Two electrons in a quantum dot (QD) can form triplet states. We analyze the exchange coupling of the triplet states of the negatively charged exciton in a QD (X$^-$, two electrons and one hole) with the spin of a magnetic atom (Mn). Two techniques are used to access the spin structure of this magnetic complex: the resonant excitation of the excited states of X$^-$-Mn and the analysis of the emission of a negatively charged biexciton in a magnetic dot (XX$^-$-Mn). The photo-luminescence (PL) excitation of X$^-$-Mn reveals excited states with a circularly polarized fine structure which strongly depends on the Mn spin state S$_z$ and gives rise to negative circular polarization emission. This fine structure arises from the coupling of the triplet states of an excited charged exciton with the Mn (X$^{-*}$-Mn) and its S$_z$ dependence can be described by a spin effective model. The recombination of XX$^-$-Mn leaves in the dot a charged exciton in its excited state and the PL structure is controlled by the coupling of triplet states of X$^{-*}$ with the Mn spin. An analysis of the polarization and magneto-optic properties of this emission gives access to the electron-hole exchange interaction within the triplets states. Comparing the fine structure of the singlet X$^-$-Mn and of the triplets of X$^{-*}$-Mn we can independently study the different source of anisotropy in the QD: the valence band mixing and the exchange interaction in an anisotropic potential
We report a giant electric field induced increase of spin orientation of excitons in n-type GaAs/AlGaAs quantum well. It correlates strongly with the formation of negatively charged excitons (trions) in the photoluminescence spectra. Under resonant excitation of neutral heavy-hole excitons, the polarization of excitons and trions increases dramatically with electrical injection of electrons within the narrow exciton-trion bias transition in the PL spectra, implying a polarization sensitivity of 200 % per Volt. This effect results from a very efficient trapping of neutral excitons by the quantu…
We present a model to take into account the interface defects contribution on the binding energy of charged exciton in GaAs/Al$_{0.3}$Ga$_{0.7}$As quantum wells. The dependence of the binding energy gain and of the trion size on the quantum well width are variationally calculated. We show that the trion is more sensitive to interface defects than the exciton.
Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular mome…
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and tripl…
Two-dimensional (2D) layered hybrid perovskites provide an ideal platform for studying the properties of excitons. Here, we report on a strong triplet-exciton and longitudinal-optical (LO) phonon coupling in 2D (C6H5CH2CH2NH3, PEA)2PbBr4 perovskites. The triplet excitons exhibit strong photoluminescence (PL) in thick perovskite microflakes, and the PL is not detectable for monolayer microflakes. The coupling strength of the triplet exciton-LO phonon is approximately two to three times greater than that of the singlet exciton-LO phonon with a LO phonon energy of about 21 meV. This difference mi…
We study the system of up to four negatively charged magneto-excitons (X-'s) in the spherical geometry, using the exact-diagonalization techniques. At low energies, X-'s are bound and behave like charged particles without internal dynamics. The pseudopotential describing X-:X- scattering is almost identical to that of electrons and the low-lying few X- states correspond to the few-electron states. The total angular momentum of the ground state depends on the effective filling factor nu and vanishes at its special values. The analogs to the Laughlin nu=1/3 state and the Jain nu=2/5 state of ele…
Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Transition metal dichalcogenides (TMDs), with their large spin-orbit coupling, have been of special interest for valleytronic applications for their coupling of circularly polarized light to excitons with selective valley and spin$^{1-4}$. In atomically thin MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructures, the unique atomic registry of vdW layers provides a quasi-angular momentu…
We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with incr…
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…
Monolayer transition metal dichalcogenides host a variety of optically excited quasiparticles species that stem from two-dimensional confinement combined with relatively large carrier effective masses and reduced dielectric screening. The magnetic response of these quasiparticles gives information on their spin and valley configurations, nuanced carrier interactions, and insight into the underlying band structure. Recently, there have been several reports of 2$s$/3$s$ charged excitons in TMDs, but very little is still known about their response to external magnetic fields. Using photoluminesce…
We study photoluminescence (PL) of charged excitons ($X^-$) in narrow asymmetric quantum wells in high magnetic fields B. The binding of all $X^-$ states strongly depends on the separation $δ$ of electron and hole layers. The most sensitive is the ``bright'' singlet, whose binding energy decreases quickly with increasing $δ$ even at relatively small B. As a result, the value of B at which the singlet--triplet crossing occurs in the $X^-$ spectrum also depends on $δ$ and decreases from 35 T in a symmetric 10 nm GaAs well to 16 T for $δ=0.5$ nm. Since the critical values of $δ$ at which differen…
We report on single-object spectroscopic studies of a characteristic set of three resonances which appear in GaAlAs/AlAs quantum dot structures. The experiments included the photoluminescence (PL) and photoluminescence excitation (PLE) spectroscopy, photon-correlation measurements, analysis of the linear polarization of the emission spectra as well as the PL and PLE spectroscopy performed as a function of magnetic field. The investigated resonances are assigned to three different states of a positively charged exciton: a singlet ground state, a conventional triplet state (involving an electron…
Exciton-polaritons are quasiparticles with mixed photon and exciton character that demonstrate rich quantum phenomena, novel optoelectronic devices and the potential to modify chemical properties of materials. Organic semiconductors are of current interest for their room-temperature polariton formation. However, within organic optoelectronic devices, it is often the 'dark' spin-1 triplet excitons that dominate operation. These triplets have been largely ignored in treatments of polariton physics. Here we demonstrate polariton population from the triplet manifold via triplet-triplet annihilatio…
We report a photoluminescence study of electron-hole complexes in specially designed semiconductor heterostructures. Placing a remote dilute layer of donors at different distances \itshape d \normalfont from the quantum well leads to the transformation of luminescence spectra of neutral ($X$) and negatively charged ($X^{-}$) excitons. The onset of an additional spectral line and its energy dependence on \itshape d \normalfont allows us to unambiguously relate the so-called $X^{-}$ trion state with charged excitons bound on charged donors in a barrier. The results indicate the overestimation in…
Two-dimensional semiconductors feature valleytronics phenomena due to locking of the spin and momentum valley of the electrons. However, the valley polarization is intrinsically limited in monolayer crystals by the fast intervalley electron-hole exchange. Hetero-bilayer crystals have been shown to have a longer exciton lifetime and valley depolarization time. But the reported valley polarization was low; the valley selection rules and mechanisms of valley depolarization remains controversial. Here, we report singlet and brightened triplet interlayer excitons both with over 80% valley polarizat…
We present a comprehensive theoretical study of the resonance fluorescence spectra of an exciton-driven quantum dot (QD) placed inside a high-$Q$ semiconductor cavity and interacting with an acoustic phonon bath. We derive a quantum master equation (ME) in the polaron frame which includes exciton-phonon and exciton-cavity coupling to all orders. This work details and extends the theory used in a recent issue of {\em Physical Review Letters} (C. Roy and S. Hughes 2011: Phys. Rev. Lett. {\bf 106} 247403) to describe the QD Mollow triplet in the regime of semiconductor cavity-QED. Here we introdu…
Light emission from higher-order correlated excitonic states has been recently reported in hBN-encapsulated monolayer WSe2 and WS2 upon optical excitation. These exciton complexes are found to be bound states of excitons residing in opposite valleys in momentum space, a promising feature that could be employed in valleytronics or other novel optoelectronic devices. However, electrically-driven light emission from such exciton species is still lacking. Here we report electroluminescence from bright and dark excitons, negatively charged trions and neutral and negatively charged biexcitons, gener…
We investigate the optical properties of spin-triplet interlayer excitons in heterobilayer transition metal dichalcogenides in comparison with the spin-singlet ones. Surprisingly, the optical transition dipole of the spin-triplet exciton is found to be in the same order of magnitude to that of the spin-singlet exciton, in sharp contrast to the monolayer excitons where the spin triplet species is considered as dark compared to the singlet. Unlike the monolayer excitons whose spin-conserved (spin-flip) transition dipole can only couple to light of in-plane (out-of-plane) polarization, such restr…
We report on strongly temperature-dependent kinetics of negatively charged carrier complexes in asymmetric InAs/AlGaInAs/InP quantum dots (dashes) emitting at telecom wavelengths. The structures are highly elongated and of large volume, which results in atypical carrier confinement characteristics with $s$-$p$ shell energy splittings far below the optical phonon energy, which strongly affects the phonon-assisted relaxation. Probing the emission kinetics with time-resolved microphotoluminescence from a single dot, we observe a strongly non-monotonic temperature dependence of the charged exciton…
A theory of charged excitons X- in a dilute 2D electron gas in a high magnetic field is presented. In contrast to previous calculations, three bound X- states (one singlet and two triplets) are found in a narrow and symmetric GaAs quantum well. The singlet and a "bright" triplet are the two optically active states observed in experiments. The bright triplet has the binding energy of about 1 meV, smaller than the singlet and a "dark" triplet. The interaction of bound X-'s with a dilute 2D electron gas is investigated using exact diagonalization techniques. It is found that the short-range chara…
We report the first theoretical calculations of excited state absorptions (ESAs) from the singlet and triplet excitons, as well as the key intermediate in the singlet fission (SF) process, the spin singlet multiexciton triplet-triplet state, for solid pentacene with herringbone crystal structure. Our goal is to compare theoretical results against ultrafast transient photoinduced absorption (PA) measurements and their interpretations, which have remained controversial. We show that the elusive triplet-triplet state absorbs both in the visible and near infrared (NIR), at or close to the PA energ…
We show that the energy differences between the lowest optical singlet exciton and the lowest triplet exciton in semiconducting single-walled carbon nanotubes with diameter $\sim 1$ nm and graphene nanoribbons with widths $\sim 2$ nm are an order of magnitude smaller than in the $π$-conjugated polymer poly(para-phenylenevinylene). Our calculated energy gaps between the singlet and triplet excitons are in excellent agreement with the measured values in three different nanotubes with diameters close to 1 nm. The spatial extent of the triplet exciton is nearly the same as that of the singlet exci…
Unveiling the Spin-Valley Structure of Dipolar Exciton Ladders in R-stacked WSe$_2$/WS$_2$ Moiré Heterobilayers
Institute of Photonics and Quantum Sciences, SUPA, Heriot-Watt University（赫瑞-瓦特大学光子与量子科学研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料纳米结构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（电子与光学材料研究中心）
研究 R 堆叠 WSe₂/WS₂ 莫尔异质双层中偶极激子阶梯的自旋-谷结构，用螺旋度分辨磁光致发光确定其微观起源，明确不同电荷填充时各激子态情况，建立超越简单占据数物理的自旋-谷分辨图像。
Quantifying the spin-spin interactions which influence electronic transitions in organic semiconductors is crucial for understanding their magneto-optoelectronic properties. By combining a theoretical model for three spin interactions in the coherent regime with pulsed electrically detected magnetic resonance experiments on MEH-PPV diodes, we quantify the spin-coupling within complexes comprising three spin-half particles. We determine that these particles form triplet-exciton:polaron pairs, where the polaron:exciton exchange is over 5 orders of magnitude weaker (less than 170 MHz) than that w…
We present experimental and theoretical results on the high-quality single-layer MoS$_{2}$ which reveal the fine structure of charged excitons, i.e., trions. In the emission spectra we resolve and identify two trion peaks, T$_{1}$ and T$_{2}$, resembling the pair of singlet and triplet trion peaks (T$_S$ and T$_{T}$) in tungsten-based materials. However, in polarization-dependent photoluminescence measurements we identify these peaks as novel intra- and inter-valley singlet trions, constituting the trion fine structure distinct from that already known in bright and dark 2D materials with large…
We present a magneto-photoluminescence study on neutral and charged excitons confined to InAs/GaAs quantum dots. Our investigation relies on a confocal microscope that allows arbitrary tuning of the angle between the applied magnetic field and the sample growth axis. First, from experiments on neutral excitons and trions, we extract the in-plane and on-axis components of the Landé tensor for electrons and holes in the s-shell. Then, based on the doubly negatively charged exciton magneto-photoluminescence we show that the p-electron wave function spreads significantly into the GaAs barriers. We…
We present a generic theory of primary photoexcitations in low band gap donor-acceptor conjugated copolymers. Because of the combined effects of strong electron correlations and broken symmetry, there is considerable mixing between a charge-transfer exciton and an energetically proximate triplet-triplet state with an overall spin singlet. The triplet-triplet state, optically forbidden in homopolymers, is allowed in donor-acceptor copolymers. For an intermediate difference in electron affinities of the donor and the acceptor, the triplet-triplet state can have stronger oscillator strength than …
We first show that, for problems dealing with trions, it is totally hopeless to use the standard many-body description in terms of electrons and holes and its associated Feynman diagrams. We then show how, by using the description of a trion as an electron interacting with an exciton, we can obtain the trion absorption through far simpler diagrams, written with electrons and \emph{excitons}. These diagrams are quite novel because, for excitons being not exact bosons, we cannot use standard procedures designed to deal with interacting true fermions or true bosons. A new many-body formalism is n…
By direct absorption spectroscopy and comparison to photoluminescence (PL), we investigate negatively charged excitons in dilute two-dimensional electron systems at temperatures down to T=40 mK in the regime of the fractional quantum Hall effect. At very low temperatures, for filling factor ν< 1/3, an additional excitation appears in the PL spectrum, between the well-known singlet and triplet excitons. The observation of a similar excitation by PL was reported very recently [G. Yusa et al., cond-mat0103561], and the excitation was assigned, in spite of a PL intensity similar to that of the neu…
We present a first-principle path integral Monte-Carlo (PIMC) study of the binding energy of excitons, trions (positively and negatively charged excitons) and biexcitons bound to single-island interface defects in quasi-two-dimensional GaAs/Al$_{x}$Ga$_{1-x}$As quantum wells. We discuss in detail the dependence of the binding energy on the size of the well width fluctuations and on the quantum-well width. The numerical results for the well width dependence of the exciton, trions and biexciton binding energy are in good quantitative agreement with the available experimental data.
Charged magneto-excitons X- in a dilute 2D electron gas in narrow and symmetric quantum wells are studied using exact diagonalization techniques. An excited triplet X- state with a binding energy of about 1 meV is found. This state and the singlet are the two optically active states observed in photoluminescence (PL). The interaction of X-'s with electrons is shown to have short range, which effectively isolates bound X- states from a dilute e-h plasma. This results in the insensitivity of PL to the filling factor nu. For the "dark" triplet X- ground state, the oscillator strength decreases ex…
Transition-metal dichalcogenides can be easily produced as atomically thin sheets, exhibiting the possibility to optically polarize and read out the valley pseudospin of extremely stable excitonic quasiparticles present in these 2D semiconductors. Here, we investigate a monolayer of tungsten disulphide in high magnetic fields up to 30\,T via photoluminescence spectroscopy at low temperatures. The valley degeneracy is lifted for all optical features, particularly for excitons, singlet and triplet trions, for which we determine the g factor separately. While the observation of a diamagnetic shif…
We present a comparative theoretical study of magnetic resonance within the polaron pair recombination (PPR) and the triplet exciton-polaron quenching (TPQ) models. Both models have been invoked to interpret the photoluminescence detected magnetic resonance (PLDMR) in $π$-conjugated materials. We show that resonance lineshapes calculated within the two models differ dramatically in several regards. First, in the PPR model, the lineshape exhibits unusual behavior upon increasing the microwave power: it evolves from fully positive at weak power to fully negative at strong power. In contrast, in …
The near-field photoluminescence of a gated two-dimensional electron gas is measured. We use the negatively charged exciton, formed by binding of an electron to a photo-excited electron-hole pair, as an indicator for the local presence of charge. Large spatial fluctuations in the luminescence intensity of the negatively charged exciton are observed. These fluctuations are shown to be due to electrons localized in the random potential of the remote ionized donors. We use these fluctuations to image the electrons and donors distribution in the plane.
We investigate the properties of a Skyrmionic exciton consisting of a negatively charged Skyrmion bound to a mobile valence hole. A variational wave function is constructed which has the generalized total momentum P as a good quantum number. It is shown that the Skyrmionic exciton can have a larger binding energy than an ordinary magnetoexciton and should therefore dominate the photoluminescence spectrum in high-mobility quantum wells and heterojunctions where the electron-hole separation exceeds a critical value. The dispersion relation for the Skyrmionic exciton is discussed.
We detect a novel radiative cascade from a neutral semiconductor quantum dot. The cascade initiates from a metastable biexciton state in which the holes form a spin-triplet configuration, Pauli-blockaded from relaxation to the spin-singlet ground state. The triplet biexciton has two photon-phonon-photon decay paths. Unlike in the singlet-ground state biexciton radiative cascade, in which the two photons are co-linearly polarized, in the triplet biexciton cascade they are crosslinearly polarized. We measured the two-photon polarization density matrix and show that the phonon emitted when the in…
The formation and possible decay processes of neutral and charged excitonic complexes in electronic integral and fractional quantum Hall systems are discussed. The excitonic complexes are bound states of a small number of the relevant negatively and positively charged quasiparticles (e.g., conduction electrons and valence holes, reversed-spin electrons and spin holes, Laughlin quasielectrons and quasiholes, composite Fermions) that can occur in a 2D electron in the presence of a strong magnetic field. Examples of such bound states are interband neutral and charged excitons, fractionally charge…
We analyze the lineshape of the quasiparticle photoluminescence of monolayer and bilayer molybdenum ditelluride in temperature- and excitation intensity-dependent experiments. We confirm the existence of a negatively charged trion in the bilayer based on its emission characteristics and find hints for a coexistence of intra- and interlayer trions with a few meV splitting in energy. From the lineshape analysis of exciton and trion emission we extract values for exciton and trion deformation potentials as well as acoustical and optical phonon-limited mobilities in MoTe2, with the mobilities show…
We show that optical transitions of charged excitons in semiconductor heterostructures are governed in magnetic fields by a novel exact selection rule, a manifestation of magnetic translations. It is shown that the spin-triplet ground state of the quasi-two-dimensional charged exciton X- --- a bound state of two electrons and one hole --- is optically inactive in photoluminescence at finite magnetic fields. Internal bound-to-bound X- triplet transition has a specific spectral position, below the electron cyclotron resonance, and is strictly prohibited in a translationally-invariant system. The…
The surprising recent observation of highly emissive triplet-states in lead halide perovskites accounts for their orders-of-magnitude brighter optical signals and high quantum efficiencies compared to other semiconductors. This makes them attractive for future optoelectronic applications, especially in bright low-threshold nano-lasers. Whilst non-resonantly pumped lasing from all-inorganic lead-halide perovskites is now well-established as an attractive pathway to scalable low-power laser sources for nano-optoelectronics, here we showcase a resonant optical pumping scheme on a fast triplet-sta…
A variational calculation of the ground state of a neutral exciton and of positively and negatively charged excitons (trions) in single quantum well is presented. We study the dependance of the correlation energy and of the binding energy on the well width and on the hole mass. Our results are are compared with previous theoretical results and with avalaible experimental data.
The formation and various possible decay processes of neutral and charged excitonic complexes in electronic integral and fractional quantum Hall systems are discussed. The excitonic complexes are bound states of a small number of the relevant negatively and positively charged quasiparticles (e.g., conduction electrons and valence holes, reversed-spin electrons and spin holes, Laughlin quasielectrons and quasiholes, composite fermions) that occur in an electron system under specific conditions (e.g., electron density, well width, electric and magnetic fields, or hydrostatic pressure). The examp…
We present a theoretical description of excitons and positively and negatively charged trions in "giant" CdSe/CdS core-shell nanocrystals (NCs). The developed theory provides the parameters describing the fine structure of excitons in CdSe/CdS core/thick shell NCs as a function of the CdSe/CdS conduction band offset and the CdSe core radius. We have also developed a general theory describing the fine structure of positively charged trions created in semiconductor NCs with a degenerate valence band. The calculations take into account the complex structure of the CdSe valence band and inter-part…
We present a theory of highly excited interacting carriers confined in a semiconductor nanostructure, incorporating Auger coupling between excited states with different number of excitations. The Coulomb matrix elements connecting exciton, bi-exciton and tri-exciton complexes are derived and an intuitive picture of breaking neutral multi-exction complexes into positively and negatively charged multi-exciton complexes is given. The general approach is illustrated by analyzing the coupling of biexciton and exciton in CdSe spherical nanocrystals. The electron and hole states are computed using at…
Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the squ…
In photovoltaics (PVs) and artificial photosynthetic systems based on excitons, the question of how energy must be lost in overcoming the Coulomb barrier, converting excitons to free charges, is fundamental, as it determines the achievable open-circuit voltage or over-potential1-3. Here, using transient and steady-state optical spectroscopy we study a model system, pentacene/C60, where pentacene triplet excitons are dissociated to form charge transfer states, which we show to be degenerate in energy with the triplet excitons. We directly track these charge transfer states undergoing efficient …
The ultrathin transition metal dichalcogenides (TMDs) have emerged as promising materials for various applications using two dimensional (2D) semiconductors. They have attracted increasing attention due to their unique optical properties originate from neutral and charged excitons. Here, we report negatively charged exciton formation in monolayer TMDs, notably tungsten disulfide WS2. Our theory is based on an effective mass model of neutral and charged excitons, parameterized by ab-initio calculations. Taking into the account the strong correlation between the monolayer WS2 and the surrounding…
We report calculations of oscillator strengths for the far infrared absorption of light by the excitonic complexes Xn- (the excess charge, n, ranging from one to four) confined in quantum dots. The magnetic field is varied in an interval which corresponds to ``filling factors'' between 2 and 3/5. Electron-hole interaction effects are seen in the deviations of the peak positions from the Kohn lines, and in the spreading of the oscillator strengths over a few final states. Transition densities are used as an additional tool to characterize the absorption peaks.
