Surface electromagnetic phenomena in pristine and atomically doped carbon nanotubes
I. V. Bondarev
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Accepted Invited Review Article for the Special Issue "Technology Trends and Theory of Nanoscale Devices for Quantum Applications" of the Journal of Computational and Theoretical Nanoscience -- JCTN, American Scientific Publishers, 14 pages, 9 figures
The article reviews recent progress in the theoretical understanding of near-field surface electromagnetic phenomena in pristine and atomically doped carbon nanotubes. The phenomena involving strong coupling effects are outlined. They are the optical absorption by single-walled carbon nanotubes doped with single atoms or ions in the frequency range close to the atomic transition frequency, the entanglement of the pair of atomic qubits strongly coupled to a common high-finesse surface photonic mode of the nanotube, and the optical response of the strongly coupled surface exciton-plasmon excitations in pristine semiconducting carbon nanotubes. The phenomena reviewed have a great potential to be exploited for the future development of the nanotube based tunable optoelectronic device applications in areas such as nanophotonics, nanoplasmonics, cavity quantum electrodynamics, and quantum information science.
We analyze optical absorption by atomically doped carbon nanotubes with a special focus on the frequency range close to the atomic transition frequency. We derive the optical absorbtion line-shape function and, having analyzed particular achiral nanotubes of different diameters, predict the effect of absorbtion line splitting due to strong atom-vacuum-field coupling in small-diameter nanotubes. We expect this effect to stimulate relevant experimental efforts and thus to open a path to new device applications of atomically doped carbon nanotubes in modern nanotechnologies.
When continued device scaling reaches the ultimate limit imposed by atoms, technology based on atomically precise structures is expected to emerge. Device fabrication will then require building blocks with identified atomic arrangements and assembly of the components without contamination. Here we report on a versatile dry transfer technique for deterministic placement of optical-quality carbon nanotubes. Single-crystalline anthracene is used as a medium which readily sublimes by mild heating, leaving behind clean nanotubes and thus enabling bright photoluminescence. We are able to position na…
We present a fabrication scheme called 'fork stamping' optimized for the dry transfer of individual pristine carbon nanotubes (CNTs) onto ferromagnetic contact electrodes fabricated by standard lithography. We demonstrate the detailed recipes for a residue-free device fabrication and in-situ current annealing on suspended CNT spin-valve devices with ferromagnetic Permalloy (Py) contacts and report preliminary transport characterization and magnetoresistance experiments at cryogenic temperatures. This scheme can directly be used to implement more complex device structures, including multiple ga…
We report a strictly non-exponential spontaneous decay dynamics of an excited two-level atom placed inside or at different distances outside a carbon nanotube (CN). This is the result of strong non-Markovian memory effects arising from the rapid variation of the photonic density of states with frequency near the CN. The system exhibits vacuum-field Rabi oscillations, a principal signature of strong atom-vacuum-field coupling, when the atom is close enough to the nanotube surface and the atomic transition frequency is in the vicinity of the resonance of the photonic density of states. Caused by…
We develop a quantum theory of near-field electrodynamical properties of carbon nanotubes and investigate spontaneous decay dynamics of excited states and van der Waals attraction of the ground state of an atomic system close to a single-wall nanotube surface. Atomic spontaneous decay exhibits vacuum-field Rabi oscillations -- a principal signature of strong atom-vacuum-field coupling. The strongly coupled atomic state is nothing but a 'quasi-1D cavity polariton'. Its stability is mainly determined by the atom-nanotube van der Waals interaction. Our calculations of the ground-state atom van de…
The electronic density of states of atomically resolved single-walled carbon nanotubes have been investigated using scanning tunneling microscopy. Peaks in the density of states due to the one-dimensional nanotube band structure have been characterized and compared with the results of tight-binding calculations. In addition, tunneling spectroscopy measurements recorded along the axis of an atomically-resolved nanotube exhibit new, low-energy peaks in the density of states near the tube end. Calculations suggest that these features arise from the specific arrangement of carbon atoms that close …
We have investigated atom-nanotube van der Waals (vdW) coupling in atomically doped carbon nanotubes (CNs). Our approach is based on the perturbation theory for degenerated atomic levels, thus accounting for both weak and strong atom-vacuum-field coupling. The vdW energy is described by an integral equation represented in terms of the local photonic density of states (DOS). By solving it numerically, we demonstrate the inapplicability of standard weak-coupling-based vdW interaction models in a close vicinity of the CN surface where the local photonic DOS effectively increases, giving rise to a…
Large variations of up to two orders of magnitude are observed in the Raman intensity of pristine, suspended quasi-metallic single-walled carbon nanotubes in response to applied gate potentials. No change in the resonance condition is observed, and all Raman bands exhibit the same changes in intensity, regardless of phonon energy or laser excitation energy. The effect is not observed in semiconducting nanotubes. The electronic energy gaps correlate with the drop in the Raman intensity, and the recently observed Mott insulating behavior is suggested as a possible explanation for this effect.
We report optically induced aggregation and consequent separation of specific diameter of pristine single walled carbon nanotubes (SWNT) from stable solution. Well dispersed solution of pristine SWNTs, without any surfactant or functionalization, show rapid aggregation by uniform exposure to UV, visible and NIR illumination. Optically induced aggregation linearly increases with consequent increase in the intensity of light. Aggregated SWNTs were separated from the dispersed supernatant and characterized using absorption and Raman spectroscopy. Separated SWNTs distinctly show enrichment of spec…
We report specifically two things, one the phenomenon of optically induced motion in pristine single walled carbon nanotubes (SWNT) on the macro-scale and other the consequent separation of metallic and semiconducting enriched SWNT aggregates. Experiments provide direct evidence of both positive and negative photophoresis of SWNTs in solution i.e. motion away and towards light respectively. This optically induced motion was found to be dependent on frequency and intensity of light. Aggregates of pristine SWNT, moving under UV and Visible lamp were separated and characterized using absorption a…
The production of spin-polarized currents in pristine carbon nanotubes with Rashba spin-orbit interaction has been shown to be very sensitive to the symmetry of the tubes and the geometry of the setup. Here we analyze the role of defects on the spin quantum conductances of metallic carbon nanotubes due to an external electric field. We show that localized defects, such as adsorbed hydrogen atoms or pentagon-heptagon pairs, increase the Rashba spin-polarized current. Moreover, this enhancement takes place for energies closer to the Fermi energy as compared to the response of pristine tubes. Suc…
We present atomically-resolved STM images of single-wall carbon nanotubes (SWNTs) embedded in a crystalline nanotube rope. Although they may be interpreted as of a chiral nanotube, the images are more consistently explained a an achiral armchair tube with a quenched twist distortion. The existence of quenched twists in SWNTs in ropes might explain the fact that both as-grown bulk nanotube material and individual ropes have insulator-like conductivity at low temperature.
We systematically study the coupling of longitudinal modes (shells) in a carbon nanotube quantum dot. Inelastic cotunneling spectroscopy is used to probe the excitation spectrum in parallel, perpendicular and rotating magnetic fields. The data is compared to a theoretical model including coupling between shells, induced by atomically sharp disorder in the nanotube. The calculated excitation spectra show good correspondence with experimental data.
Recent years have seen the development of several experimental systems capable of tuning local parameters of quantum Hamiltonians. Examples include ultracold atoms, trapped ions, superconducting circuits, and photonic crystals. By design, these systems possess negligible disorder, granting them a high level of tunability. Conversely, electrons in conventional condensed matter systems exist inside an imperfect host material, subjecting them to uncontrollable, random disorder, which often destroys delicate correlated phases and precludes local tunability. The realization of a condensed matter sy…
Usually, in optical spectra of double-walled carbon nanotubes (DWCNTs) weak van der Waals coupling between the layers leads only to a small shift of transition energies with respect to their values in pristine single-walled nanotubes. However, recent results have shown that the Rayleigh spectrum of the DWCNT (12,11)@(17,16) contains additional peaks. Using the tight binding approximation, we demonstrate that in specific DWCNTs the interlayer coupling can slightly modify the band structure of pristine nanotubes in such a way that the unconventional inter-tube electronic transitions become possi…
Spatially-resolved Raman spectra of individual pristine suspended carbon nanotubes are observed under electrical heating. The Raman G+ and G- bands show unequal temperature profiles. The preferential heating is more pronounced in short nanotubes (2 um) than in long nanotubes (5 um). These results are understood in terms of the decay and thermalization of non-equilibrium phonons, revealing the mechanism of thermal transport in these devices. The measurements also enable a direct estimate of thermal contact resistances and the spatial variation of thermal conductivity.
In this work, we have examined how the multi-vacancy defects induced in the horizontal direction change the energetics and the electronic structure of semiconducting Single-Walled Carbon Nanotubes (SWCNTs). The electronic structure of SWCNTs is computed for each deformed configuration by means of real space, Order(N) Tight Binding Molecular Dynamic (O(N) TBMD) simulations. Energy band gap is obtained in real space through the behavior of electronic density of states (eDOS) near the Fermi level. Vacancies can effectively change the energetics and hence the electronic structure of SWCNTs. In thi…
Raman spectra and electrical conductance of individual, pristine, suspended, metallic single-walled carbon nanotubes are measured under applied gate potentials. The G- band is observed to downshift with small applied gate voltages, with the minima occurring at EF = +/- 1/2 Ephonon, contrary to adiabatic predictions. A subsequent upshift in the Raman frequency at higher gate voltages results in a 'W'-shaped Raman shift profile that agrees well with a non-adiabatic phonon renormalization model. This behavior constitutes the first experimental confirmation of the theoretically predicted breakdown…
Prompted by recent reports on $\sqrt{3} \times \sqrt{3}$ graphene superlattices with intrinsic inter-valley interactions, we perform first-principles calculations to investigate the electronic properties of periodically nitrogen-doped graphene and carbon nanotube nanostructures. In these structures, nitrogen atoms substitute one-sixth of the carbon atoms in the pristine hexagonal lattices with exact periodicity to form perfect $\sqrt{3} \times \sqrt{3}$ superlattices of graphene and carbon nanotubes. Multiple nanostructures of $\sqrt{3} \times \sqrt{3}$ graphene ribbons and carbon nanotubes ar…
We study both experimentally and theoretically the fundamental interplay of exciton localization and polarization in semiconducting single-walled carbon nanotubes. From Stark spectroscopy of individual carbon nanotubes at cryogenic temperatures we identify localized excitons as permanent electric dipoles with dipole moments of up to 1eÅ. Moreover, we demonstrate field-effect doping of localized excitons with an additional charge which results in defect-localized trions. Our findings provide not only fundamental insight into the microscopic nature of localized excitons in carbon nanotubes, they…
We propose an ab-initio combination of the Linear Muffin-Tin Orbital and the Recursion Methods to study the effect of extended Stone-Wales defects in single layer Carbon nanotubes. We have successfully applied this to zigzag and armchair tubes. The methodology involves no intrinsic mean-field like assumptions or external parameter fitting. As defects proliferate, the low density of states near the Fermi levels of the pristine tubes is filled with defect states. The increase of DOS at the Fermi level leads to enhanced conduction, which indicates enhanced metallicity due to SW defects in the nan…
Electron spin resonance (ESR) investigation of graphene nanoribbons (GNRs) prepared through longitudinal unzipping of multiwalled carbon nanotubes (MWCNTs) indicates the presence of C-related dangling bond centers, exhibiting paramagnetic features. ESR signal broadening from pristine or oxidized graphene nanoribbons (OGNRs) is explained in terms of unresolved hyperfine structure, and in the case of reduced GNRs (RGNRs), the broadening of ESR signal can be due to enhancement in conductivity upon reduction. The spin dynamics observed from ESR linewidth-temperature data reflect a variable range h…
Photoluminescence spectroscopy measurements are performed on suspended carbon nanotubes in a field-effect configuration, and the gate voltage dependence of photoluminescence spectra are compared for the pristine and the molecularly adsorbed states of the nanotubes. We quantify the molecular screening effect on the trion binding energies by determining the energy separation between the bright exciton and the trion emission energies for the two states. The voltage dependence shows narrower voltage regions of constant photoluminescence intensity for the adsorbed states, consistent with a reductio…
Although carbon nanotubes are potential candidates for DNA encapsulation and subsequent delivery of biological payloads to living cells, the thermodynamical spontaneity of DNA encapsulation under physiological conditions is still a matter of debate. Using enhanced sampling techniques, we show for the first time that, given a sufficiently large carbon nanotube, the confinement of a double-stranded DNA segment, 5'-D(*CP*GP*CP*GP*AP*AP*TP*TP*CP*GP*CP*G)-3', is thermodynamically favourable under physiological environments (134 mM, 310 K, 1 bar), leading to DNA-nanotube hybrids with lower free ener…
By employing the first-principles calculations, we investigate electronic properties of a novel carbon nanostructure called a carbon nanobud, in which a $C_{60}$ molecule covalently attaches or embeds in an armchair carbon nanotube. We find that the carbon nanobud exhibits either semiconducting or metallic behavior, depending on the size of the nanotube, as well as the combination mode. Moreover, with respect to the case of the corresponding pristine nanotubes, some new electronic states appear at 0.3-0.8 eV above the Fermi level for the carbon nanobuds with the attaching mode, which agrees we…
We introduce a new simplified method for computing the electron field emission current in short carbon nanotubes using ab-initio computation in periodic simulation cells. We computed the evolution of the wave functions using Time-Dependent Density Functional Theory, where we have utilized the Crank-Nicholson propagator. We found that in pristine carbon nanotubes, the emitted charge tends to emerge mostly from electrons that are concentrated at the nanotube tip region. The charge beam concentrates into specific channel structures, showing the utility of carbon nanotubes in precision emission ap…
The enhancement of spin-phonon coupling in gadolinium filled double walled carbon nanotubes (GdCl3@DWNTs) is demonstrated through temperature dependent magnetrometry and polarized Raman Spectroscopy (PRS). Temperature dependent susceptibility measurements show that the GdCl3@DWNTs undergo a superparamagnetic phase transion at temperatures below 100 K with a blocking temperature at approximately 47 K. From the temperature dependent PRS, it is observed that a distinct phonon hardening occurs for the G-band modes at temperatures close to the onset of the superparamagentic phase. This is in contra…
Diazonium reactions with carbon nanotubes form optical $sp^3$ defects that can be used in optical and electrical circuits. We investigate a direct on-device reaction supported by confined laser irradiation and present a technique where an arbitrary carbon nanotube can be preferentially functionalized within a device by matching the light frequency with its transition energy. An exemplary reaction was carried out between (9,7) nanotube and 4-bromobenzenediazonium tetrafluoroborate. The substrate supported nanotubes of multiple semiconducting chiralities were locally exposed to laser light while…
Coupling carbon nanotube devices to microwave circuits offers a significant increase in bandwidth and signal-to-noise ratio. These facilitate fast non-invasive readouts important for quantum information processing, shot noise and correlation measurements. However, creation of a device that unites a low-disorder nanotube with a low-loss microwave resonator has so far remained a challenge, due to fabrication incompatibility of one with the other. Employing a mechanical transfer method, we successfully couple a nanotube to a gigahertz superconducting matching circuit and thereby retain pristine t…
We have performed experiments on single-wall carbon nanotube (SWNT) networks and compared with density-functional theory (DFT) calculations to identify the microscopic origin of the observed sensitivity of the network conductivity to physisorbed O2 and N2. Previous DFT calculations of the transmission function for isolated pristine SWNTs have found physisorbed molecules have little influence on their conductivity. However, by calculating the four-terminal transmission function of crossed SWNT junctions, we show that physisorbed O2 and N2 do affect the junction's conductance. This may be unders…
We numerically investigate the electronic transport properties of graphene nanoribbons and carbon nanotubes with inter-valley coupling, e.g., in \sqrt{3}N \times \sqrt{3}N and 3N \times 3N superlattices. By taking the \sqrt{3} \times \sqrt{3} graphene superlattice as an example, we show that tailoring the bulk graphene superlattice results in rich structural configurations of nanoribbons and nanotubes. After studying the electronic characteristics of the corresponding armchair and zigzag nanoribbon geometries, we find that the linear bands of carbon nanotubes can lead to the Klein tunnelling-l…
We report optically induced aggregation and subsequent separation of selective single-walled carbon nanotubes (SWNT) functionalized with bacteriorhodopsin in the aqueous solution. Well-dispersed, aqueous solutions of hydrophobic pristine SWNT were prepared using a biocompatible surfactant. Dispersed SWNTs were then functionalized with biologically synthesized, optically active purple membrane from Halobacterium salinarium S9. Bacteriorhodopsin is the optically active protein of the purple membrane. Charge transfer and interactions between an optically active purple membrane (PM) and nanotubes …
A Reactive Molecular Dynamics Study on the Mechanical Properties of a Recently Synthesized Amorphous Carbon Monolayer Converted into a Nanotube/Nanoscroll
University of Brasília（巴西利亚大学）；University of Campinas（坎皮纳斯大学）
Here we address a theoretical study on the behaviour of electronic states of heterojunctions and quantum dots based on carbon nanotubes under magnetic fields. Emphasis is put on the analysis of the local density of states, the conductance, and on the characteristic curves of current versus voltage. The heterostructures are modeled by joining zigzag tubes through single pentagon-heptagon pair defects, and described within a simple tight binding calculation. The conductance is calculated using the Landauer formula in the Green functions formalism. The used theoretical approach incorporates the a…
We study the binding of chlorine atoms to carbon nanotubes and graphene at a Stone-Wales defect and to the sidewalls of pristine nanotubes. We show using ab initio thermodynamics that if the environment is chlorine-rich enough, the unzipping of carbon nanotubes into graphene nanoribbons with chlorinated edges may be thermodynamically feasible. By controlling the Cl chemical potential through temperature and pressure, opening selectively tubes below a threshold diameter might be possible. Additionally, we find increased binding energies for chlorine atoms bound to Stone-Wales defects as compare…
A simple scalable scheme is reported for fabricating suspended carbon nanotube field effect transistors (CNT-FETs) without exposing pristine as-grown carbon nanotubes to subsequent chemical processing. Versatility and ease of the technique is demonstrated by controlling the density of suspended nanotubes and reproducing devices multiple times on the same electrode set. Suspending the carbon nanotubes results in ambipolar transport behavior with negligible hysteresis. The Hooges constant of the suspended CNT-FETs (2.6 x 10-3) is about 20 times lower than for control CNT-FETs on SiO2 (5.6 x 10-2…
The electrical conductivity of metallic carbon nanotubes (CNTs) quickly saturates with respect to bias voltage due to scattering from a large population of optical phonons. Decay of these dominant scatterers in pristine CNTs is too slow to offset an increased generation rate at high voltage bias. We demonstrate from first principles that encapsulation of 1D atomic chains within a single-walled CNT can enhance decay of "hot" phonons by providing additional channels for thermalisation. Pacification of the phonon population growth reduces electrical resistivity of metallic CNTs by 51% for an exam…
Spins confined in quantum dots are considered as a promising platform for quantum information processing. While many advanced quantum operations have been demonstrated, experimental as well as theoretical efforts are now focusing on the development of scalable spin quantum bit architectures. One particularly promising method relies on the coupling of spin quantum bits to microwave cavity photons. This would enable the coupling of distant spins via the exchange of virtual photons for two qubit gate applications, which still remains to be demonstrated with spin qubits. Here, we use a circuit QED…
Bottom-up synthesized graphene nanoribbons (GNRs) are quantum materials that can be structured with atomic precision, providing unprecedented control over their physical properties. Accessing the intrinsic functionality of GNRs for quantum technology applications requires the manipulation of single charges, spins, or photons at the level of an individual GNR. However, experimentally, contacting individual GNRs remains challenging due to their nanometer-sized width and length as well as their high density on the metallic growth substrate. Here, we demonstrate the contacting and electrical chara…
Atomistic simulations using a combination of classical forcefield and Density-Functional-Theory (DFT) show that carbon atoms remain essentially sp2 coordinated in either bent tubes or tubes pushed by an atomically sharp AFM tip. Subsequent Green's-function-based transport calculations reveal that for armchair tubes there is no significant drop in conductance, while for zigzag tubes the conductance can drop by several orders of magnitude in AFM-pushed tubes. The effect can be attributed to simple stretching of the tube under tip deformation, which opens up an energy gap at the Fermi surface.
Electron microscopes have been improved to achieve ever smaller beam spots, a key parameter that determines the instrument's resolution. The techniques to measure the size of the beam, however, have not progressed to the same degree. There is an on-going need to develop detection technologies that can potentially characterize the smallest electron beam to further improve the capabilities of these instruments. We report on a new electron beam detector based on a single-walled carbon nanotube. Nanotubes are atomically smooth, have a well-defined diameter that is similar in size to the finest ele…
The interaction between hydrogen molecules and platinum (Pt)-decorated carbon nanotubes (CNTs) with boron (B)-, nitrogen (N)-dopants or sidewall vacancies is discussed from first-principle calculations. The adsorption patterns of hydrogen molecules on four types of Pt-decorated CNTs are investigated, and the partial density of states projected on the Pt atom is computed to reveal the response to the number of hydrogen molecules, dopants or vacancies. It is found that the B-, N-dopants or sidewall vacancies can adjust the binding energy between the hydrogen molecules and the Pt atom deposited o…
Despite recent successes in the synthesis of boron nanotubes (BNTs), the atomic arrangement of their walls has not yet been determined and many questions about their basic properties do remain. Here, we unveil the dynamical stability of BNTs by means of first-principles molecular dynamics simulations. We find that free-standing, single-wall BNTs with diameters larger than 0.6 nm are thermally stable at the experimentally reported synthesis temperature of 870$^\circ$C and higher. The walls of thermally stable BNTs are found to have a variety of different mixed triangular-hexagonal morphologies.…
The construction of atomically-precise carbon nanostructures holds promise for developing novel materials for scientific study and nanotechnology applications. Here we show that graphene origami is an efficient way to convert graphene into atomically-precise, complex, and novel nanostructures. By scanning-tunneling-microscope manipulation at low temperature, we repeatedly fold and unfold graphene nanoislands (GNIs) along arbitrarily chosen direction. A bilayer graphene stack featuring a tunable twist angle and a tubular edge connection between the layers are formed. Folding single-crystal GNIs…
Albeit difficult to access experimentally, the density of states (DOS) is a key parameter in solid state systems which governs several important phenomena including transport, magnetism, thermal, and thermoelectric properties. We study DOS in an ensemble of potassium intercalated single-wall carbon nanotubes (SWCNT) and show using electron spin resonance spectroscopy that a sizeable number of electron states are present, which gives rise to a Fermi-liquid behavior in this material. A comparison between theoretical and the experimental DOS indicates that it does not display significant correlat…
The controlled introduction of covalent sp$^{3}$ defects into semiconducting single-walled carbon nanotubes (SWCNTs) gives rise to exciton localization and red-shifted near-infrared luminescence. The single-photon emission characteristics of these functionalized SWCNTs make them interesting candidates for electrically driven quantum light sources. However, the impact of sp$^{3}$ defects on the carrier dynamics and charge transport in carbon nanotubes remains an open question. Here, we use ultrafast, time-resolved optical-pump terahertz-probe spectroscopy as a direct and quantitative technique …
We study the effects of covalent functionalization of single wall carbon nanotubes (CNT) on their elastic properties. We consider simple organic molecules -NH, -NH2, -CH2, -CH3, -OH attached to CNTs' surface at various densities. The studies are based on the first principles calculations in the framework of density functional theory. We have determined the changes in the geometry and the elastic moduli of the functionalized CNTs as a function of the density of adsorbed molecules. It turns out that elastic moduli diminish with increasing concentration of adsorbands, however, the functionalized …
We report on the first direct observation of a transition from a Tomonaga-Luttinger liquid to a Fermi liquid behavior in potassium intercalated mats of single wall carbon nanotubes (SWCNT). Using high resolution photoemission spectroscopy an analysis of the spectral shape near the Fermi level reveals a Tomonaga-Luttinger liquid power law scaling in the density of states for the pristine sample and for low dopant concentration. As soon as the doping is high enough to fill bands of the semiconducting tubes a distinct transition to a bundle of only metallic SWCNT with a scaling behavior of a norm…
One-dimensional crystals have long range translational invariance which manifests as long exciton diffusion lengths, but such intrinsic properties are often obscured by environmental perturbations. We use a first-passage approach to model single-walled carbon nanotube (SWCNT) exciton dynamics (including exciton-exciton annihilation and end effects) and compare it to results from both continuous-wave and multi-pulse ultrafast excitation experiments to extract intrinsic SWCNT properties. Excitons in suspended SWCNTs experience macroscopic diffusion lengths, on the order of the SWCNT length, (1.3…
Carbon nanotube quantum dots allow accurate control of electron charge, spin and valley degrees of freedom in a material which is atomically perfect and can be grown isotopically pure. These properties underlie the unique potential of carbon nanotubes for quantum information processing, but developing nanotube charge, spin, or spin-valley qubits requires efficient readout techniques as well as understanding and extending quantum coherence in these devices. Here, we report on microwave spectroscopy of a carbon nanotube charge qubit in which quantum information is encoded in the spatial position…
We propose to use the damping signal of an oscillating cantilever in dynamic atomic force microscopy as a noninvasive tool to study the vibrational structure of the substrate. We present atomically resolved maps of damping in carbon nanotube peapods, capable of identifying the location and packing of enclosed Dy@C82 molecules as well as local excitations of vibrational modes inside nanotubes of different diameter. We elucidate the physical origin of damping in a microscopic model and provide quantitative interpretation of the observations by calculating the vibrational spectrum and damping of …
Recently experiments showed that nodal structural defects are readily formed in the synthesis of single-walled carbon nanotubes (SWNTs) and consequently, SWNTs are likely to deviate from well-defined seamless tubular structures. Here, using graphene-helix growth model, we describe structural details of feasible nodal defects in SWNTs and investigate how mechanical and electronic properties of SWNTs would change in the presence of them using computational methods. Surprisingly atomistic simulations of SWNTs with nodal defects show excellent agreement with previous structural, tensile, and ball-…
Graphene and related two-dimensional (2D) materials associate remarkable mechanical, electronic, optical and phononic properties. As such, 2D materials are promising for hybrid systems that couple their elementary excitations (excitons, phonons) to their macroscopic mechanical modes. These built-in systems may yield enhanced strain-mediated coupling compared to bulkier architectures, e.g., comprising a single quantum emitter coupled to a nano-mechanical resonator. Here, using micro-Raman spectroscopy on pristine monolayer graphene drums, we demonstrate that the macroscopic flexural vibrations …
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 d…
Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interaction, thus giving rise to a high density of optical states, as quantified by the so-called Purcell factor - the ratio of the decay rate of an optical quantum emitter to its value in free space. Here, we…
Singlet fission (SF) process, where a singlet exciton decays into a pair of spin one exciton states which are in the total spin singlet state, is one of the possible channels for multiple exciton generation (MEG). In chiral single-wall carbon nanotubes (SWCNTs) efficient SF is present within the solar spectrum energy range which is shown by the many-body perturbation theory (MBPT) calculations based on the density functional theory (DFT) simulations. We calculate SF exciton-to-biexction decay rates ${\rm R}_{1\to 2}$ and biexciton-to-exction rates ${\rm R}_{2\to1}$ in the (6,2), (6,5), (10,5) …
We report the effects of passivation on the various properties like electronic structure, structural stability and optical properties of CdTe in the different nanostructure forms such as ultra-thin slabs, monolayers, nanorods and nanotubes. Further, based on these properties, the self-healing ability of each nanostructure has been predicted. The optical properties suggest that all of the passivated and specific unpassivated nanostructures are suitable for optoelectronic applications. The 2D system in <110> orientation and nanotube derived from the <111> monolayer show significant self-healing …
