Exciton Motion Research Articles

Exciton insulator in a moiré lattice

Interlayer electron and hole can be paired up through coulomb interaction to form an exciton insulator when their kinetic energy is substantially smaller than the interaction energy. The traditional platform to realize such an interlayer interaction is the double quantum well with dielectric material between electron and hole, for which an external magnetic field is required to generate Landau level flat bands that can reduce the kinetic energy of charged carriers. When both quantum wells are at the half filling of the lowest landau level, the electron-electron repulsive interaction, by the particle-hole transformation in one well, will be equivalent to electron-hole attractive interaction, from which interlayer exciton and its condensation can emerge. In a two-dimensional twisted homostructure or an angle aligned heterostructure, there exists a moiré superlattice, in which bands are folded into the mini-Brillouin zone by the large moiré period. Gap opening at the boundary of mini-Brillouin zone can form the well-known moiré flat band. This review will discuss how to use the moiré flat bands to generate exciton insulator in the absence of external magnetic field in transitional metal dichalcogenide (TMD) moiré heterostructure. Unlike the double quantum well where symmetric well geometry is used, the moiré related sample can have multiple different geometries, including monolayer TMD-hexagonal boron nitride-moiré structure, moiré-moiré structure, and monolayer TMD-bilayer TMD structure. The carriers in those structures can be well tuned to locate equally in different layers, and particle-hole transformation in the moiré first Hubbard band can transform the interlayer repulsive coulomb interaction into attractive interaction, which is the same as that in quantum well under magnetic field. We will show that by using differential contrast reflection spectrum, interlayer photoluminescence, 2s exciton sensing, quantum capacitance and microwave impedance microscopy, the signature of exciton fluid can be identified. The excitonic coherence features in those structures will promise by using the coulomb drag technique and counter flow technique in future. In general, exciton in moiré lattice is a promising candidate for studying the Bose-Hubbard model in solids and can well realize exciton superfluidity, excitonic mott insulator as well as the crossover between them.

Excitonic Enhancement and Excited Excitonic States in CsPbBr3 Halide Perovskite Single Crystals

Halide perovskites are novel photonics materials promising numerous applications in fields such as photovoltaics, LED light sources, microlasers, and radiation detectors. Many halide perovskites are direct-gap semiconductors, and Wannier-Mott excitons play a significant role in their optical properties near the fundamental absorption edge. The high oscillator strength of these states favors applications where efficient interaction with light is required. In this work, to study excitonic states in CsPbBr3 halide perovskite single crystals, the reflection spectroscopy at temperatures from 4 K was used. A reflection coefficient up to 70% was observed for the n=1 exciton state, followed by weak excited states of excitons with n=2 and n=3. It should be noted that the Sommerfeld enhancement factor should be considered for a correct description of the behavior of the dielectric constant, taking into account excitonic effects.

Quantum criticality of excitonic Mott metal-insulator transitions in black phosphorus

Quantum phase transition refers to the abrupt change of ground states of many-body systems driven by quantum fluctuations. It hosts various intriguing exotic states around its quantum critical points approaching zero temperature. Here we report the spectroscopic and transport evidences of quantum critical phenomena of an exciton Mott metal-insulator-transition in black phosphorus. Continuously tuning the interplay of electron-hole pairs by photo-excitation and using Fourier-transform photo-current spectroscopy as a probe, we measure a comprehensive phase diagram of electron-hole states in temperature and electron-hole pair density parameter space. We characterize an evolution from optical insulator with sharp excitonic transition to metallic electron-hole plasma phases featured by broad absorption and population inversion. We also observe strange metal behavior that resistivity is linear in temperature near the Mott transition boundaries. Our results exemplify an ideal platform to investigating strongly-correlated physics in semiconductors, such as crossover between superconductivity and superfluity of exciton condensation.

Strong exciton bandwidth reduction in pentacene as a function of temperature

The motion of excitons in organic semiconductors represents a key contribution to the performance of organic solar cells. It is determined by intermolecular exciton coupling. In momentum space, exciton coupling results in the exciton dispersion and defines the exciton bandwidth. We demonstrate that the exciton bandwidth in pentacene as measured using electron energy-loss spectroscopy is substantially temperature dependent, and it is drastically reduced going from 20 to 380 K. Following recent theoretical developments, we rationalize this reduction by a huge reduction of the (effective) charge carrier transfer integrals by about 60%. Our results indicate a strongly temperature-dependent energy transport in pentacene and related organic semiconductors.

Tailoring the superposition of finite-momentum valley exciton states in transition-metal dichalcogenide monolayers by using polarized twisted light

A twisted light is a spatially structured light that carries quantized orbital angular momenta (OAM), being a new degree of freedom useful in quantum information technology in addition to that of intrinsic spin angular momentum (SAM), i.e., polarization. Using polarized twisted light to excite valley excitons in transition-metal dichalcogenide monolayers (TMD-ML's) sets up an intriguing photoexcited system which couples comprehensively the excitonic and photonic multi-degrees of freedom, including the center-of-mass motion and valley polarization of exciton and the both optical OAM and SAM. In this work, we present a systematic theoretical investigation of the photoexcited valley excitons in TMD-ML's by polarized Laguerre-Gaussian beams, one of the best known twisted light (TL). We show that the photoexcitation of polarized TL incident to a TMD-ML leads to the formation of the superposition of finite-momentum exciton (SFME) states, spatially localized with the OAM- and SAM-encoded geometrical patterns.

Electrically tunable quantum confinement of neutral excitons.

Confining particles to distances below their de Broglie wavelength discretizes their motional state. This fundamental effect is observed in many physical systems, ranging from electrons confined in atoms or quantum dots1,2 to ultracold atoms trapped in optical tweezers3,4. In solid-state photonics, a long-standing goal has been to achieve fully tunable quantum confinement of optically active electron-hole pairs, known as excitons. To confine excitons, existing approaches mainly rely on material modulation5, which suffers from poor control over the energy and position of trapping potentials. This has severely impeded the engineering of large-scale quantum photonic systems. Here we demonstrate electrically controlled quantum confinement of neutral excitons in 2D semiconductors. By combining gate-defined in-plane electric fields with inherent interactions between excitons and free charges in a lateral p-i-n junction, we achieve exciton confinement below 10 nm. Quantization of excitonic motion manifests in the measured optical response as a ladder of discrete voltage-dependent states below the continuum. Furthermore, we observe that our confining potentials lead to a strong modification of the relative wave function of excitons. Our technique provides an experimental route towards creating scalable arrays of identical single-photon sources and has wide-ranging implications for realizing strongly correlated photonic phases6,7 and on-chip optical quantum information processors8,9.

Quantized Exciton Motion and Fine Energy-Level Structure of a Single Perovskite Nanowire.

The quantum-confinement effect profoundly influences the exciton energy-level structures and recombination dynamics of semiconductor nanostructures but remains largely unexplored in traditional one-dimensional nanowires mainly due to their poor optical qualities. Here, we show that in defect-tolerant perovskite material of highly luminescent CsPbBr3 nanowires, the exciton's center-of-mass motion perpendicular to the axial direction is severely confined. This is reflected in the two sets of photoluminescence spectra emitted from a single CsPbBr3 nanowire, each of which consists of doublet peaks with linear polarizations perpendicular and parallel to the axial direction. Moreover, different exciton states can be mixed by the Rashba spin-orbit coupling effect, resulting in two single photoluminescence peaks with linear polarizations both along the nanowire axis. The above findings mark the emergence of an ideal platform for the exploration of intrinsic one-dimensional exciton photophysics and optoelectronics, thus bridging the long-missing research gap between the well-studied two- and zero-dimensional semiconductor nanostructures.

Omnidirectional exciton diffusion in quasi-2D hybrid organic-inorganic perovskites.

Exciton transport plays a central role in optoelectronic and photonic devices. In quasi-two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs), tightly bound excitons are found to diffuse within 2D layers rapidly with a non-monotonic temperature dependence. Surprisingly, the interlayer exciton diffusion is quite effective as well despite the large interlayer distance. This is in sharp contrast to electron transport, where the interlayer mobility is several orders of magnitude smaller than the intralayer one. Here, we show that the unusual exciton diffusion behaviors can be systematically modeled via the excitonic band structure arising from a long-range dipolar coupling. Coherent exciton motion is interrupted by scattering of impurities at low temperatures and of acoustic/optical phonons at high temperatures. Acoustic and optical phonons modulate the dipole-dipole distance and the dipole orientation, respectively. The ratio of intralayer and interlayer diffusion constants, Dxx/Dzz, is comparable to az/ax with az and ax being the interlayer and intralayer lattice constants of 2D HOIPs, respectively. The efficient and omnidirectional exciton diffusion suggests a great potential of 2D HOIPs in novel excitonic and polaritonic applications.

The low temperature limit of the excitonic Mott density in GaN: an experimental reassessment

The research on GaN lasers aims for a continuous reduction of the lasing threshold. An approach to achieve it consists in exploiting stimulated polariton scattering. This mechanism, and the associated polariton lasers, requires an in-depth knowledge of the GaN excitonic properties, as polaritons result from the coupling of excitons with photons. Under high excitation intensities, exciton states no longer exist due to the Coulomb screening by free carriers; this phenomenon occurs at the so-called Mott density. The aim of this work is to study the bleaching of excitons under a quasi-continuous optical excitation in a bulk GaN sample of high quality through power dependent micro-photoluminescence and time-resolved experiments at 5 K. Time-resolved photoluminescence allows to measure the carrier lifetime as a function of excitation intensity, which is required for a reliable evaluation of the injected carrier density. The vanishing of excitonic lines together with the red-shift of the main emission evidences the occurrence of the Mott transition for a carrier concentration of (6 ± 3) × 1016 cm−3. This value is more than an order of magnitude smaller than previous determinations published in the literature and is in accordance with many-body calculations.

Intrachain Exciton Motion Can Compete with Interchain Hopping in Conjugated Polymer Films with a Strong J-Aggregate Property.

Understanding exciton diffusion properties in organic semiconductor films is crucial for organic solar cells because excitons need to diffuse to an electron donor/acceptor interface to dissociate into charges. We previously found that singlet excitons generated in the thin films of a novel naphthobisoxadiazole-based low-bandgap polymer PNOz4T exhibit two-dimensional exciton diffusion characteristics along the backbone and π-stacking directions owing to the HJ-aggregate property of PNOz4T. However, the diffusion constants along these directions could not be determined owing to the difficulty of data analysis. Herein, we present a detailed analysis based on a simulated annealing metaheuristic. We found that intrachain exciton motion can be faster than interchain hopping. On the basis of temperature dependence measurements, we found that exciton diffusion is more favorable at lower temperatures because the coherent component partly contributes to exciton motion.

In English

It is shown that electron tunneling through a potential barrier that separates two quantum dots of germanium leads to the splitting of electron states localized over spherical interfaces (a quantum dot – a silicon matrix). The dependence of the splitting values of the electron levels on the parameters of the nanosystem (the radius a quantum dot germanium, as well as the distance D between the surfaces of the quantum dots) is obtained. It has been shown that the splitting of electron levels in the QD chain of germanium causes the appearance of a zone of localized electron states, which is located in the bandgap of silicon matrix. It has been found that the motion of a charge-transport exciton along a chain of quantum dots of germanium causes an increase in photoconductivity in the nanosystem. It is shown that in the QD chain of germanium a zone of localized electron states arises, which is located in the bandgap of the silicon matrix. Such a zone of local electron states is caused by the splitting of electron levels in the QD chain of germanium. Moreover, the motion of an electron in the zone of localized electron states causes an increase in photoconductivity in the nanosystem. The effect of increasing photoconductivity can make a significant contribution in the process of converting the energy of the optical range in photosynthesizing nanosystems. It has been found that comparison of the splitting dependence of the exciton level Eех(а) at a certain radius a QD with the experimental value of the width of the zone of localized electron states arising in the QD chain of germanium, allows us to obtain the distances D between the QD surfaces. It has been shown that by changing the parameters of Ge/Si heterostructures with germanium QDs (radius of a germanium QD, as well as the distance D between the surfaces of the QDs), it is possible to vary the positions and widths of the zones of localized electronic states. The latter circumstance opens up new possibilities in the use of such nanoheterostructures as new structural materials for the creation of new nano-optoelectronics and nano-photosynthesizing devices of the infrared range.

Exciton Transitions in Monolayer WS2 Activated by Swift Heavy Ion Irradiation

The emergence of monolayer transition metal dichalcogenides (TMDCs) has provided a favorable platform for exploring a broad range of novel optoelectronic device applications and quantum phenomena due to their remarkable physical and chemical characteristics. Understanding the transition and motion of excitons in TMDCs is of fundamental interest for their optoelectronic devices. Here, we demonstrate the exciton transition in monolayer WS2 that can be fine-tuned by swift heavy ion (SHI) irradiation. The dependence of trion and exciton emissions on SHI irradiation in the as-transferred and as-grown monolayer WS2 was investigated by micro photoluminescence (PL) spectra where different PL responses were monitored. The trion-to-exciton transition in the as-transferred WS2 monolayer was ascribed to SHI irradiation that resulted in charge localization and pre-existing defect annealing, whereas the exciton-to-trion transition in the as-grown WS2 monolayer was attributed to the competition of charge localization and charge transfer caused by SHI irradiation. Femtosecond transient absorption measurements were performed to study the exciton relaxation dynamics in SHI-irradiated WS2, and it was shown that defect-assisted recombination dominates the exciton relaxation process for SHI-irradiated WS2. These results open up new opportunities to manipulate and tune the optical properties of two-dimensional TMDCs, which are of special importance for the development of optoelectronic and valleytronic devices.

An excitonic model for the electron\u2013hole plasma relaxation in proton-irradiated insulators

The relaxation of free electron–hole pairs generated after proton irradiation is modelled by means of a simplified set of hydrodynamic equations. The model describes the coupled evolution of the electron–hole pair and self-trapped exciton (STE) densities, along with the electronic and lattice temperatures. The equilibration of the electronic and lattice excitations is based on the two-temperature model, while two mechanisms for the relaxation of free electron–hole pairs are considered: STE formation and Auger recombination. Coulomb screening and band gap renormalisation are also taken into account. Our numerical results show an ultrafast ({ll },{mathrm {1}} ps) free electron–hole pair relaxation time in amorphous {{mathrm {SiO}}_{mathrm {2}}} for initial carrier densities either below or above the exciton Mott transition. Coulomb screening alone is not found to yield the long relaxation time ({mathrm {gg }}{mathrm {10}} ps) experimentally observed in amorphous {{mathrm {SiO}}_{mathrm {2}}} and borosilicate crown glass BK7 irradiated with high-intensity laser pulses or BK7 irradiated by short proton pulses. Another mechanism, e.g. thermal detrapping of STEs, is required to correctly model the long free electron–hole pair relaxation time observed experimentally.Graphical

Modeling excitonic Mott transitions in two-dimensional semiconductors

We analyze the many-particle correlations that affect the optical properties of two-dimensional semiconductors. These correlations manifest themselves through the specific optical resonances such as excitons, trions, etc. Starting from the generic electron-hole Hamiltonian and employing the microscopic Heisenberg equation of motion the infinite hierarchy of differential equations can be obtained. In order to decouple the system we address the cluster expansion technique which provides a regular procedure of consistent accounting of many-particle correlation contributions into the interband polarization dynamics. In particular, the partially taken into account three-particle correlations modify the behavior of absorption spectra with the emergence of a trion-like peak additional to excitonic ones. In contrast to many other approaches, the proposed one allows us to model the optical response of 2d semiconductors in the regime when the Fermi energies are of the order of the exciton and trion binding energies, thus allowing us to rigorously model the onset of the excitonic Mott transition, the regime being recently studied in various 2d semiconductors, such as transition metal dichalcogenides.

Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores

The particle-like nature of light becomes evident in the photon statistics of fluorescence from single quantum systems as photon antibunching. In multichromophoric systems, exciton diffusion and subsequent annihilation occurs. These processes also yield photon antibunching but cannot be interpreted reliably. Here we develop picosecond time-resolved antibunching to identify and decode such processes. We use this method to measure the true number of chromophores on well-defined multichromophoric DNA-origami structures, and precisely determine the distance-dependent rates of annihilation between excitons. Further, this allows us to measure exciton diffusion in mesoscopic H- and J-type conjugated-polymer aggregates. We distinguish between one-dimensional intra-chain and three-dimensional inter-chain exciton diffusion at different times after excitation and determine the disorder-dependent diffusion lengths. Our method provides a powerful lens through which excitons can be studied at the single-particle level, enabling the rational design of improved excitonic probes such as ultra-bright fluorescent nanoparticles and materials for optoelectronic devices.

Complexity of the dipolar exciton Mott transition in GaN/(AlGa)N nanostructures

The Mott transition from a dipolar excitonic liquid to an electron-hole plasma is demonstrated in a wide GaN/(Al,Ga)N quantum well at $T=7$K by means of spatially-resolved magneto-photoluminescence spectroscopy. Increasing optical excitation density we drive the system from the excitonic state, characterized by a diamagnetic behavior and thus a quadratic energy dependence on the magnetic field, to the unbound electron-hole state, characterized by a linear shift of the emission energy with the magnetic field. The complexity of the system requires to take into account both the density-dependence of the exciton binding energy and the exciton-exciton interaction and correlation energy that are of the same order of magnitude. We estimate the carrier density at Mott transition as $n_\mathrm{Mott}\approx 2\times 10^{11}$cm$^{-2}$ and address the role played by excitonic correlations in this process. Our results strongly rely on the spatial resolution of the photoluminescence and the assessment of the carrier transport. We show, that in contrast to GaAs/(Al,Ga)As systems, where transport of dipolar magnetoexcitons is strongly quenched by the magnetic field due to exciton mass enhancement, in GaN/(Al,Ga)N the band parameters are such that the transport is preserved up to $9$T.

Excitons in a reconstructed moiré potential in twisted WSe2/WSe2 homobilayers.

Moiré superlattices in twisted van der Waals materials have recently emerged as a promising platform for engineering electronic and optical properties. A major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate direct imaging of the moiré structure with optical and electronic properties. Here we develop a secondary electron microscope technique to directly image stacking domains in fully functional van der Waals heterostructure devices. After demonstrating the imaging of AB/BA and ABA/ABC domains in multilayer graphene, we employ this technique to investigate reconstructed moiré patterns in twisted WSe2/WSe2 bilayers and directly correlate the increasing moiré periodicity with the emergence of two distinct exciton species in photoluminescence measurements. These states can be tuned individually through electrostatic gating and feature different valley coherence properties. We attribute our observations to the formation of an array of two intralayer exciton species that reside in alternating locations in the superlattice, and open up new avenues to realize tunable exciton arrays in twisted van der Waals heterostructures, with applications in quantum optoelectronics and explorations of novel many-body systems.

All-optical manipulation of singlet exciton transport in individual supramolecular nanostructures by triplet gating.

Directed transport of singlet excitation energy is a key process in natural light-harvesting systems and a desired feature in assemblies of functional organic molecules for organic electronics and nanotechnology applications. However, progress in this direction is hampered by the lack of concepts and model systems. Here we demonstrate an all-optical approach to manipulate singlet exciton transport pathways within supramolecular nanostructures via singlet-triplet annihilation, i.e., to enforce an effective motion of singlet excitons along a predefined direction. For this proof-of-concept, we locally photo-generate a long-lived triplet exciton population and subsequently a singlet exciton population on single bundles of H-type supramolecular nanofibres using two temporally and spatially separated laser pulses. The local triplet exciton population operates as a gate for the singlet exciton transport since singlet-triplet annihilation hinders singlet exciton motion across the triplet population. We visualize this manipulation of singlet exciton transport via the fluorescence signal from the singlet excitons, using a detection-beam scanning approach combined with time-correlated single-photon counting. Our reversible, all-optical manipulation of singlet exciton transport can pave the way to realising new design principles for functional photonic nanodevices.

Long-range exciton diffusion in a non-fullerene acceptor: approaching the incoherent limit

Low energetic disorder enables the accurate and high-speed prediction of exciton diffusion parameters in a non-fullerene acceptor.

Switching resonance character within merocyanine stacks and its impact on excited-state dynamics

Summary In this study, the optical properties and excited-state dynamics of the unique self-assembled donor-acceptor (DA) merocyanine dye stacks from dimer up to octamer, prepared via dipole-dipole interactions, are reported in terms of coherent exciton dynamics and formation of an excimer-like state. Our findings are based on the steady-state absorption/emission, time-resolved fluorescence, and transient absorption (anisotropy) measurements, including wavepacket analysis and quantum mechanical calculations. Coherent exciton of torsional motions-restricted dye stacks rapidly localizes into the weakly emissive excimer-like state, by shortening the inter-moiety distance and changing the bond-length alternation pattern. The inner merocyanine moiety, having two neighboring units, has a reversed resonance character (non-polar (N) Z) in the ground state. This difference has led to two conclusions: (1) tetramers and octamers exhibit different features of excimer-like state than the dimer, and (2) octamers exhibit slower localization dynamics due to the enhanced homogeneity (six inner-moieties) compared with tetramers (two inner moieties).