We performed detailed photoluminescence (PL) spectroscopy studies of three different types of single-walled carbon nanotubes (SWNTs) by using samples that contain essentially only one chiral type of SWNT, (6,5), (7,5), or (10,5). The observed PL spectra unambiguously show the existence of an emission sideband at ~ 145 meV below the lowest singlet excitonic (E11) level, whose identity and origin are now under debate. We find that the energy separation between the E11 level and the sideband is almost independent of the SWNT diameter. Based on this, we ascribe the origin of the observed sideband to coupling between K-point LO phonons and dipole-forbidden dark excitons, as recently suggested based on the measurement of (6,5) SWNTs.
The GaSb and Ga0.62In0.38Sb nanocrystals were embedded in the SiO2 films by radio-frequency magnetron co-sputtering and were grown on GaSb and Si substrates at different temperatures. We present results on the 10K excitonic photoluminescence (PL) properties of nanocrystalline GaSb and Ga0.62In0.38Sb as a function of their size. The measurements show that the PL of the GaSb and Ga0.62In0.38Sb nanocrystallites follows the quantum confinement model very closely. By using deconvolution of PL spectra, origins of structures in photoluminescence were identified.
We have studied photoluminescence (PL) and resonant Raman scatterings of single-walled carbon nanotubes (SWNTs) consisting of carbon-13 (SW13CNTs) synthesized from a small amount of isotopically modified ethanol. There was almost no change in the Raman spectra shape for SW13CNTs except for a downshift of the Raman shift frequency by the square-root of the mass ratio 12/13. By comparing photoluminescence excitation (PLE) spectra of SW13CNTs and normal SWNTs, the excitonic phonon sideband due to strong exciton-phonon interaction was clearly identified with the expected isotope shift.
We present photoluminescence measurements in monolayer WSe$_2$, which point to the importance of the interaction between charged particles and excitonic complexes. The theoretical analysis highlights the key role played by exchange scattering, referring to cases wherein the particle composition of the complex changes after the interaction. For example, exchange scattering renders bright excitonic complexes dark in monolayer WSe$_2$ on accounts of the unique valley-spin configuration in this material. In addition to the ultrafast energy relaxation of hot excitonic complexes following their inte…
Hybrid perovskite thin films have demonstrated impressive performance for solar energy conversion and optoelectronic applications. However, further progress will benefit from a better knowledge of the intrinsic photophysics of materials. Here, the low temperature emission properties of CH3NH3PbI3 single crystals are investigated and compared to those of thin polycrystalline films by means of steady-state and time-resolved photoluminescence spectroscopy. While the emission properties of thin films and crystals appear relatively similar at room temperature, low temperature photoluminescence spec…
The excitonic radiative recombination of intercalated Cl2 molecules for two different polytypes 2H-MoS2 and 3R-MoS2 layered crystals are presented. The structure of the excitonic emission is unique and provides a robust experimental signature of crystal polytype investigated. This result is confirmed by X-ray diffraction analysis and DFT electronic band structure calculations. Thus, the bound exciton emission provides a nondestructive fingerprint for the reliable identification of the polytype of MoS2 layered crystals.
We investigate excitonic polaron states comprising a local exciton and phonons in the longitudinal optical (LO) mode by solving the Schrödinger equation. We derive an exact expression for the ground state (GS), which includes multi-phonon components with coefficients satisfying the Huang-Rhys factors. The recombination of GS and excited polaron states gives one set of sidebands in photoluminescence (PL): the multi-phonon components in the GS produce the Stokes lines and the zero-phonon components in the excited states produce the anti-Stokes lines. By introducing the mixing of the LO mode and …
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.
Time-resolved ARPES in pumped excitonic systems: Floquet physics induced by excitonic fields
Dipartimento di Fisica “E.R. Caianiello”, Università degli Studi di Salerno（萨莱诺大学 E.R. 卡亚涅洛物理系）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会 SPIN 研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（萨莱诺大学 CNISM 研究所萨莱诺分部）
We measure the homogeneous excitation linewidth of regioregular poly(3-hexylthiophene), a model semicrystalline polymeric semiconductor, by means of two-dimensional coherent photoluminescence excitation spectroscopy. At a temperature of 8\,K, we find a linewidth that is always $\gtrsim 110$\,meV full-width-at-half-maximum, which is a significant fraction of the total linewidth. It displays a spectral dependence and is minimum near the 0--0 origin peak. We interpret this spectral dependence of the homogeneous excitation linewidth within the context of a weakly coupled aggregate model.
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…
The effect of an external electric field F on the excitonic photoluminescence (PL) spectra of a symmetric coupled double quantum well (DQW) is investigated both theoretically and experimentally. We show that the variational method in a two-particle electron-hole wave function approximation gives a good agreement with measurements of PL on a narrow DQW in a wide interval of F including flat-band regime. The experimental data are presented for an MBE-grown DQW consisting of two 5 nm wide GaAs wells, separated by a 4 monolayers (MLs) wide pure AlAs central barrier, and sandwiched between Ga_{0.7}…
Magnetic field dependent polarization selective photoluminescence(PL) study has been carried out at 1.5~K on Gd-doped GaN epitaxial layers grown on c-SiC substrates by molecular beam epitaxy technique. It has been found that the incorporation of Gd in GaN leads to the generation of three types of donor like defects that result in neutral donor bound excitonic features in low temperature PL. The study reveals that the rate of spin-flip scattering for all the three excitonic features becomes almost $B$-independent suggesting that these signals must be stemming from defects which are ferromagneti…
One- and two-photon luminescence excitation spectroscopy showed a series of distinct excitonic states in single-walled carbon nanotubes. The energy splitting between one- and two-photon-active exciton states of different wavefunction symmetry is the fingerprint of excitonic interactions in carbon nanotubes. We determine exciton binding energies of 0.3-0.4 eV for different nanotubes with diameters between 0.7 and 0.9 nm. Our results, which are supported by ab-initio calculations of the linear and non-linear optical spectra, prove that the elementary optical excitations of carbon nanotubes are s…
Low-temperature (1.8 K) excitonic absorption, reflection and photoluminescence spectra of mixed $Zn(P_{1 - x}As_{x})_{2}$ crystals were studied at $x = $0.01, 0.02, 0.03 and 0.05. Energy gap and rydbergs of excitonic B, C and A-series decrease monotonically at the increase of $x$. Spectral half-widths of absorption $n = 1$ lines of B and A-series increase monotonically at the increase of $x$ due to fluctuations of crystal potential. Emission lines of excitonic molecules were observed in photoluminescence spectra of $Zn(P_{1 - x}As_{x})_{2}$ crystals. Binding energy of molecule increases at the…
We investigate effects of the local structure on the excitonic transport in C60 thin films by means of temperature-dependent photoluminescence quenching studies in a range of 5 to 300 K. Exciton motion in the X-ray amorphous layers indicates thermally activated transport initiated above 80 K accompanied by a thermalization of excitations into low lying states within the excitonic density of states. Discontinuities in the temperature-dependent photoluminescence behavior can be attributed to a continuous phase transition at 80 K and a first order phase transition at 180 K, thereby revealing stru…
We investigate the interband transitions in several ensembles of self-assembled InAs/GaAs quantum dots by using photoluminescence excitation spectroscopy under strong magnetic field. Well defined resonances are observed in the spectra. A strong anticrossing between two transitions is observed in all samples, which cannot be accounted for by a purely excitonic model. The coupling between the mixed exciton-LO phonon states is calculated using the Fröhlich Hamiltonian. The excitonic polaron energies as well as the oscillator strengths of the interband transitions are determined. An anticrossing i…
We report on a new approach to detect excitonic qubits in semiconductor quantum dots by observing spontaneous emissions from the relevant qubit level. The ground state of excitons is resonantly excited by picosecond optical pulses. Emissions from the same state are temporally resolved with picosecond time resolution. To capture weak emissions, we greatly suppress the elastic scattering of excitation beams, by applying obliquely incident geometry to the micro photoluminescence set-up. Rabi oscillations of the ground-state excitons appear to be involved in the dependence of emission intensity on…
Excitonic properties in 2D heterobilayers are closely governed by charge transfer (CT) and excitonic energy transfer (ET) at van der Waals interfaces. Various means have been employed to modulate the interlayer CT and ET, including electrical gating and modifying interlayer spacing, but with limited extent in their controllability. Here, we report a novel method to modulate these transfers in MoS2/WS2 heterobilayer by applying compressive strain under hydrostatic pressure. Raman and photoluminescence measurements, combined with density functional theory calculations show pressure-enhanced inte…
Zinc oxide (ZnO) films having various thicknesses were synthesized on sapphire substrates by thermal oxidation of Zn-metallic films in air ambient. X-ray diffraction (XRD) spectra indicate that the resulting films possess a polycrystalline hexagonal wurtzite structure without preferred orientation. For films having a thickness of 200 nm, crystal grain size was observed to decrease with increasing annealing temperature up to 600C, and then increase at higher temperatures. Thicker films demonstrated a modest increase in grain size as temperature increased from 300C to 1200C. The influence of fil…
Micro-photoluminescence spectroscopy at variable temperature, excitation intensity and energy was performed on a single InAs/AlAs self-assembled quantum dot. The exciton emission line (zero-phonon line, ZPL) exhibits a broad sideband due to exciton-acoustic phonon coupling by the deformation potential mechanism. Additionally, narrow low-energy sidebands at about 0.25 meV of the ZPL are attributed to exciton-acoustic phonon piezoelectric coupling. In lowering the excitation energy or intensity these bands gradually dominate the emission spectrum of the quantum dot while the ZPL disappears. At h…
The excitonic luminescence of an isolated polydiacetylene polymer chain in its monomer matrix is studied by micro-photoluminescence. These chains behave as perfect 1D excitonic systems with the expected 1/sqrt{E} density of states between 5 and 50 K. The temperature dependence of the homogeneous width is quantitatively explained by interaction with longitudinal acoustic phonons of the crystal in the range of temperature explored.
We report on low temperature photoluminescence (PL) and EPR study of bulk polycrystalline ZnO . Variation of peak position of donor bound exciton transition (D1XA) and FXAn=1-1LO with pump intensity show red shift and blue shift respectively due to exciton-exciton scattering. EPR spectra reveals three peaks at g value of 1.985, 1.956 and 1.939 respectively, g=1.956 and g=1.985 is due to shallow donors Zn interstitial and oxygen vacancy respectively An EPR spectrum at 100 K reveals higher degree of asymmetry and hyperfine splitting due to crystal field and inhomogeneous relaxation of paramagnet…
Optical and magneto-optical properties of ZnMnO films grown at low temperature by Atomic Layer Deposition are discussed. A strong polarization of excitonic photoluminescence is reported, surprisingly observed without splitting or spectral shift of excitonic transitions. Present results suggest possibility of Mn recharging in ZnO lattice. Strong absorption, with onset at about 2.1 eV, is related to Mn 2+ to 3+ photo-ionization. We propose that the observed strong circular polarization of excitonic emission is of a similar character as the one observed by us for ZnSe:Cr.
We find that the optical properties of carbon nanotubes reflect remarkably strong effects of exciton-phonon coupling. Tight-binding calculations show that a significant fraction of the spectral weight of the absorption peak is transferred to a distinct exciton+phonon sideband, which is peaked at around 200 meV above the main absorption peak. This sideband provides a distinctive signature of the excitonic character of the optical transition. The exciton-phonon coupling is reflected in a dynamical structural distortion, which contributes a binding energy of up to 100 meV. The distortion is surpr…
Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find that encapsulation in hexagonal boron nitride (h-BN) sharply reduces the PL linewidth, and that passivation of the oxide substrate by an alkyl monolayer further decreases the linewidth and also minimizes…
We study the energy structure of two-dimensional holes in p-type single Al_{1-x}Ga_{x}As/GaAs heterojunctions under a perpendicular magnetic field. Photoluminescence measurments with low densities of excitation power reveal rich spectra containing both free and bound-carrier transitions. The experimental results are compared with energies of valence-subband Landau levels calculated using a new numerical procedure and a good agreement is achieved. Additional lines observed in the energy range of free-carrier recombinations are attributed to excitonic transitions. We also consider the role of ma…
Monolayer transition metal dichalcogenides (TMDs) exhibit a remarkably strong Coulomb interaction that manifests in tightly bound excitons. Due to the complex electronic band structure exhibiting several spin-split valleys in the conduction and valence band, dark excitonic states can be formed. They are inaccessibly by light due to the required spin-flip and/or momentum transfer. The relative position of these dark states with respect to the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials and thus on their technological potential. Based o…
The near-field scanning optical microscopy images of excitonic wavefunctions in self-assembled InAs/GaAs quantum dots are calculated using an empirical pseudopotential method, followed by the configuration interaction (CI) treatment of many-particle effects. We show the wavefunctions of neutral exciton $X^0$ of different polarizations, and compare them to those of the biexciton $XX$ and the charged excitons $X^+$ and $X^-$. We further show that the exciton $X(P_h \to S_e)$ transition which is forbidden in the far-field photoluminescence has comparable intensities to that of $X(S_h \to S_e)$ tr…
MoTe2 belongs to the semiconducting transition metal dichalcogenide family with some properties differing from the other well-studied members (Mo,W)(S,Se)2. The optical band gap is in the near infrared region and both monolayers and bilayers may have a direct optical band gap. We first simulate the band structure of both monolayer and bilayer MoTe2 with DFT-GW calculations. We find a direct (indirect) electronic band gap for the monolayer (bilayer). By solving the Bethe-Salpeter equation, we calculate similar energies for the direct excitonic states in monolayer and bilayer. We then study the …
We investigate the diffusion process of negatively charged excitons (trions) in WSe2 transition metal dichalcogenide monolayer. We measure time-resolved photoluminescence spatial profiles of these excitonic complexes which exhibit a non-linear diffusion process with an effective negative diffusion behavior. Specifically, we examine the dynamics of the two negatively charged bright excitons (intervalley and intravalley trion) as well as the dark trion. The time evolution allows us to identify the interplay of different excitonic species: the trionic species appear after the neutral excitonic on…
When Cubic Is Not Isotropic: Phonon-Exciton Decoupling in CuInSnS$_4$ Single Crystals
Helmholtz-Zentrum Berlin für Materialien und Energie（柏林赫尔姆霍兹中心）；University of Manchester（曼彻斯特大学）；University of Zurich（苏黎世大学）；University of Basel（巴塞尔大学）；University of Cambridge（剑桥大学）；Freie Universität Berlin（柏林自由大学）
Through an investigation of photoemission properties of highly-photoexcited single-walled carbon nanotubes, we demonstrate that there is an upper limit on the achievable excitonic density. As the intensity of optical excitation increases, all photoluminescence emission peaks arising from different chirality single-walled carbon nanotubes 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 excitonic density for each nanotube species. We propose that this saturation behavior…
Photoluminescence from bulk HfS$_2$ grown by the chemical vapor transport method is reported. A series of emission lines is apparent at low temperature in the energy range of 1.4 - 1.5 eV. Two groups of the observed excitonic transitions followed by their replicas involving acoustic and optical phonons are distinguished using classical intensity correlation analysis. The emission is attributed to the recombination of excitons bound to iodine (I$_2$) molecules intercalated between layers of HfS$_2$. The I$_2$ molecules are introduced to the crystal during the growth as halogen transport agents …
Identification of carbon-related color centers in hBN by high-resolution ab initio photoluminescence modeling
University of Oslo（奥斯陆大学）；State Research Institute Center for Physical Sciences and Technology (FTMC)（立陶宛国家物理科学技术研究中心）；Warsaw University of Technology（华沙理工大学）
We present direct experimental observation of exciton-phonon bound states in the photoluminescence excitation spectra of isolated single walled carbon nanotubes in aqueous suspension. The photoluminescence excitation spectra from several distinct single-walled carbon nanotubes show the presence of at least one sideband related to the tangential modes, lying {200 meV} above the main absorption/emission peak. Both the energy position and line shapes of the sidebands are in excellent agreement with recent calculations [PRL {\bf 94},027402 (2005)] that predict the existence of exciton-phonon bound…
The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (> 6 $μ$s) and…
Heterobilayers consisting of MoSe$_2$ and WSe$_2$ monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Te…
We report a combined theoretical/experimental study of dynamic screening of excitons in media with frequency-dependent dielectric functions. We develop an analytical model showing that interparticle interactions in an exciton are screened in the range of frequencies from zero to the characteristic binding energy depending on the symmetries and transition energies of that exciton. The problem of the dynamic screening is then reduced to simply solving the Schrodinger equation with an effectively frequency-independent potential. Quantitative predictions of the model are experimentally verified us…
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 n…
Single-layer WS$_2$ is a direct-gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature-dependent photoluminescence measurements on mechanically exfoliated single-layer WS$_2$, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n-type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion do…
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
Exciton intervalley scattering, annihilation and relaxation dynamics, and diffusive transport in a monolayer transition metal dichalcogenides are central to the functionality of devices based on them. This motivated us to investigate these properties in exfoliated high-quality monolayer MoSe2 using heterodyned nonlinear four-wave-mixing transient grating spectroscopy. While free exciton excitations are found to be long-lived (~230 ps), an extremely fast intervalley scattering ( less than 120 fs) is observed leading to a negligible valley polarization, consistent with steady state photoluminesc…
Lead halide perovskites possess high photoluminescence (PL) efficiency and strong electron-phonon interactions, and therefore the optical cooling using up-conversion PL has been expected. We investigate anti-Stokes PL from green-luminescent Cs$_4$PbBr$_6$, whose origin is attributable to CsPbBr3 nanostructures embedded in a Cs$_4$PbBr$_6$ crystal. Because of the high transparency, low refractive index, and high stability of Cs$_4$PbBr$_6$, the green PL displays high external quantum efficiency without photo-degradation. Time-resolved PL spectroscopy reveals the excitonic behaviors in recombina…
Intra- and Interlayer Excitonic Fine Structure of the Two-Dimensional Perovskite (PEA)$_2$PbI$_4$
Julius-Maximilians-University Würzburg（维尔茨堡大学）；MESA+ Institute for Nanotechnology, University of Twente（特温特大学 MESA+ 纳米技术研究所）；School of Metallurgy and Materials, University of Birmingham（伯明翰大学冶金与材料学院）
We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of $n$-doped WS$_2$ monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically-inactive complexes. The semi-dark trions and negative biexciton…
Atomic layers of Black Phosphorus (BP) present unique opto-electronic properties dominated by a direct tunable bandgap in a wide spectral range from visible to mid-infrared. In this work, we investigate the infrared photoluminescence of BP single crystals at very low temperature. Near-bandedge recombinations are observed at 2 K, including dominant excitonic transitions at 0.276 eV and a weaker one at 0.278 eV. The free-exciton binding energy is calculated with an anisotropic Wannier-Mott model and found equal to 9.1 meV. On the contrary, the PL intensity quenching of the 0.276 eV peak at high …
Unidirectional in-plane structural anisotropy in Rhenium-based transition metal dichalcogenides (TMDs) introduces a new class of 2-D materials, exhibiting anisotropic optical properties. In this work, we perform temperature dependent, polarization-resolved photoluminescence and reflectance measurements on several-layer ReS$_{2}$. We discover two additional excitonic resonances (X$_{3}$ and X$_{4}$), which can be attributed to splitting of spin degenerate states. Strong in-plane oscillator strength of exciton species X$_{1}$ and X$_{2}$ are accompanied by weaker counterparts X$_{3}$ and X$_{4}$…
The fine structure of excited excitonic states in a quantum dot with an embedded magnetic ion is studied theoretically and experimentally. The developed theory takes into account the Coulomb interaction between charged carriers, the anisotropic long-range electron-hole exchange interaction in the zero-dimensional exciton, and the exchange interaction of the electron and the hole with the $d$-electrons of a Mn ion inserted inside the dot. Depending on the relation between the quantum dot anisotropy and the exciton-Mn coupling the photoluminescence excitation spectrum has a qualitatively differe…
Controlling the flow of charge neutral interlayer exciton (IX) quasiparticles can potentially lead to low loss excitonic circuits. Here, we report unidirectional transport of IXs along nanoscale electrostatically defined channels in an MoSe$_2$-WSe$_2$ heterostructure. These results are enabled by a lithographically defined triangular etch in a graphene gate to create a potential energy ''slide''. By performing spatially and temporally resolved photoluminescence measurements, we measure smoothly varying IX energy along the structure and high-speed exciton flow with a drift velocity up to 2 * 1…
