surface growth of graphene films whose average thickness is controlled by implantation dose. The graphene film quality, as probed with Raman and electrical measurements, is comparable to previously reported synthesis methods. The implantation synthesis method can be generalized to a variety of metallic substrates and growth temperatures, since it does not require a decomposition of chemical precursors or a solvation of carbon into the substrate.
    Applied Physics Letters 11/2010; 97(18):183103. · 3.79 Impact Factor
  • Source
    S Garaj, W Hubbard, A Reina, J Kong, D Branton, J A Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: Isolated, atomically thin conducting membranes of graphite, called graphene, have recently been the subject of intense research with the hope that practical applications in fields ranging from electronics to energy science will emerge. The atomic thinness, stability and electrical sensitivity of graphene motivated us to investigate the potential use of graphene membranes and graphene nanopores to characterize single molecules of DNA in ionic solution. Here we show that when immersed in an ionic solution, a layer of graphene becomes a new electrochemical structure that we call a trans-electrode. The trans-electrode's unique properties are the consequence of the atomic-scale proximity of its two opposing liquid-solid interfaces together with graphene's well known in-plane conductivity. We show that several trans-electrode properties are revealed by ionic conductance measurements on a graphene membrane that separates two aqueous ionic solutions. Although our membranes are only one to two atomic layers thick, we find they are remarkable ionic insulators with a very small stable conductance that depends on the ion species in solution. Electrical measurements on graphene membranes in which a single nanopore has been drilled show that the membrane's effective insulating thickness is less than one nanometre. This small effective thickness makes graphene an ideal substrate for very high resolution, high throughput nanopore-based single-molecule detectors. The sensitivity of graphene's in-plane electronic conductivity to its immediate surface environment and trans-membrane solution potentials will offer new insights into atomic surface processes and sensor development opportunities.
    Nature 09/2010; 467(7312):190-3. · 38.60 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We observe the capture and field ionization of individual atoms near the side wall of a single suspended nanotube. Extremely large cross sections for ionization from an atomic beam are observed at modest voltages due to the nanotube's small radius and extended length. The effects of the field strength on both the atomic capture and the ionization process are clearly distinguished in the data, as are prompt and delayed ionizations related to the locations at which they occur. Efficient and sensitive neutral atom detectors can be based on the nanotube capture and wall ionization processes.
    Physical Review Letters 04/2010; 104(13):133002. · 7.73 Impact Factor
  • David Hoogerheide, Slaven Garaj, Jene Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: Solid-state nanopores are promising sensors for single biomolecules. Most sensing applications rely on electronic detection of changes in the ionic transport through or across the nanopore in the 0.1--10 kHz frequency band. Our recent studies of the electronic noise properties of silicon nitride nanopores highlight both the suitability of nanopores for physical measurements and their limits of detection (PRL 102, 256804 (2009)). We explore the dependence of excess white noise, which is dominant at detection frequencies, on electrolyte concentration, temperature, and pH. We detect two distinct processes: number fluctuations and surface charge fluctuations. Number fluctuations arise from carrier diffusion through the nanopore and represent a fundamental limit of voltage-driven detection techniques. This sort of noise is minimized at high electrolyte concentrations in low viscosity solutions. In addition, the interaction of ions in the solution with the surface produces fluctuations in the surface charge, and hence the conductance. This noise varies strongly with pH. Both are masked by /f noise at low frequencies. The usefulness of these noise sources for measuring physical constants such as diffusivity and reaction kinetics will be discussed.
    03/2010;
  • T. Ristroph, A. Goodsell, J. Golovchenko, L. V. Hau
    [Show abstract] [Hide abstract]
    ABSTRACT: Laser-cooled rubidium atoms are captured by the inhomogeneous electric field surrounding a single charged suspended carbon nanotube. The atom experiences an induced dipole attractive potential with a singular inverse square scaling. The ultimate fate of the captured atom is field ionization near the wall of the nanotube. Field ionization detection is fast, efficient, and position sensitive, and could become the detection method for a new generation of atom-nanotube traps.
    01/2010;
  • 10/2008;
  • [Show abstract] [Hide abstract]
    ABSTRACT: We demonstrate a single molecule trap based on a solid state nanopore. A single molecule of DNA is driven through a nanopore by an applied eletric field. The passage of the molecule through the nanopore is detected by a decrease in the ionic current through the pore. After the molecule has passed through the pore, we reverse the applied field to recapture the molecule and drive it through the pore again. Upon detection of this second passage, we again reverse the applied field, leading to a third passage through the pore, and so on. Thus the molecule is continually confined by a 1r potential maintained by active feedback. Upon each passage through the pore, the state of the molecule is electronically interrogated via the measured current blockage. Molecules can be trapped, detected, and analyzed in free solution without any labels or chemical modifications. Repeated electronic interrogation of a single molecule provides a means for greatly enhancing the accuracy with which each molecule can be characterized by a nanopore and allows measurement over time of dynamical properties such as the molecule's conformation and chemical state.
    03/2008;
  • Xinghua Lu, Eric Brandin, Jene Golovchenko, Daniel Brandon
    [Show abstract] [Hide abstract]
    ABSTRACT: The single-strand deoxyribonucleic acid (ssDNA) - carbon nanotube (CNT) complex on Au(111) surfaces has been studied via scanning tunneling microscopy (STM). The interaction between ssDNA and CNT not only disperses the nanotubes, but also makes the ssDNA more accessible for the STM study. Sputtering on the ssDNA-CNT complex helps to reveal the internal structure. Scanning tunneling spectroscopy (STS) has been carried out to study the electronic structure of the ssDNA-CNT complex.
    03/2008;
  • Source
    Marc Gershow, J A Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: The development of solid-state nanopores, inspired by their biological counterparts, shows great potential for the study of single macromolecules. Applications such as DNA sequencing and the exploration of protein folding require control of the dynamics of the molecule's interaction with the pore, but DNA capture by a solid-state nanopore is not well understood. By recapturing individual molecules soon after they pass through a nanopore, we reveal the mechanism by which double-stranded DNA enters the pore. The observed recapture rates and times agree with solutions of a drift-diffusion model. Electric forces draw DNA to the pore over micrometer-scale distances, and upon arrival at the pore, molecules begin translocation almost immediately. Repeated translocation of the same molecule improves measurement accuracy, offers a way to probe the chemical transformations and internal dynamics of macromolecules on sub-millisecond time and sub-micrometre length scales, and demonstrates the ability to trap, study and manipulate individual macromolecules in solution.
    Nature Nanotechnology 12/2007; 2(12):775-9. · 31.17 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: Nanopores fabricated with low energy noble gas ion beams in a silicon nitride membrane can be employed as the fundamental element of single biomolecule detection and characterization devices. The effect of morphology, annealing, and physical surface treatments are systematically studied to determine their effect on the electrical noise characteristics of the nanopore when used as part of a nanofluidic detector. Atomic Force Microscopy (AFM) is used to measure the morphology of the region near the pore, while X-ray Photoelectron Spectroscopy (XPS) and Rutherford Backscattering (RBS) are used to measure the change in the surface composition with annealing as well as initial depth profiles of imbedded ions. We qualitatively discuss the underlying physical processes that contribute to the electrical noise characteristics of the pore in comparison with our measurements and present optimized conditions for fabricating the quietest pores.
    01/2007;
  • Source
    H. B. Peng, M. E. Hughes, J. A. Golovchenko
    [Show abstract] [Hide abstract]
    ABSTRACT: Electrical current fluctuation studies are reported for coaxial p-type and n-type single-wall carbon nanotube field-effect transistors (FETs). Abrupt discrete switching of the source-drain current is observed at room temperature. The authors attribute these random telegraph signals to charge fluctuating electron traps near the FET conduction channels. Evolution of the current-switching behavior associated with the occupancy of individual electron traps is demonstrated and analyzed statistically. The result strongly indicates room temperature single charge sensitivity in carbon nanotube FETs, which may offer potential applications for single molecule sensors based on suitably prepared FET devices.
    Applied Physics Letters 12/2006; 89(24):243502-243502-3. · 3.79 Impact Factor

Publication Stats

5k Citations
946.79 Total Impact Points

Institutions

  • 1987–2011
    • Harvard University
      • • Department of Physics
      • • Department of Molecular and Cell Biology
      • • School of Engineering and Applied Sciences
      • • Area of Applied Physics
      Cambridge, MA, United States
  • 1982
    • University at Albany, The State University of New York
      • Department of Physics
      New York City, NY, United States