Pump-dependent photoluminescence imaging and 2nd order photon correlation studies have been performed on individual single-walled carbon nanotubes (SWCNTs) at room temperature that enable the extraction of both the exciton diffusion constant and the Auger recombination coefficient. A linear correlation between these is attributed to the effect of environmental disorder in setting the exciton mean free-path and capture-limited Auger recombination at this lengthscale. A suppression of photon antibunching is attributed to creation of multiple spatially non-overlapping excitons in SWCNTs whose diffusion length is shorter than the laser spot size. We conclude that complete antibunching at room temperature requires an enhancement of exciton-exciton annihilation rate that may become realizable in SWCNTs allowing for strong exciton localization.
Luminescence properties of carbon nanotubes are strongly affected by exciton diffusion, which plays an important role in various nonradiative decay processes. Here we perform photoluminescence microscopy on hundreds of individual air-suspended carbon nanotubes to elucidate the interplay between exciton diffusion, end quenching, and exciton-exciton annihilation processes. A model derived from random-walk theory as well as Monte Carlo simulations are utilized to analyze nanotube length dependence and excitation power dependence of emission intensity. We have obtained the values of exciton diffus…
We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (~1 nm) semiconducting single-walled carbon nanotubes. We show that these interactions can result in strong exciton-surface-plasmon coupling. The exciton absorption lineshapes exhibit the line (Rabi) splitting $~0.1-0.3$ eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. We expect this effect to open a path to new optoelectronic device applications of semiconducting carbon nanotubes.
We report optical studies of quantum dot excitons in individual suspended carbon nanotubes at cryogenic temperatures. Narrow optical linewidths, strongly suppressed spectral wandering, and photoluminescence lifetimes in the range of nanoseconds emerge as key signatures of exciton localization. We infer exciton quantum dot formation with a characteristic length of a few exciton Bohr radii. Localization inhibits exciton diffusion and protects the exciton from dephasing by structural or environmental inhomogeneities as well as from exploring nonradiative quenching sites. In consequence, quantum d…
Direct measurements of the diffusion length of excitons in air-suspended single-walled carbon nanotubes are reported. Photoluminescence microscopy is used to identify individual nanotubes and to determine their lengths and chiral indices. Exciton diffusion length is obtained by comparing the dependence of photoluminescence intensity on the nanotube length to numerical solutions of diffusion equations. We find that the diffusion length in these clean, as-grown nanotubes is significantly longer than those reported for micelle-encapsulated nanotubes.
We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (~1 nm) semiconducting single-walled carbon nanotubes. We show that these interactions can result in strong exciton-surface-plasmon coupling. The exciton absorption line shape exhibits Rabi splitting ~0.1 eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. We also show that the quantum confined Stark effect may be used as a tool to control the exciton binding energy and the nanotube band gap in carbon nanotubes in order, e.g., to bri…
We report the first observation of trions (charged excitons), three-particle bound states consisting of one electron and two holes, in hole-doped carbon nanotubes at room temperature. When p-type dopants are added to carbon nanotube solutions, the photoluminescence and absorption peaks of the trions appear far below the E11 bright exciton peak, regardless of the dopant species. The unexpectedly large energy separation between the bright excitons and the trions is attributed to the strong electron-hole exchange interaction in carbon nanotubes.
Simultaneous photoluminescence and photocurrent measurements on individual single-walled carbon nanotubes reveal spontaneous dissociation of excitons into free electron-hole pairs. Correlation of luminescence intensity and photocurrent shows that a significant fraction of excitons are dissociating during their relaxation into the lowest exciton state. Furthermore, the combination of optical and electrical signals also allows for extraction of the absorption cross section and the oscillator strength. Our observations explain the reasons for photoconductivity measurements in single-walled carbon…
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 demonstrate a possibility for exciton Bose-Einstein condensation in individual small-diameter (~1-2 nm) semiconducting carbon nanotubes. The effect occurs under the exciton-interband-plasmon coupling controlled by an external electrostatic field applied perpendicular to the nanotube axis. It requires fields ~1 V/nm and temperatures below 100 K that are experimentally accessible. The effect offers a testing ground for fundamentals of condensed matter physics in one dimension and opens up perspectives to develop tunable coherent polarized light source with carbon nanotubes.
We examine the excitonic nature of high-lying optical transitions in single-walled carbon nanotubes by means of Rayleigh scattering spectroscopy. A careful analysis of the principal transitions of individual semiconducting and metallic nanotubes reveals that in both cases the lineshape is consistent with an excitonic model, but not one of free-carriers. For semiconducting species, side-bands are observed at ~200 meV above the third and fourth optical transitions. These features are ascribed to exciton-phonon bound states. Such side-bands are not apparent for metallic nanotubes,as expected from…
Photoluminescent carbon nanotubes are expected to become versatile room-temperature single-photon sources that have applications in quantum information processing. Quantum emission from carbon nanotubes is often induced by localization of excitons or exciton-exciton annihilation. Here, we modify the local energy landscape of excitons by decorating nanoscale pentacene particles onto air-suspended single-walled carbon nanotubes. Directional exciton diffusion from the undecorated region to the decorated site is demonstrated, suggesting exciton trapping induced by local dielectric screening from p…
The difficulty of describing excitons in semiconducting SWNTs analytically lies with the fact that excitons can neither be considered strictly 1D nor 2D objects. However, the situation changes in the case of metallic nanotubes where, by virtue of screening from gapless metallic subbands, the radius of the exciton becomes much larger than the radius of the nanotube $R_\text{ex}\gg R$. Taking advantage of this, we develop the theory of excitons in metallic nanotubes, determining that their binding energy is about $0.08v/R$, in agreement with the existing experimental data. Additionally, because …
We calculate the exciton binding energy in single-walled carbon nanotubes with narrow band gaps, accounting for the quasi-relativistic dispersion of electrons and holes. Exact analytical solutions of the quantum relativistic two-body problem are obtain for several limiting cases. We show that the binding energy scales with the band gap, and conclude on the basis of the data available for semiconductor nanotubes that there is no transition to an excitonic insulator in quasi-metallic nanotubes and that their THz applications are feasible.
We present evidence that the strong electron-electron interactions in gapped carbon nanotubes lead to finite hierarchies of excitons within a given nanotube subband. We study these hierarchies by employing a field theoretic reduction of the gapped carbon nanotube permitting electron-electron interactions to be treated exactly. We analyze this reduction by employing a Wilsonian-like numerical renormalization group. We are so able to determine the gap ratios of the one-photon excitons as a function of the effective strength of interactions. We also determine within the same subband the gaps of t…
An analytical expression is obtained for the biexciton binding energy as a function of the inter-exciton distance and binding energy of constituent quasi-one-dimensional excitons in carbon nanotubes. This allows one to trace biexciton energy variation and relevant non-linear absorption under external conditions whereby the exciton binding energy varies. The non-linear absorption lineshapes calculated exhibit characteristic asymmetric (Rabi) splitting as the exciton energy is tuned to the nearest interband plasmon resonance. These results are useful for tunable optoelectronic device application…
The efficiencies of photonic devices are primarily governed by radiative quantum efficiency, which is a property given by the light emitting material. Quantitative characterization for carbon nanotubes, however, has been difficult despite being a prominent material for nanoscale photonics. Here we determine the radiative quantum efficiency of bright excitons in carbon nanotubes by modifying the exciton dynamics through cavity quantum electrodynamical effects. Silicon photonic crystal nanobeam cavities are used to induce the Purcell effect on individual carbon nanotubes. Spectral and temporal b…
We show that the absorption spectrum in semiconducting nanotubes can be determined using the bosonization technique combined with mean-field theory and a harmonic approximation. Our results indicate that a multiple band semiconducting nanotube reduces to a system of weakly coupled harmonic oscillators. Additionally, the quasiparticle nature of the electron and hole that comprise an optical exciton emerges naturally from the bosonized model.
The theory of exciton spectrum in multi-shell hexagonal semiconductor nanotube is developed within the effective masses and rectangular potentials approximations using the method of effective potential. It is shown that the exciton binding energy for all states non-monotonously depends on the inner wire diameter, approaching several minimal and maximal magnitudes. The obtained theoretical results explain well the experimental positions of luminescence peaks for GaAs/Al_{0.4}Ga_{0.6}As nanotubes.
We use the macroscopic quantum electrodynamics approach suitable for absorbing and dispersing media to study the properties and role of collective surface excitations --- excitons and plasmons --- in single-wall and double-wall carbon nanotubes. We show that the interactions of excitonic states with surface electromagnetic modes in individual small-diameter (<~1 nm) single-walled carbon nanotubes can result in strong exciton-surface-plasmon coupling. Optical response of individual nanotubes exhibits Rabi splitting ~0.1 eV, both in the linear excitation regime and in the non-linear excitation r…
We investigate electric-field induced redshifts of photoluminescence from individual single-walled carbon nanotubes. The shifts scale quadratically with field, while measurements with different excitation powers and energies show that effects from heating and relaxation pathways are small. We attribute the shifts to the Stark effect, and characterize nanotubes with different chiralities. By taking into account exciton binding energies for air-suspended tubes, we find that theoretical predictions are in quantitative agreement.
We show that strong light-matter coupling can be used to overcome a long standing problem that has prevented efficient optical emission from carbon nanotubes. The luminescence from the nominally bright exciton states of carbon nanotubes is quenched due to the fast nonradiative scattering to the dark exciton state having a lower energy. We present a theoretical analysis to show that by placing carbon nanotubes in an optical microcavity the bright exctonic state may be split into two hybrid exciton-polariton states, while the dark state remains unaltered. For sufficiently strong coupling between…
Electroluminescence from individual carbon nanotubes within split-gate devices is investigated. By characterizing the air-suspended nanotubes with photoluminescence spectroscopy, chirality is identified and electroluminescence peaks are assigned. We observe electroluminescence linewidth comparable to photoluminescence, indicating negligible heating and state-mixing effects. Split-gate and bias voltage dependences are consistent with emission from an electrostatically formed $pn$-junction.
We report the first high-field magneto-optical study on the exciton-phonon sideband of single-walled carbon nanotubes (SWNTs) consisting only of (6,5) species. Both energy and intensity of the observed phonon sideband were found to be independent of the external magnetic field. Comparing with theoretical calculations, we confirmed that these sidebands originate from the optically forbidden K-momentum singlet excitons. Energy of these K-momentum dark excitons was extracted to be ~ 21.5 meV above the bright zero-momentum singlet excitons, in close agreement with recent theoretical predictions an…
We report that dark excitons can have a large contribution to the emission intensity in carbon nanotubes due to an efficient exciton conversion from a dark state to a bright state. Time-resolved photoluminescence measurements are used to investigate decay dynamics and diffusion properties of excitons, and we obtain intrinsic lifetimes and diffusion lengths of bright excitons as well as diffusion coefficients for both bright and dark excitons. We find that the dark-to-bright transition rates can be considerably high, and that more than half of the dark excitons can be transformed into the brigh…
The bright exciton emission of semiconducting carbon nanotubes is appealing for optoelectronic and quantum photonic devices as well as fundamental studies of light-matter interaction in one-dimensional nanostructures. The photophysics of excitons in carbon nanotubes till date is however largely affected by extrinsic effects of the dielectric environment. Here we carried out time-resolved photoluminescence measurements over 14 orders of magnitude for ultra-clean carbon nanotubes bridging an airgap over pillar posts. Our measurements demonstrate a new regime of intrinsic exciton photophysics wit…
We report high field magneto-optical study on the first and second sub-band transitions of single-chirality single-walled carbon nanotubes. The ordering and relative energy splitting between bright and dark excitonic states were found to be inverse between the first and second subbands. We verified that the zero-momentum dark singlet exciton lies below the bright exciton for the first subband transitions, while for the second sub-band transitions, it was found to have higher energy than the bright excitonic state. Effect of this peculiar excitonic structure was found to manifest itself in dist…
Optical excitations of molecular systems can be modified by their physical environment. We analyze the underlying mechanisms within many-body perturbation theory, which is particularly suited to study non-local polarizability effects on the electronic structure. Here we focus on the example of a semiconducting carbon nanotube, which observes redshifts of its excitons when the tube is touched by another nanotube or other physisorbates. We show that the redshifts mostly result from the polarizability of the attached ad-system. Electronic coupling may enhance the redshifts, but depends very sensi…
Covalent functionalization of semiconducting single-wall carbon nanotubes (CNT) introduces new photoluminescent emitting states. Theses states are spatially localized at around functionalization sites and strongly red-shifted relative to the emission commonly observed from the nanotube band-edge exciton state. A particularly important feature of these localized exciton states is that, because the exciton is no longer free to diffusively sample photoluminescent quenching sites along the CNT length, its lifetime is significantly extended. We have recently demonstrated that an important relaxatio…
Carbon nanotubes are quantum sources whose emission can be tuned at telecommunication wavelengths by choosing the diameter appropriately. Most applications require the smallest possible linewidth. Therefore, the study of the underlying dephasing mechanisms is of utmost interest. Here, we report on the low-temperature photoluminescence of high crystalline quality individual single-wall carbon nanotubes synthesized by laser ablation (L-SWNTs) and emitting at telecommunication wavelengths. A thorough statistical analysis of their emission spectra reveals a typical linewidth one order of magnitude…
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…
Photophysics of single-wall carbon nanotubes (SWCNTs) is intensively studied due to their potential application in light harvesting and optoelectronics. Excited states of SWCNTs form strongly bound electron-hole pairs, excitons, of which only singlet excitons participate in application relevant optical transitions. Long-living spin-triplet states hinder applications but they emerge as candidates for quantum information storage. Therefore knowledge of the triplet exciton energy structure, in particular in a SWCNT chirality dependent manner, is greatly desired. We report the observation of light…
High-field magneto-optical spectroscopy was conducted on highly-selected chiral (6,5) specific single-walled carbon nanotubes. Spectra of phonon sidebands in both 1st and 2nd sub-bands were observed to be unchanged by the application of an external magnetic field up to 52 T. Our analyses led to the conclusion that both phonon sidebands in respective sub-band originate from the dark K-momentum singlet (D-K-S) excitons. Moreover, while the relative ordering between the bandedge bright exciton and its zero-momentum anti-bonding counterpart was found to be opposite for the 1st and 2nd sub-bands, t…
We develop a theoretical background to treat exciton states of semiconductor single-walled carbon nanotubes (SWCNTs) in presence of a periodic potential induced by the surface acoustic wave (SAW) propagating along semiconducting SWCNT. The formalism naturally accounts for the electronic bands splitting into the Floquet sub-bands brought about by the Bragg scattering on the SAW potential. Optically induced transitions within the Floquet states and formation of correlated electron-hole pairs, i.e., exciton states, are examined numerically. We discuss dynamical formation of new van Hove singulari…
We investigate adsorption effects of copper phthalocyanine molecules on excitons and trions in air-suspended carbon nanotubes. Using photoluminescence excitation spectroscopy, we observe that exciton energy redshifts gradually with the molecular deposition thickness. The trion emission is also observed at large deposition amounts, which indicates charge transfer between the phthalocyanine molecules and carbon nanotubes. Analysis of the spectra for individual tubes reveal a correlation between the exciton-trion energy separation and the exciton emission energy, showing that the many-body intera…
Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic and optoelectronic applications but are also known to severely suffer from low optical quantum yields. Here we demonstrate SWCNTs excitons coupled to plasmonic nanocavities reaching deeply into the Purcell regime with FP=234 (average FP=76), near unity quantum yields of 70% (average 41%), and a photon emission rate of 1.7 MHz into the first lens. The measured ultra-narrow exciton linewidth (18 micro eV) implies furthermore generation of indistinguishable single photons from a SWCNT. To demonst…
Condensed-matter emitters offer enriched cavity quantum electrodynamical effects due to the coupling to external degrees of freedom. In the case of carbon nanotubes a very peculiar coupling between localized excitons and the one-dimensional acoustic phonon modes can be achieved, which gives rise to pronounced phonon wings in the luminescence spectrum. By coupling an individual nanotube to a tunable optical micro-cavity, we show that this peculiar exciton-phonon coupling is a valuable resource to enlarge the tuning range of the single-photon source while keeping an excellent exciton-photon coup…
We studied multi-exciton dynamics in monolayer WSe2 using nonlinear photoluminescence (PL) spectroscopy and Monte Carlo simulations. We observed strong nonlinear saturation behavior of exciton PL with increasing excitation power density, and long-distance exciton diffusion reaching several micrometers. We demonstrated that the diffusion-assisted exciton-exciton annihilation model accounts for the observed nonlinear PL behavior. The long-distance exciton diffusion and subsequent efficient exciton-exciton annihilation process determined the unusual multi-exciton dynamics in atomically thin layer…
Optical emission from carbon nanotube transistors (CNTFETs) has recently attracted significant attention due to its potential applications. In this paper, we use a self-consistent numerical solution of the Boltzmann transport equation in the presence of both phonon and exciton scattering to present a detailed study of the operation of a partially suspended CNTFET light emitter, which has been discussed in a recent experiment. We determine the energy distribution of hot carriers in the CNTFET, and, as reported in the experiment, observe localized generation of excitons near the trench-substrate…
Optical properties of single-wall carbon nanotubes (SWCNTs) for light polarized parallel to the nanotube axis have been extensively studied, whereas their response to light polarized perpendicular to the nanotube axis has not been well explored. Here, by using a macroscopic film of highly aligned single-chirality (6,5) SWCNTs, we performed a systematic polarization-dependent optical absorption spectroscopy study. In addition to the commonly observed angular-momentum-conserving interband absorption of parallel-polarized light, which generates $E_{11}$ and $E_{22}$ excitons, we observed a small …
We present a study of free carrier photo-generation and multi-carrier bound states, such as biexcitons and trions (ionized excitons), in semiconducting single-walled carbon nanotubes. Pump-and-probe measurements performed with fs pulses reveal the effects of strong Coulomb interactions between carriers on their dynamics. Biexciton formation by optical transition from exciton population results in an induced absorption line (binding energy 130 meV). Exciton-exciton annihilation process is shown to evolve at high densities towards an Auger process that can expel carriers from nanotubes. The rema…
Theory predicts peculiar features for excited-state dynamics in one dimension (1D) that are difficult to be observed experimentally. Single-walled carbon nanotubes (SWNTs) are an excellent approximation to 1D quantum confinement, due to their very high aspect ratio and low density of defects. Here we use ultrafast optical spectroscopy to probe photogenerated charge-carriers in (6,5) semiconducting SWNTs. We identify the transient energy shift of the highly polarizable S33 transition as a sensitive fingerprint of charge-carriers in SWNTs. By measuring the coherent phonon amplitude profile we ob…
We study theoretically the in-plane electromagnetic response and the exciton-plasmon interactions for an experimentally feasible carbon nanotube (CN) film systems composed of parallel aligned periodic semiconducting CN arrays embedded in an ultrathin finite-thickness dielectric. For homogeneous single-CN films, the intertube coupling and thermal broadening bring the exciton and interband plasmon resonances closer together. They can even overlap due to the inhomogeneous broadening for films composed of array mixtures with a slight CN diameter distribution. In such systems the real part of the r…
The exciton dynamics in monolayer black phosphorus is investigated over a very wide range of photoexcited exciton densities using time resolved photoluminescence. At low excitation densities, the exciton dynamics is successfully described in terms of a double exponential decay. With increasing exciton population, a fast, non-exponential component develops as exciton-exciton annihilation takes over as the dominant recombination mechanism under high excitation conditions. Our results identify an upper limit for the injection density, after which exciton-exciton annihilation reduces the quantum y…
Auger-ionized carriers in a one-dimensional semiconductor are predicted to result in a strong band-gap renormalization. Isolated single-walled carbon nanotubes (SWCNT) under high-intensity laser irradiation exhibit strong nonlinear photoluminescence (PL) due to exciton-exciton annihilation (EEA). The presence of exciton disassociation during the rapid Auger-ionization caused by EEA would lead to a strong nonlinear absorption. By simultaneously measuring SWCNT PL and optical absorption of isolated SWCNT clusters in the PL saturation regime, we give evidence that Auger-ionized excitons do not di…
We studied the excitation density dependence of photoluminescence (PL) spectra of excitons and trions (charged excitons) in hole-doped single-walled carbon nanotubes. We found that the PL intensity of trions exhibited a strong nonlinear saturation behavior as the excitation density increased, whereas that of excitons exhibited a weak sublinear behavior. The strong PL saturation of trions is attributed to depletion of doped holes that are captured by excitons in the formation processes. Moreover, the effective radiative lifetime of a trion was evaluated to be approximately 20 ns.
We demonstrate that electron-phonon interaction in quantum dots embedded in one-dimensional systems leads to pronounced, non-Markovian decoherence of optical transitions. The experiments we present focus on the lineshape of photoluminescence from low-temperature axially localized carbon nanotube excitons. The independent boson model that we use to model the phonon interactions reproduces with very high accuracy the broad and asymmetric emission lines and the weak red-detuned radial breathing mode replicas observed in the experiments. The intrinsic phonon-induced pure-dephasing of the zero-phon…
Free electrons or holes can mediate the nonradiative recombination of excitons in carbon nanotubes. Kinematic constraints arising from the quasi one-dimensional nature of excitons and charge carriers lead to a thermal activation barrier for the process. However, a model calculation suggests that the rate for recombination mediated by a free electron is the same order of magnitude as that of two-exciton recombination. Small amounts of doping may contribute to the short exciton lifetimes and low quantum yields observed in carbon nanotubes.
We measure low-temperature micro-photoluminescence spectra along a MoS$_2$ nanotube, which exhibit the peaks of the optical whispering gallery modes below the exciton resonance. The variation of the position and intensity of these peaks is used to quantify the change of the nanotube geometry. The width of the peaks is shown to be determined by the fluctuations of the nanotube wall thickness and propagation of the detected optical modes along the nanotube. We analyse the dependence of the energies of the optical modes on the wave vector along the nanotube axis and demonstrate the potential of t…
Using a collection of twelve semiconducting carbon nanotube samples, each highly enriched in a single chirality, we study the chirality dependence of the $K$-momentum dark singlet exciton using phonon sideband optical spectroscopy. Measurements of bright absorptive and emissive sidebands of this finite momentum exciton identify its energy as 20 - 38 meV above the bright singlet exciton, a separation that exhibits systematic dependencies on tube diameter, $2n+m$ family, and semiconducting type. We present calculations that explain how chiral angle dependence in this energy separation relates to…
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 sat…
We show that new low-energy photoluminescence (PL) bands can be created in semiconducting single-walled carbon nanotubes by intense pulsed excitation. The new bands are attributed to PL from different nominally dark excitons that are "brightened" due to defect-induced mixing of states with different parity and/or spin. Time-resolved PL studies on single nanotubes reveal a significant reduction of the bright exciton lifetime upon brightening of the dark excitons. The lowest energy dark state has longer lifetimes and is not in thermal equilibrium with the bright state.
We present evidence of all optical trion generation and emission in undoped single walled carbon nanotubes (SWCNTs). Luminescence spectra, recorded on individual SWCNTs over a large CW excitation intensity range, show trion emission peaks red-shifted with respect to the bright exciton peak. Clear chirality dependence is observed for 22 separate SWCNT species, allowing for determination of electron-hole exchange interaction and trion binding energy contributions. Luminescence data together with ultrafast pump probe experiments on chirality sorted bulk samples suggest that exciton-exciton annihi…
We report the direct observation of the spin-singlet dark excitonic state in individual single-walled carbon nanotubes through low-temperature micro-photoluminescence spectroscopy in magnetic fields. A magnetic field up to 5 T, applied along the nanotube axis, brightened the dark state, leading to the emergence of a new emission peak. The peak rapidly grew in intensity with increasing field at the expense of the originally-dominant bright exciton peak and finally became dominant at fields $>$3 T. This behavior, universally observed for more than 50 nanotubes of different chiralities, can be qu…
Statistics of photons emitted by mobile excitons in individual carbon nanotubes are investigated. Photoluminescence spectroscopy is used to identify the chiralities and suspended lengths of air-suspended nanotubes, and photon correlation measurements are performed at room temperature on telecommunication-wavelength nanotube emission with a Hanbury-Brown-Twiss setup. We obtain zero-delay second-order correlation $g^{(2)}(0)$ less than 0.5, indicating single photon generation. Excitation power dependence of the photon antibunching characteristics is examined for nanotubes with various chiralitie…
In high magnetic fields, the exciton absorption spectrum of a semiconducting single-walled carbon nanotube splits as a result of Aharonov-Bohm magnetic flux. A magnetic field of 370 T, generated by the electro-magnetic flux compression destructive pulsed magnet-coil technique, was applied to single-chirality semiconducting carbon nanotubes. Using streak spectroscopy, we demonstrated the separation of the independent band-edge exciton states at the K and K' points of the Brillouin zone after the mixing of the dark and bright states above 150 T. These results enable a quantitative discussion of …
Exciton-exciton recombination in isolated semiconducting single-walled carbon nanotubes was studied using femtosecond transient absorption. Under sufficient excitation to saturate the optical absorption, we observed an abrupt transition between reaction- and diffusion- limited kinetics, arising from reactions between incoherent localized excitons with a finite probability of ~ 0.2 per encounter. This represents the first experimental observation of a crossover between classical and critical kinetics in a 1D coalescing random walk, which is a paradigm for the study of non- equilibrium systems.
Highly efficient exciton-exciton annihilation process unique to one-dimensional systems is utilized for super-resolution imaging of air-suspended carbon nanotubes. Through the comparison of fluorescence signals in linear and sublinear regimes at different excitation powers, we extract the efficiency of the annihilation processes using conventional confocal microscopy. Spatial images of the annihilation rate of the excitons have resolution beyond the diffraction limit. We investigate excitation power dependence of the annihilation processes by experiment and Monte Carlo simulation, and the reso…
Blends of carbon nanotubes with conjugated polymer and fullerene derivatives are complex nanocomposite systems, which have recently attracted a great research interest for their photovoltaic ability. Therefore, gaining a better understanding of the excitonic dynamics in such materials can be important to boost the efficiency of excitonic solar cells. Here, we studied the photophysics of a ternary system in which the polymer PTB7 and the fullerene derivative PCBM are integrated with (6,5) SWNTs. We highlight the contribution of SWNTs in the exciton dissociation and in the charge transfer proces…
