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.
Titanic acid nanotubes (with a chemical formula H2Ti2O4(OH)2, abbreviated as TANTs) were synthesized by the hydrothermal method using commercial TiO2 nanoparticle powder (P25, Degussa, Germany) including anatase and rutile phase as a starting material. Conversion from nanoparticles to nanotubes was achieved by treating the nanoparticle powder with 10 M NaOH aqueous solution. Absorption and photoluminescence (PL) data indicate that the nanotubes obtained under slow and suitable drying and heating conditions had very strong and stable visible absorption with three peaks at 515, 575, and 675 nm a…
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.
Photonic crystal nanocavities are used to enhance photoluminescence from single-walled carbon nanotubes. Micelle-encapsulated nanotubes are deposited on nanocavities within Si photonic crystal slabs and confocal microscopy is used to characterize the devices. Photoluminescence spectra and images reveal nanotube emission coupled to nanocavity modes. The cavity modes can be tuned throughout the emission wavelengths of carbon nanotubes, demonstrating the ability to enhance photoluminescence from a variety of chiralities.
Often a modification of microscopic symmetry in a system can result in a dramatic change in its macroscopic properties. Here we report that symmetry breaking by a tube-threading magnetic field can drastically increase the photoluminescence quantum yield of semiconducting single-walled carbon nanotubes, by as much as a factor of six, at low temperatures. To explain this striking connection between seemingly unrelated properties, we have developed a comprehensive theoretical model based on magnetic-field-dependent one-dimensional exciton band structure and the interplay of strong Coulomb interac…
Gate-voltage effects on photoluminescence spectra of suspended single-walled carbon nanotubes are investigated. Photoluminescence microscopy and excitation spectroscopy are used to identify individual nanotubes and to determine their chiralities. Under an application of gate voltage, we observe slight blueshifts in the emission energy and strong quenching of photoluminescence. The blueshifts are similar for different chiralities investigated, suggesting extrinsic mechanisms. In addition, we find that the photoluminescence intensity quenches exponentially with gate voltage.
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 report a photoluminescence (PL) and transient reflection spectroscopy study of exciton dynamics in monolayer transition transition-metal dichalcogenides (TMDs). PL saturation in monolayer MoSe2 occurs an excitation intensity more than two orders of magnitude lower than in monolayer MoS2. Transient reflection shows that the nonlinear exciton-exciton annihilation is the dominant exciton decay process in monolayer MoSe2 in contrast to the previously reported linear exciton decay in monolayer MoS2. In addition, the exciton lifetime in MoSe2, > 125 ps, is more than an order of magnitude longer t…
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…
The exciton decay rate at a rough interface in type-II semiconductor superlattices is investigated. It is shown that the possibility of recombination of indirect excitons at a plane interface essentially affects kinetics of the exciton photoluminescence at a rough interface. This happens because of strong correlation between the exciton recombination at the plane interface and at the roughness. Expressions that relate the parameters of the luminescence kinetics with statistical characteristics of the rough interface are obtained. The mean height and length of roughnesses in GaAs/AlAs superlatt…
We investigate valley exciton dynamics in MoSe2 monolayers in polarization- and time-resolved photoluminescence (PL) spectroscopy at 4K. Following circularly polarized laser excitation, we record a low circular polarization degree of the PL of typically $\leq5\%$. This is about 10 times lower than the polarization induced under comparable conditions in MoS2 and WSe2 monolayers. The evolution of the exciton polarization as a function of excitation laser energy and power is monitored in PL excitation (PLE) experiments. Fast PL emission times are recorded for both the neutral exciton of $\leq3$ p…
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.
At low temperature the photoluminescence of single-wall carbon nanotubes show a large variety of spectral profiles ranging from ultra narrow lines in suspended nanotubes to broad and asymmetrical line-shapes that puzzle the current interpretation in terms of exciton-phonon coupling. Here, we present a complete set of photoluminescence profiles in matrix embedded nanotubes including unprecedented narrow emission lines. We demonstrate that the diversity of the low-temperature luminescence profiles in nanotubes originates in tiny modifications of their low-energy acoustic phonon modes. When low e…
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 $>$3 T. This behavior, universally observed for more than 50 nanotubes of different chiralities, can be qu…
We report the first observation of photon antibunching in the photoluminescence from single carbon nanotubes. The emergence of a fast luminescence decay component under strong optical excitation indicates that Auger processes are partially responsible for inhibiting two-photon generation. Additionally, the presence of exciton localization at low temperatures ensures that nanotubes emit photons predominantly one by one. The fact that multiphoton emission probability can be smaller than 5% suggests that carbon nanotubes could be used as a source of single photons for applications in quantum cryp…
In high magnetic fields, the exciton absorption spectrum of a semiconducting single-walled carbon nanotube splits as a result of Aharonov-Bohm magnetic flux. A magnetic field of 370 T, generated by the electro-magnetic flux compression destructive pulsed magnet-coil technique, was applied to single-chirality semiconducting carbon nanotubes. Using streak spectroscopy, we demonstrated the separation of the independent band-edge exciton states at the K and K' points of the Brillouin zone after the mixing of the dark and bright states above 150 T. These results enable a quantitative discussion of …
The spectral and spatiotemporal dynamics of photoluminescence in monolayers of transition metal dichalcogenide WSe$_2$ obtained by mechanical exfoliation on a Si/SiO$_2$ substrate is studied over a wide range of temperatures and excitation powers. It is shown that the dynamics is nonexponential and, for times $t$ exceeding $\sim$50 ps after the excitation pulse, is described by a dependence of the form $1/(t+t_0)$. Photoluminescence decay is accelerated with a decrease in temperature, as well as with a decrease in the energy of emitting states. It is shown that the observed dynamics cannot be …
The photoluminescence (PL) spectrum of transition metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of momentum-dark excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as result of different configurations of bright…
Shallow hole-doping in small diameter single-wall carbon nanotubes by H$_2$O$_2$ is shown to result in delocalized excited state quenching with no effects on the ground state absorption spectrum. To account for this process, the dissociation of excitons by shallow level electronic impurities is predicted to occur by multi-particle Auger decay. This mechanism, which relies on the chirality of the electronic states, causes the exciton to decay into electron-hole pairs with very high efficiencies.
Monolayer WSe$_2$ hosts a series of exciton Rydberg states denoted by the principal quantum number n = 1, 2, 3, etc. While most research focuses on their absorption properties, their optical emission is also important but much less studied. Here we measure the photoluminescence from the 1s - 5s exciton Rydberg states in ultraclean monolayer WSe$_2$ encapsulated by boron nitride under magnetic fields from -31 T to 31 T. The exciton Rydberg states exhibit similar Zeeman shifts but distinct diamagnetic shifts from each other. From their luminescence spectra, Zeeman and diamagnetic shifts, we dedu…
We calculate the optical properties of carbon nanotubes in an external static electric field directed along the tube axis. We predict strong Franz-Keldysh oscillations in the first and second band-to-band absorption peaks, quadratic Stark effect of the first two excitons, and the field dependence of the bound exciton ionization rate for a wide range of tube chiralities. We find that the phonon assisted mechanism dominates the dissociation rate in electro-optical devices due to the hot optical phonons. We predict a quadratic dependence of the Sommerfeld factor on the electric field and its incr…
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 ran…
The Ajiki-Ando (A-A) splitting of single-walled carbon nanotubes(SWNT) originating from the Aharanov-Bohm effect was observed in chiral specific SWNTs by the magneto-absorption measurements conducted at magnetic fields of up to 78 T. The absorption spectra from each chirality showed clear A-A splitting of the $E_{11}$ optical excitonic transitions. The parameters of both the dark-bright exciton energy splitting and the rate of A-A splitting in a magnetic field were determined for the first time from the well-resolved absorption spectra.
We report a femtosecond mid-infrared study of the broadband low-energy response of individually separated (6,5) and (7,5) single-walled carbon nanotubes. Strong photoinduced absorption is observed around 200 meV, whose transition energy, oscillator strength, resonant chirality enhancement and dynamics manifest the observation of quasi-1D intra-excitonic transitions. A model of the nanotube 1s-2p cross section agrees well with the signal amplitudes. Our study further reveals saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs.
We probe the room temperature photoluminescence of $N$-layer molybdenum ditelluride (MoTe$_2$) in the continuous wave (cw) regime. The photoluminescence quantum yield of monolayer MoTe$_2$ is three times larger than in bilayer MoTe$_2$ and forty times greater than in the bulk limit. Mono- and bilayer MoTe$_2$ display almost symmetric emission lines at $1.10~\rm eV$ and $1.07~\rm eV$, respectively, which predominantly arise from direct radiative recombination of the A exciton. In contrast, $N\geq3-$layer MoTe$_2$ exhibits a much reduced photoluminescence quantum yield and a broader, redshifted …
We report a photoluminescence observation of robust excitonic polarons due to strong coupling of exciton and longitudinal optical (LO) phonon as well as Fano-type interference in high quality ZnO crystal. At low enough temperatures, the strong coupling of excitons and LO phonons leads to not only traditional Stokes lines (SLs) but also up to second-order anti-Stokes lines (ASLs) besides the zero-phonon line (ZPL). The SLs and ASLs are found to be not mirror symmetric with respect to the ZPL, strongly suggesting that they are from different coupling states of exciton and phonons. It is more int…
We present a systematic study of the exciton/electron-hole plasma photoluminescence dynamics in bulk GaAs for various lattice temperatures and excitation densities. The competition between the exciton and electron-hole pair recombination dominates the onset of the luminescence. We show that the metal-to-insulator transition, induced by temperature and/or excitation density, can be directly monitored by the carrier dynamics and the time-resolved spectral characteristics of the light emission. The dependence on carrier density of the photoluminescence rise time is strongly modified around a latt…
Fifty years ago Walter Kohn speculated that a zero-gap semiconductor might be unstable against the spontaneous generation of excitons---electron-hole pairs bound together by Coulomb attraction. The reconstructed ground state would then open a gap breaking the symmetry of the underlying lattice, a genuine consequence of electronic correlations. Here we show that this excitonic insulator is realized in zero-gap carbon nanotubes by performing first-principles calculations through many-body perturbation theory as well as quantum Monte Carlo. The excitonic order modulates the charge between the two…
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…
We studied the nonlinear time-resolved luminescence signals due to multiexciton recombination processes in single-walled carbon nanotubes (SWNTs) using femtosecond excitation correlation (FEC) spectroscopy. From theoretical analysis of the FEC signals, we found that the FEC signals in the long time range are dominated by the single exciton decay in SWNTs, where the exciton-exciton annihilation process is efficient. Our results provide a simple method to clarify the single exciton decay dynamics in low-dimensional materials.
Electroabsorption spectroscopy of well-identified index-defined semiconducting carbon nanotubes is reported. The measurement of high definition electroabsorption spectra allows direct indexation with unique nanotube chirality. Results show that at least for a limited range of diameters, electroabsorption is directly proportional to the exciton binding energy of nanotubes. Electroabsorption is a powerful technique which directly probes into carbon nanotube excitonic states, and may become a useful tool for in situ study of excitons in future nanotube-based photonic devices such as electroabsorp…
We discuss how excitons can affect the generation of coherent radial breathing modes in ultrafast spectroscopy of single wall carbon nanotubes. Photoexcited excitons can be localized spatially and give rise to a spatially distributed driving force in real space which involves many phonon wavevectors of the exciton-phonon interaction. The equation of motion for the coherent phonons is modeled phenomenologically by the Klein-Gordon equation, which we solve for the oscillation amplitudes as a function of space and time. By averaging the calculated amplitudes per nanotube length, we obtain time-de…
The lack of long range order in organic semiconductor thin films prevents the unveiling of the complete nature of excitons in optical experiments, because the diffraction limited beam diameters in the bandgap region far exceed typical crystalline grain sizes. Here we present spatially-, temporally- and polarization-resolved dual photoluminescence/linear dichroism microscopy experiments that investigate exciton states within a single crystalline grain in solution-processed phthalocyanine thin films. These experiments reveal the existence of a delocalized singlet exciton, polarized along the hig…
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'').
Excitons dominate the optics of atomically-thin transition metal dichalcogenides and 2D van der Waals heterostructures. Interlayer 2D excitons, with an electron and a hole residing in different layers, form rapidly in heterostructures either via direct charge transfer or via Coulomb interactions that exchange energy between layers. Here, we report prominent intertube excitonic effects in quasi-1D van der Waals heterostructures consisting of C/BN/MoS$_2$ core/shell/skin nanotubes. Remarkably, under pulsed infrared excitation of excitons in the semiconducting CNTs we observed a rapid (sub-picose…
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…
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 use Boltzmann transport equation (BE) to study time evolution of a photo-excited state in a nanoparticle including phonon-mediated exciton relaxation and the multiple exciton generation (MEG) processes, such as exciton-to-biexciton multiplication and biexciton-to-exciton recombination. BE collision integrals are computed using Kadanoff-Baym-Keldysh many-body perturbation theory (MBPT) based on density functional theory (DFT) simulations, including exciton effects. We compute internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon in the course of …
We propose an unconventional scheme of photoluminescence in a semiconductor thin film, where the nonlocal correlation between an excitonic wave and a light wave prominently enhances the exciton-light coupling beyond the long-wavelength approximation (the so-called excitonic superradiance regime). On the basis of the developed method extending input-output theory, we elucidate atypical photoluminescence effects due to the strong wave-wave correlation. In particular, the up-converted photoluminescence based on the coherent superposition of excitons is found to be highly efficient, i.e., it can b…
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.
In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this new material enables intrinsically ultrastrong emitter-cavity interactions: rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ~25 nm domains…
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…
The remarkably strong Coulomb interaction in atomically thin transition metal dichalcogenides (TMDs) results in an extraordinarily rich many-particle physics including the formation of tightly bound excitons. Besides optically accessible bright excitonic states, these materials also exhibit a variety of dark excitons. Since they can even lie below the bright states, they have a strong influence on the exciton dynamics, lifetimes, and photoluminescence. While very recently, the presence of dark excitonic states has been experimentally demonstrated, the origin of these states, their formation, a…
The dynamics of exciton and electron-hole plasma populations is studied via time-resolved photoluminescence after nonresonant excitation. By comparing the peak emission at the exciton resonance with the emission of the continuum, it is possible to experimentally identify regimes where the emission originates predominantly from exciton and/or plasma populations. The results are supported by a microscopic theory which allows one to extract the fraction of bright excitons as a function of time.
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…
We study spatial photoluminescence characteristics of neutral and charged excitons across extended monolayer MoS$_2$ synthesized by chemical vapor deposition. Using two-dimensional hyperspectral photoluminescence mapping at cryogenic temperatures we identify regions with increased emission from charged excitons associated with both spin-orbit split valence subbands. Such regions are attributed to unintentional doping at defect sites with excess charge that bind neutral excitons to form defect-pinned trions. Our findings imply comparable timescales for the formation, relaxation, and radiative d…
We study the photoluminescence dynamics of ultra-cold indirect excitons optically created in a double quantum well heterostructure. Above a threshold laser excitation, our experiments reveal the apparition of the so-called inner photoluminescence ring. It is characterized by a ring shaped photoluminescence which suddenly collapses once the laser excitation is terminated. We show that the spectrally resolved dynamics is in agreement with an excitonic origin for the inner-ring which is formed due to a local heating of indirect excitons by the laser excitation. To confirm this interpretation and …
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 present the numerical tool DECaNT (Diffusion of Excitons in Carbon NanoTubes) that simulates exciton transport in thin films of carbon nanotubes. Through a mesh of nanotubes generated using the Bullet Physics C++ library, excitons move according to an ensemble Monte Carlo algorithm, with the scattering rates that account for tube chirality, orientation, and distance. We calculate the diffusion tensor from the position--position correlation functions and analyze its anisotropy and dependence on the film composition, morphology, and defect density.
