With the shrinking of dimensionality, Coulomb interactions play a distinct role in two-dimensional (2D) semiconductors owing to the reduced dielectric screening in the out-of-plane direction. Apart from dielectric screening, free charge carriers and/or dipoles can also make a non-negligible contribution to Coulomb interaction. While the Thomas-Fermi model is effective in describing charge carrier screening in three dimensions, the extent of screening to two dimensions resulting from charge carriers and charge-neutral dipoles remains quantitatively unclear. Herein, we present an analytical solution based on linear response theory, offering a comprehensive depiction of the Coulomb screened potential in both 2D and 3D systems, where screening effects from both charge carriers and charge-neutral dipoles are addressed. Our work provides a useful and handy tool for directly analysing and evaluating Coulomb interaction strength in atomically thin materials, particularly in the context of electronic and optoelectronic engineering. As a demonstration, we utilized the derived modified Coulomb potential for the exciton system in 2D semiconductors to estimate the exciton binding energy variation arising from the exciton density fluctuation and temperature-dependent exciton polarizability, yielding excellent agreement with the computational and experimental findings.
Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton…
The competition between the electron-hole Coulomb attraction and the three-dimensional dielectric screening dictates the optical properties of layered semiconductors. In low-dimensional materials, the equilibrium dielectric environment can be significantly altered by the ultrafast excitation of photo-carriers, leading to renormalized band gap and exciton binding energies. Recently, black phosphorus emerged as a 2D material with strongly layer-dependent electronic properties. Here, we resolve the coherent response of screening to sub-gap photo-excitation in bulk black phosphorus and find that m…
I present a fully abinitio scheme to model transient spectroscopy signals in presence of strongly bound excitons. Using LiF as a prototype material, I show that the scheme is able to capture the exciton signature both in time-resolved ARPES and transient absorption experiments. The approach is completely general and can become the reference scheme for modelling pump and probe experiment in a wide range of materials.
We derive a gap equation for bilayer excitonic systems based on density functional theory and benchmark our results against quantum Monte-Carlo simulations and recent experiments on double bilayer graphene. The gap equation has a mean-field form but includes a consistent treatment of dynamical screening. We show that the gap survives at much higher densities than previously thought from mean-field estimates which gives strong indications that the double-bilayer graphene systems at zero magnetic field can be used as model systems to investigate the BCS-BEC crossover. Furthermore, we show that J…
Engineering of the dielectric environment represents a powerful strategy to control the electronic and optical properties of two-dimensional (2D) materials without compromising their structural integrity. Here we show that the recent development of high-$κ$ 2D materials present new opportunities for dielectric engineering. By solving a 2D Mott-Wannier exciton model for WSe$_2$ on different substrates using a screened electron-hole interaction obtained from first principles, we demonstrate that the exciton Rydberg series changes qualitatively when the dielectric screening within the 2D semicond…
We examine a mechanism by which excitons are generated via the LO (longitudinal optical) phonon-assisted scattering process after optical excitation of monolayer transition metal dichalcogenides. The exciton formation time is computed as a function of the exciton center-of-mass wavevector, electron and hole temperatures, and carrier densities for known values of the Fröhlich coupling constant, LO phonon energy, lattice temperature, and the exciton binding energy in layered structures. For the monolayer MoS$_2$, we obtain ultrafast exciton formation times on the sub-picosecond time scale at cha…
Quasiparticle phono-conversion: filming carriers coalescing into excitons
Università di Roma Tor Vergata（罗马托尔维加塔大学）；INFN, Sezione di Roma Tor Vergata（意大利国家核物理研究所罗马托尔维加塔分部）；Okinawa Institute of Science and Technology Graduate University（冲绳科学技术大学院大学）；University of Gdansk（格但斯克大学）；Brookhaven National Laboratory（布鲁克海文国家实验室）
The ab initio Bethe-Salpeter equation (BSE) approach, an established method for the study of excitons in materials, is typically solved in a limit where only static screening from electrons is captured. Here, we generalize this framework to also include dynamical screening from phonons at lowest order in the electron-phonon interaction. We apply this generalized BSE approach to a series of inorganic lead halide perovskites, CsPbX3, with X = Cl, Br, and I. We find that inclusion of screening from phonons significantly reduces the computed exciton binding energies of these systems. By deriving a…
Due to its wide band gap and high carrier mobility, ZnO is an attractive material for light-harvesting and optoelectronic applications. Its functional efficiency, however, is strongly affected by defect-related in-gap states that open up extrinsic decay channels and modify relaxation timescales. As a consequence, almost every ZnO sample behaves differently, leading to irreproducible or even contradicting observations. Here, a complementary set of time-resolved spectroscopies is applied to two ZnO samples of different defect density to disentangle the competing contributions of charge carriers,…
We unravel the influence of quasiparticle screening in the non-equilibrium exciton dynamics of monolayer WS$_2$. We report pump photon energy-dependent exciton blue and red-shifts from time-resolved-reflectance contrast measurements. Based on a phenomenological model, we isolate the effective impact of excitons and free carriers on the renormalization of the quasi-free particle band gap, exciton binding energy and linewidth broadening. By this, our work does not only provide a comprehensive picture of the competing phenomena governing the exciton dynamics in WS$_2$ upon photoexcitation, but al…
The rise of organic electronics calls for versatile modeling tools. In this context, we develop a semiclassical Boltzmann theory that describes transport and excitonic processes in crystalline organic semiconductors on equal footing. The generation of singlet and triplet excitons out of the ground state, their formation from free electrons and holes, the reverse processes, as well as the fusion and fission of excitons are included. The corresponding scattering integrals respect spin conservation, which requires matrix-valued distribution functions. They also include fermionic and bosonic many-…
Carrier and spin recombination are investigated in p-type GaAs of acceptor concentration NA = 1.5 x 10^(17) cm^(-3) using time-resolved photoluminescence spectroscopy at 15 K. At low pho- tocarrier concentration, acceptors are mostly neutral and photoelectrons can either recombine with holes bound to acceptors (e-A0 line) or form excitons which are mostly trapped on neutral acceptors forming the (A0X) complex. It is found that the spin lifetime is shorter for electrons that recombine through the e-A0 transition due to spin relaxation generated by the exchange scattering of free electrons with …
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…
In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on tem…
Atomically thin layers of transition metal dichalcogenides (TMDCs) exhibit exceptionally strong Coulomb interaction between charge carriers due to the two-dimensional carrier confinement in connection with weak dielectric screening. The van der Waals nature of interlayer coupling makes it easy to integrate TMDC layers into heterostructures with different dielectric or metallic substrates. This allows to tailor electronic and optical properties of these materials, as Coulomb interaction inside atomically thin layers is very susceptible to screening by the environment. Here we theoretically inve…
We have quantified substitutional impurity concentrations in synthetic diamond crystals down to sub parts-per-billion levels. The capture lifetimes of electrons and excitons injected by photoexcitation were compared for several samples with different impurity concentrations. Based on the assessed impurity concentrations, we have determined the capture cross section of electrons to boron impurity, sA=1.3x10^-14 cm2, and that of excitons to nitrogen impurity, sD^ex=3.1x10^-14 cm2. The general tendency of the mobility values for different carrier species is successfully reproduced by including ca…
Monolayer transition-metal dichalcogenides (ML-TMDs) offer exciting opportunities to test the manifestations of many-body interactions through changes in the charge density. Tuning the charge density by a gate voltage leads to profound changes in the optical spectra of excitons in ML-TMDs. We review the band-gap renormalization and dynamical screening as a function of charge density, and then incorporate these effects through various approximations that model long-wavelength charge excitations in the Bethe-Salpeter Equation (BSE). We then show that coupling between excitons and shortwave charg…
Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (SWCNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100~meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent …
Two-dimensional Ruddlesden-Popper hybrid lead halide perovskites have become a major topic in perovskite optoelectronics. Here, we aim to unravel the ultrafast dynamics governing the evolution of charge carriers and excitons in these materials. Using a combination of ultrabroadband time-resolved THz (TRTS) and fluorescence upconversion spectroscopies, we find that sequential carrier cooling and exciton formation best explain the observed dynamics, where exciton-exciton interactions play an important role in the form of Auger heating and biexciton formation. We show that the presence of a longe…
We investigate, both theoretically and experimentally, the drift, diffusion, and recombination of excitons in the strain field of an edge threading dislocation intersecting the GaN{0001} surface. We calculate and measure hyperspectral cathodoluminescence maps around the dislocation outcrop for temperatures between 10 to 200 K. Contrary to common belief, the cathodoluminescence intensity contrast is only weakly affected by exciton diffusion, but is caused primarily by exciton dissociation in the piezoelectric field at the dislocation outcrop. Hence, the extension of the dark spots around disloc…
Solar cells based on organometal halide perovskites have recently become very promising among other materials because of their cost-effective character and improvements in efficiency. Such performance is primarily associated with effective light absorption and large diffusion length of charge carriers. Our paper is devoted to the explanation of large diffusion lengths in these systems. The transport mean free path of charged carriers in a perovskite/${\it TiO_2}$ heterojunction that is an important constituent of the solar cells have been analyzed. Large transport length is explained by the pl…
NaSbS2 is a semiconductor that was recently shown to have remarkable efficacy as a solar absorber indicating efficient charge collection even in defected material. We report first principles calculations of properties that show (1) an indirect gap only slightly smaller than the direct gap, which may impede recombination of photoexcited carriers, (2) highly anisotropic electronic and optical properties reflecting a layered crystal structure, (3) a pushed up valence band maximum due to repulsion from the Sb 5s states and (4) cross-gap hybridization between the S p derived valence bands and the S…
When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a fermionic plasma of unbound particles or a bosonic exciton gas. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory including dynamical screening, we show that the exciton-to-plasma ratio can be efficiently tuned by dielectric substrate screening as …
Van der Waals heterostructures provide a versatile tool to not only protect or control, but also enhance the properties of a 2D material. We use ab initio calculations and semi-analytical models to find strategies which boost the mobility of a current-carrying 2D semiconductor within an heterostructure. Free-carrier screening from a metallic "screener" layer remotely suppresses electron-phonon interactions in the current-carrying layer. This concept is most effective in 2D semiconductors whose scattering is dominated by screenable electron-phonon interactions, and in particular the Fröhlich co…
Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena - critical to both many-body physics exploration and device applications - presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energi…
Several models of the charge transfer exciton (CTE) have been proposed to explain its dissociation at the donor-acceptor (DA) interface. However, the underlying physics is still under debate. Here, we derive temperature ($T$)-dependent tight-binding model for an electron-hole pair at the DA interface. The main finding is the existence of the localization-delocalization transition at a critical $T$, which can explain the CTE dissociation. The present study highlights the combined effect of entropy (finite-$T$) and carrier delocalization in the CTE dissociation.
