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Register a new userNonlinear Photoluminescence Excitation Spectroscopy of Carbon Nanotubes: Exploring the Upper Density Limit of One-Dimensional Excitons
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We have studied emission properties of high-density excitons in single-walled carbon nanotubes through nonlinear photoluminescence excitation spectroscopy. As the excitation intensity was increased, all emission peaks arising from different chiralities showed clear saturation in intensity. Each peak exhibited a saturation value that was independent of the excitation wavelength, indicating that there is an upper limit on the exciton density for each nanotube species. We developed a theoretical model based on exciton diffusion and exciton-exciton annihilation that successfully reproduced the saturation behavior, allowing us to estimate exciton densities. These estimated densities were found to be still substantially smaller than the expected Mott density even in the saturation regime, in contrast to conventional semiconductor quantum wires.
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Rydberg excitons are, with their ultrastrong mutual interactions, giant optical nonlinearities, and very high sensitivity to external fields, promising for applications in quantum sensing and nonlinear optics at the single-photon level. To design quantum applications it is necessary to know how Rydberg excitons and other excited states relax to lower-lying exciton states. Here, we present photoluminescence excitation spectroscopy as a method to probe transition probabilities from various excitonic states in cuprous oxide, and we show giant Rydberg excitons at $T=38$ mK with principal quantum numbers up to $n=30$, corresponding to a calculated diameter of 3 $mu$m.
We have used resonant Raman scattering spectroscopy to fully analyze the relative abundances of different (n,m) species in single-walled carbon nanotube samples that are metallically enriched by density gradient ultracentrifugation. Strikingly, the data clearly show that our density gradient ultracentrifugation process enriches the metallic fractions in armchair and near-armchair species. We observe that armchair carbon nanotubes constitute more than 50% of each (2n + m) family.
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 system that is disorder-free and locally-tunable thus remains an outstanding challenge. Here, we demonstrate a new technique for deterministic creation of locally-tunable, ultra-low-disorder electron systems in carbon nanotubes suspended over circuits of unprecedented complexity. Using transport experiments we show that electrons can be localized at any position along the nanotube and that the confinement potential can be smoothly moved from location to location. Nearly perfect mirror symmetry of transport characteristics about the centre of the nanotube establishes the negligible effects of electronic disorder, thus allowing experiments in precision engineered one-dimensional potentials. We further demonstrate the ability to position multiple nanotubes at chosen separations, generalizing these devices to coupled one-dimensional systems. These new capabilities open the door to a broad spectrum of new experiments on electronics, mechanics, and spins in one dimension.
Near-infrared magneto-optical spectroscopy of single-walled carbon nanotubes reveals two absorption peaks with an equal strength at high magnetic fields ($>$ 55 T). We show that the peak separation is determined by the Aharonov-Bohm phase due to the tube-threading magnetic flux, which breaks the time-reversal symmetry and lifts the valley degeneracy. This field-induced symmetry breaking thus overcomes the Coulomb-induced intervalley mixing which is predicted to make the lowest exciton state optically inactive (or ``dark).
Through ultrafast pump-probe spectroscopy with intense pump pulses and a wide continuum probe, we show that interband exciton peaks in single-walled carbon nanotubes (SWNTs) are extremely stable under high laser excitations. Estimates of the initial densities of excitons from the excitation conditions, combined with recent theoretical calculations of exciton Bohr radii for SWNTs, suggest that their positions do not change at all even near the Mott density. In addition, we found that the presence of lowest-subband excitons broadens all absorption peaks, including those in the second-subband range, which provides a consistent explanation for the complex spectral dependence of pump-probe signals reported for SWNTs.
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