Single-layer transition metal dichalcogenides are at the center of an ever increasing research effort both in terms of fundamental physics and applications. Exciton-phonon coupling plays a key role in determining the (opto)electronic properties of these materials. However, the exciton-phonon coupling strength has not been measured at room temperature. Here, we develop two-dimensional micro-spectroscopy to determine exciton-phonon coupling of single-layer MoSe2. We detect beating signals as a function of waiting time T, induced by the coupling between the A exciton and the A'1 optical phonon. Analysis of two-dimensional beating maps combined with simulations provides the exciton-phonon coupling. The Huang-Rhys factor of ~1 is larger than in most other inorganic semiconductor nanostructures. Our technique offers a unique tool to measure exciton-phonon coupling also in other heterogeneous semiconducting systems with a spatial resolution ~260 nm, and will provide design-relevant parameters for the development of optoelectronic devices.
We report a photoluminescence observation of robust excitonic polarons due to strong coupling of exciton and longitudinal optical (LO) phonon as well as Fano-type interference in high quality ZnO crystal. At low enough temperatures, the strong coupling of excitons and LO phonons leads to not only traditional Stokes lines (SLs) but also up to second-order anti-Stokes lines (ASLs) besides the zero-phonon line (ZPL). The SLs and ASLs are found to be not mirror symmetric with respect to the ZPL, strongly suggesting that they are from different coupling states of exciton and phonons. It is more int…
We analyse the interaction of exciton and exciton-polariton condensates in semiconductor microcavity with a coherent acoustic wave. An analytical solution for the dispersion of excitations of coupled condensate-phonon system is found in the approximation of k-independent interactions. Accounting for k-dependence results in a stronger modification of the dispersion, and even in the appearance of the "roton instability" region.
Temperature-dependent radiative recombination of free excitons involving one or two LO phonons in GaN is investigated in detail. It is found that both phonon sidebands possess asymmetric lineshape and their energy spacings from the zero phonon line strongly deviate from the characteristic energy of LO phonons as the temperature increases. Furthermore, the deviation rates of one and two phonon sidebands are significantly different. Segall-Mahan theory, taking the exciton-photon and exciton-phonon interactions into account, is employed to calculate the sidebands of one or two LO phonons for free…
Moiré patterns with angular mismatch in van der Waals heterostructures composed of atomically thin semiconducting materials are a fascinating platform to engineer the optically generated excitonic properties towards novel quantum phenomena. The moiré pattern as a periodic trap potential can give rise to spatially ordered zero-dimensional (0D) exciton ensembles, which offers the possibility for dense coherent quantum emitters and quantum simulation of many-body physics. The intriguing moiré exciton properties are affected by their dynamics and exciton-phonon interaction. However, the moiré exci…
We study theoretically the contribution of quantum effects to the exciton diffusion coefficient in atomically thin crystals. It is related to the weak localization caused by the interference of excitonic wavefunctions on the trajectories with closed loops. Due to a weak inelasticity of the exciton-phonon interaction the effect is present even if the excitons are scattered by long-wavelength acoustic phonons. We consider exciton interaction with longitudinal acoustic phonons with linear dispersion and with flexural phonons with quadratic dispersion. We identify the regimes where the weak locali…
We investigate the spin-nonconserving relaxation channel of excitons by their couplings with phonons in two-dimensional transition metal dichalcogenides using $\textit{ab initio}$ approaches. Combining $\text{GW}$-Bethe-Salpeter equation method and density functional perturbation theory, we calculate the electron-phonon and exciton-phonon coupling matrix elements for the spin-flip scattering in monolayer WSe$_{\text{2}}$, and further analyze the microscopic mechanisms influencing these scattering strengths. We find that phonons could produce effective in-plane magnetic fields which flip spin o…
We develop a theory of the linear optical spectrum of excitons in quantum dot molecules, including the effect of exciton-phonon coupling beyond the Markov limit. The model reproduces the general trend of the zero-phonon line broadening as a function of interdot distance, that were recently measured. The unexpectedly broad linewidths and their large variation are explained in terms of both the non-Markov nature of the coupling and of the matching of the phonon wavelength to the interdot distance.
We report resonant Raman spectroscopy of neutral excitons X$^0$ and intravalley trions X$^-$ in hBN-encapsulated MoS$_2$ monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS$_2$ lattice phonons and X$^0$/X$^-$ emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X$^0$-induced Raman scattering and a suppression for X$^-$-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermedia…
Moiré Phonons and Emergent Exciton-Phonon Coupling in a Moiré Heterobilayer
University of California, Berkeley（加州大学伯克利分校）；Kavli Energy NanoScience Institute（卡弗里能源纳米科学研究所）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Indian Institute of Science（印度科学学院）；Newcastle University（纽卡斯尔大学）；National Institute for Materials Science（国立材料研究所）；University of Texas at Austin（德克萨斯大学奥斯汀分校）；Northeastern University（东北大学）
Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications in nano-electronics. In this work, we study the incoherent optical phonon and exciton population dynamics in monolayer WS2 by time-resolved spontaneous Raman scattering spectroscopy. Upon excitation of the exciton transition, both the Stokes and anti-Stokes optical phonon scattering strength exhibit a large reduction. Based on the detailed balance, the optical phonon population is retrieved, which shows an instant build-up and a relaxation lifet…
Electron-phonon ($e$-ph) interactions are key to understanding the dynamics of electrons in materials, and can be modeled accurately from first-principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for computing exciton-phonon (ex-ph) interactions and the associated exciton dynamical processes from first principles. Starting from the ab initio Bethe-Salpeter equation, we derive expressions for the ex-ph matrix elements and relaxation tim…
The photoluminescence (PL) spectrum of transition metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of momentum-dark excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as result of different configurations of bright…
In monolayer semiconductor transition metal dichalcogenides, the exciton-phonon interaction is expected to strongly affect the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M). Oscillatory behavior is also observed in the steady-state emission linewidth and in timeresolved photoluminescence excitation data, which reveals variation with excitation energy in the exciton lifetime. T…
The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects because they possess unique spin-valley locking physics for hosting rich excitonic species and the reduced screening for strong Coulomb interactions. Here, we report the observation of multiple valley phonons, phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone, and the resulting exciton complexes…
We discuss how excitons can affect the generation of coherent radial breathing modes in ultrafast spectroscopy of single wall carbon nanotubes. Photoexcited excitons can be localized spatially and give rise to a spatially distributed driving force in real space which involves many phonon wavevectors of the exciton-phonon interaction. The equation of motion for the coherent phonons is modeled phenomenologically by the Klein-Gordon equation, which we solve for the oscillation amplitudes as a function of space and time. By averaging the calculated amplitudes per nanotube length, we obtain time-de…
We study theoretically the non-equilibrium exciton transport in monolayer transition metal dichalcogenides. We consider the situation where excitons interact with non-equilibrium phonons, e.g., under the conditions of localized excitation where a ``hot spot'' in formed. We develop the theory of the exciton drag by the phonons and analyze in detail the regimes of diffusive propagation of phonons and ballistic propagation of phonons where the phonon wind is formed. We demonstrate that a halo-like spatial distribution of excitons akin observed in [Phys. Rev. Lett. 120, 207401 (2018)] can be forme…
We present an \textit{ab initio} method to calculate phonon-assisted absorption and emission spectra in the presence of strong excitonic effects. We apply the method to bulk hexagonal BN which has an indirect band gap and is known for its strong luminescence in the UV range. We first analyse the excitons at the wave vector $\overline{q}$ of the indirect gap. The coupling of these excitons with the various phonon modes at $\overline{q}$ is expressed in terms of a product of the mean square displacement of the atoms and the second derivative of the optical response function with respect to atomi…
Excitonic quasi-particles, excitons/trions/bi-excitons, and their coupling with phonons and charge carriers play a crucial role in controlling the optical properties of atomically thin semiconducting 2D materials. In this work, we unravelled the dynamics of excitons/trions and their coupling with phonons and charge carriers in a few layers vertically and horizontally aligned MoS2. We observed trion signature up to the highest recorded temperature (330 K) in both systems and have shown that the dynamics of excitons/trions and their coupling with phonons and electrons are more affected in vertic…
In organic semiconductors working under ambient circumstance, there are remarkable quantum effects lack of comprehensive understanding, and an exotic composite particle named charge transfer (CT) exciton is normally regarded as the key ingredient. Another essential substance is the phonons stemming from intra- and inter-molecular vibrations, and the relevant diagonal electron-phonon couplings give rise to spatial localization and the off-diagonal couplings refer to the dispersion of electron wavefunctions. In this work, we first propose a toy model based upon the fracton physics to phenomenolo…
Hexagonal boron nitride (hBN) is a wide band gap material with both strong excitonic light emission in the ultraviolet and strong exciton-phonon coupling. Luminescence experiments performed on the recently synthesized monolayer form (m-hBN) present emission spectra that differ from one another, with some suggesting a coexistence between phonon-assisted and direct emission channels. Motivated by these results, we investigated the optical response of (m-hBN) using a new \textit{ab initio} approach that takes into account the effects of atomic vibrations on the luminescence spectra. We construct …
Far from resonance, the coupling of the G-band phonon to magneto-excitons in single layer graphene displays kinks and splittings versus filling factor that are well described by Pauli blocking and unblocking of inter- and intra- Landau level transitions. We explore the non-resonant electron-phonon coupling by high-magnetic field Raman scattering while electrostatic tuning of the carrier density controls the filling factor. We show qualitative and quantitative agreement between spectra and a linearized model of electron-phonon interactions in magnetic fields. The splitting is caused by dichrois…
The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is…
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）
The optical properties of the two-dimensional (2D) crystals are dominated by tightly bound electron-hole pairs (excitons) and lattice vibration modes (phonons). The exciton-phonon interaction is fundamentally important to understand the optical properties of 2D materials and thus help develop emerging 2D crystal based optoelectronic devices. Here, we presented the excitonic resonant Raman scattering (RRS) spectra of few-layer WS$_2$ excited by 11 lasers lines covered all of A, B and C exciton transition energies at different sample temperatures from 4 to 300 K. As a result, we are not only abl…
We study exciton radiative decay in a two-dimensional material, taking into account large thermal population in the non-radiative states, from which excitons are scattered into the radiative states by acoustic phonons. We find an analytical solution of the kinetic equation for the non-equilibrium distribution function of excitons in the radiative states. Our estimates for bright excitons in transition metal dichalcogenides indicate a strong depletion of radiative state population due to insufficient exciton-phonon scattering rate at low temperatures.
The ability to assemble layers of two-dimensional (2D) materials to form permutations of van der Waals heterostructures provides significant opportunities in materials design and synthesis. Interlayer interactions provide a path to new properties and functionality, and understanding such interactions is essential to that end. Here we report formation of interlayer exciton-phonon bound states in Bi2Se3/WS2 heterostructures, where the Bi2Se3 A1(3) surface phonon, a mode particularly susceptible to electron-phonon coupling, is imprinted onto the excitonic emission of the WS2. The exciton-phonon b…
The dynamics of an exciton-LO-phonon system after an ultrafast optical excitation in an InAs/GaAs quantum dot is studied theoretically. Influence of anharmonic phonon damping and its interplay with the phonon dispersion is analyzed. The signatures of the zone-edge decay process in the absorption spectrum and time evolution are highlighted, providing a possible way of experimental investigation on phonon anharmonicity effects.
We report the direct observation of intervalley exciton between the Q conduction valley and $Γ$ valence valley in bilayer WSe$_2$ by photoluminescence. The Q$Γ$ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe$_2$. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between Q$Γ$ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between Q$Γ$ and QK excitons. Both Q$Γ$ and QK excitons exhibit pronounced phonon re…
We measured absorption spectra of T-shaped quantum wires at room temperature using waveguide-transmission spectroscopy. Strong and narrow room-temperature one-dimensional-exciton absorption peak was observed, which shows peak modal absorption coefficient of 160 cm$^{-1}$ per 20 wires with $Γ$-factor of $4.3\times10^{-3}$, width of 7.2 meV, and strong polarization anisotropy.
For monolayer transition metal chalcogenides (TMDs), electrons and excitons in different valleys can be driven to opposite directions by the Berry curvature, serving as a valley-dependent effective magnetic field. In addition to monolayer TMDs, Van der Waals heterostructures provide an attractive platform for emerging valley physics and devices with superior physics properties. Interlayer excitons in TMD heterostructures have a long valley lifetime as compared to monolayer intralayer excitons. Here we report an interlayer exciton valley polarization and valley Hall effect in MoS2/WSe2 in room …
Indirect excitons (IXs) in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by a high binding energy making them stable at room temperature and giving the opportunity for exploring fundamental phenomena in excitonic systems and developing excitonic devices operational at high temperatures. We present the observation of IXs at room temperature in van der Waals TMD heterostructures based on monolayers of MoS$_2$ separated by atomically thin hexagonal boron nitride. The IXs realized in the TMD heterostructure have lifetimes orders of magnitude longer than lif…
By considering driven diffusive dynamics of exciton polaritons in an optical microcavity with an embedded molybdenum disulfide monolayer, we determine experimentally relevant range of parameters at which room-temperature superfuidity can be observed. It is shown that the superfluid transitions occurs in a trapped polariton gas at laser pumping power $P>600$ mW and and trapping potential strength $k > 50$ eV/cm$^2$. We also propose a simple analytic model that provides a useful estimate for the polariton gas density, which enables one to determine the conditions for observation of room temperat…
Phonons are well known to be the main mechanism for the coupling between bright and dark excitons in nonmagnetic semiconductors. Here, we investigate diluted magnetic semiconductors where this process is in direct competition with the scattering at localized magnetic impurities. To this end, a recently developed quantum kinetic description of the exciton spin dynamics in diluted magnetic semiconductor quantum wells is extended by the scattering with longitudinal acoustic phonons. A strong phonon impact is found in the redistribution of exciton momenta on the exciton parabola that becomes espec…
Tungsten-based monolayer transition metal dichalcogenides host a long-lived dark exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located be…
Electron-phonon and exciton-phonon interactions in nanoclusters are formulated and computed under the framework of GW-BSE (Bethe-Salpeter equation) approach. The phonon effect is modeled with the two-particle representation for the first time. The nonradiative relaxation rates of electrons and excitons are calculated. It is uncovered that both single-phonon relaxation and multiple-phonon relaxation are significant in nanocrystals, and correspond to two types of physical processes that have totally different spectral lineshapes. Furthermore, the multiple-phonon relaxation always occurs and its …
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 observe a set of three replica luminescent peaks at ~21.4 meV below the dark exciton, negative and positive dark trions (or exciton-polarons) in monolayer WSe2. The replica redshift energy matches the energy of the zone-center E"-mode optical phonons. The phonon replicas exhibit parallel gate dependence and same g-factors as the dark excitonic states, but follow the valley selection rules of the bright excitonic states. While the dark states exhibit out-of-plane transition dipole and valley-independent linearly polarized emission in the in-plane directions, their phonon replicas exhibit in-…
Systems supporting exciton-polaritons represent solid-state optical platforms with a strong built-in optical nonlinearity provided by exciton-exciton interactions. In conventional semiconductors with hydrogen-like excitons the nonlinearity rate demonstrates the inverse scaling with the binding energy. This makes excitons stable at room temperatures weakly interacting, which obviously limits the possibilities of practical applications of the corresponding materials for nonlinear photonics. We demonstrate experimentally and theoretically, that these limitations can be substantially softened in h…
Engineering non-linear hybrid light-matter states in tailored optical lattices is a central research strategy for the simulation of complex Hamiltonians. Excitons in atomically thin crystals are an ideal active medium for such purposes, since they couple strongly with light and bear the potential to harness giant non-linearities and interactions while presenting a simple sample-processing and room temperature operability. We demonstrate lattice polaritons, based on an open, high-quality optical cavity, with an imprinted photonic lattice strongly coupled to excitons in a WS$_{2}$ monolayer. We …
Large-radius excitons in polar crystals are considered. It is shown that translation invariant description of excitons interacting with a phonon field leads to a nonzero contribution of phonons into the exciton ground state energy only in the case of weak or intermediate electron-phonon coupling. A conclusion is made that self-trapped excitons cannot exist in the limit of strong coupling. Peculiarities of the absorption and emission spectra of translation invariant excitons in a phonon field are discussed. Conditions when the hydrogen-like exciton model remains valid in the case of electron-ph…
We report on the exciton formation and relaxation dynamics following photocarrier injection in a single-layer two-dimensional lead-iodide perovskite. We probe the time evolution of four distinct exciton resonances by means of time-resolved photoluminescence and transient absorption spectroscopies, and find that at 5\,K a subset of excitons form on a $\lesssim$ 1-ps timescale, and that these relax subsequently to lower-energy excitons on $\sim$ 5--10\,ps with a marked temperature dependence over $<$ 100\,K. We implement a mode projection analysis that determines the relative contribution of all…
In semiconductor quantum dots the coupling to the environment, i.e. to phonons, plays a crucial role for optical state preparation. We analyze the phonon impact on two methods for a direct optical preparation of the dark exciton, which is enabled by a tilted magnetic field: the excitation with a chirped laser pulse and the excitation with a detuned pulse. Our study reveals that for both methods phonons either do not impede the proposed mechanism or are even useful by widening the parameter range where a dark state preparation is possible due to phonon-assisted dark exciton preparation. In view…
Hybrid Perovskites have shown a great potential for applications in photovoltaics and light-emitting devices with high efficiency. Interaction between defect-induced trapped excitons and phonons plays an important role in understanding the emerging phenomena for such an excellent figure-of-merit. Here we demonstrate hot polarons with narrow linewidth in $\mathrm{CH_{3}NH_{3}PbBr_{3}}$ nanowires, which originate from the interaction between trapped excitons and octahedra-twist phonons. The observation of hot polarons in photoluminescence without gain methods indicates the large interaction stre…
The interaction between exciton and acoustic phonons via deformation potential in PbS nanocrystals is calculated in the ${\bf k} \cdot {\bf p}$ model. The size-dependence of the Huang-Rhys factors for the fundamental breathing mode and its overtones as well as for spheroidal vibrations with the total angular momentum $j=2$ are evaluated.
Two-dimensional transition metal dichalcogenides (TMDs) provide an attractive platform for studying strain dependent exciton transport at room temperature due to large exciton binding energy and strong bandgap sensitivity to mechanical stimuli. Here, we use Rayleigh type surface acoustic wave (SAW) to demonstrate controlled and directional exciton transport under weak coupling regime at room temperature. We screen the in-plane piezoelectric field using photogenerated carriers to study transport under type-I bandgap modulation and measure a maximum exciton drift velocity of 600 m/s. Furthermore…
We investigate the correction of interlayer exciton binding energy in transition metal dichalcogenides double layers arising from the exciton-optical phonon coupling using the method of Lee-Low-Pines unitary transformation. We find that the binding energy varies in several tens of meV, depending on the polarizability of materials and interlayer distance between double layers. Moreover, the correction of binding energy results in the remarkable increasing of the critical temperature for the condensation of dilute excitonic gas basing on the Berezinskii-Kosterlitz-Thouless model. These results n…
Impact of exciton-phonon and exciton-magnon interaction on transport in anisotropic 2D magnetic semiconductors
Philipps-Universität Marburg（马尔堡菲利普斯大学）；mar.quest—Marburg Center for Quantum Materials and Sustainable Technologies（mar.quest——马尔堡量子材料与可持续技术中心）；University of Münster（明斯特大学）
Memory and correlation effects in the interband absorption from quantum wells due to exciton-phonon dynamics are investigated. They are traced back to the frequency dependence and matrix character of the self energy arising in a 2nd Born theory. It is found that interpeak absorption increases with respect to the case in which this memory and correlation effects are neglected.
We report the first high-field magneto-optical study on the exciton-phonon sideband of single-walled carbon nanotubes (SWNTs) consisting only of (6,5) species. Both energy and intensity of the observed phonon sideband were found to be independent of the external magnetic field. Comparing with theoretical calculations, we confirmed that these sidebands originate from the optically forbidden K-momentum singlet excitons. Energy of these K-momentum dark excitons was extracted to be ~ 21.5 meV above the bright zero-momentum singlet excitons, in close agreement with recent theoretical predictions an…
The novel method of observation and controlling of Bose-Einstein condensation in the system of spatially and momentum-space indirect excitons in coupled quantum wells using in-plane magnetic and normal electric fields is proposed. Fields are used for exciton dispersion engeneering. In the presence of in-plane magnetic field ground state of spatially indirect exciton becomes also indirect in the momentum space. Manipulation of electric field magnitude is used for tuning to resonance of transition of "dark" long-life spatially and momentum-space indirect exciton in condensate into spatially and …
