Ultrafast charge-transfer exciton dynamics in C$_{60}$ thin films
Sebastian Emmerich, Sebastian Hedwig, Benito Arnoldi, Johannes Stöckl, Florian Haag, Ralf Hemm, Mirko Cinchetti, Stefan Mathias, Benjamin Stadtmüller, Martin Aeschlimann
The high flexibility of organic molecules offers great potential for designing the optical properties of light-active materials for the next generation of optoelectronic and photonic applications. However, despite successful implementations of molecular materials in todays' display and photovoltaic technology, many fundamental aspects of the light-to-charge conversion have still to be uncovered. Here, we focus on the ultrafast dynamics of optically excited excitons in C$_{60}$ thin films depending on the molecular coverage and the light-polarization of the optical excitons. Using time- and momentum-resolved photoemission with fs-XUV radiation, we follow the depopulation dynamics in the excited states while simultaneously monitoring the signatures of the excitonic charge character in the molecular valence states. Optical excitation with visible light results in the instantaneous formation of charge-transfer (CT) excitons, which transform stepwise into energetically lower Frenkel-like excitons. While the number and energetic position of energy levels within this cascade process are independent of the molecular coverage and the light polarization of the optical excitation, we find quantitative differences in the depopulation times and the optical excitation efficiency. Our comprehensive study reveals the crucial role of CT excitons for the excited state dynamics of homo-molecular fullerene materials and thin films.
Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic $B$ transition after optical excitation of the energetically lower excitonic $A$ transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a popul…
We study the screened dynamics of the nonequilibrium excitonic consensate forming in a bulk WSe$_{2}$ when illuminated by coherent light resonant with the lowest-energy exciton. Intervalley scattering causes electron migration from the optically populated K valley to the conduction band minimum at $Σ$. Due to the electron-hole unbalance at the K point a plasma of quasi-free holes develops, which efficiently screens the interaction of the remaining excitons. We show that this plasma screening causes an ultrafast melting of the nonequilibrium consensate and that during melting coherent excitons …
Atomically precise lateral heterojunctions based on transition metal dichalcogenides provide a new platform for exploring exciton Mott transition in one-dimension. To investigate the intrinsically non-equilibrium Mott transition, we employed ultrafast microscopy with ~ 200 fs temporal resolution to image the transport of different exciton phases in a type II WSe2-WS1.16Se0.84 lateral heterostructure. These measurements visualized the extremely rapid expansion of a highly non-equilibrium electron-hole (e-h) plasma phase with a Fermi velocity up to 3.2*10^6 cm*s-1. An abrupt first-order exciton …
We demonstrate theoretically and experimentally that the nonlinear interaction between excitations whose harmonic energies coincide gives rise to a strong coupling that opens a new coherent ultrafast energy relaxation path. Instead of an incoherent decay of excitations, that should take a finite time that depends on the energy difference between the initial state and the final state, the nonlinear interaction allows their coherent superposition and thus an instantaneous transfer of the excitation over energies as large as the electron-volt. Such a situation should be encountered in many system…
We study theoretically the ultrafast nonlinear optical response of quantum well excitons in a perpendicular magnetic field. We address the role of many-body correlations originating from the electron scattering between Landau levels (LL). In the linear optical response, the processes involving inter-LL transitions are suppressed provided that the magnetic field is sufficiently strong. However, in the nonlinear response, the Auger processes involving inter-LL scattering of two photoexcited electrons remain unsuppressed. We show that Auger scattering plays the dominant role in the coherent excit…
We discuss a theory of the ultrafast non-linear optical response of excitons in the Quantum Hall system. Our theory focusses on the role of the low energy collective electronic excitations of the cold, strongly correlated, two-dimensional electron gas (2DEG) present in the ground state. It takes into account ground state electron correlations and Pauli exchange and interaction effects between the photoexcited excitons and the collective excitations. Our formulation addresses both the initial coherent regime, where the dynamics is determined by exciton and 2DEG polarizations, and the subsequent…
The newly developed two-dimensional layered materials provide perfect platform for valley-spintronics exploration. To determine the prospect of utilizing the valley degree of freedom, it is of great importance to directly detect and understand the valley dynamics in these materials. Here, the exciton valley dynamics in monolayer WSe$_2$ is investigated by the two-color pump-probe magneto-optical Kerr technique. By tuning the probe photon energy in resonance with the free excitons and trions, the valley relaxation time of different excitonic states in monolayer WSe$_2$ is determined. Valley rel…
Calculations combining first-principles electron-phonon ($e$-ph) interactions with the Boltzmann equation enable studies of ultrafast carrier and phonon dynamics. However, in materials with weak Coulomb screening, electrons and holes form bound excitons and their scattering processes become correlated, posing additional challenges for modeling nonequilibrium physics. Here we show calculations of ultrafast exciton dynamics and related time-domain spectroscopies using $ab~initio$ exciton-phonon (ex-ph) interactions together with an excitonic Boltzmann equation. Starting from the nonequilibrium e…
Using the Feynman-Dyson diagram technique, we study nonlinear polariton-polariton scattering in a two-dimensional micropillar-based optical superlattice with hexagonal symmetry. We demonstrate that both the emerging polariton chirality and the loop Feynman diagrams up to infinite order should be strictly accounted for in the evaluation of the self-energy of the system. Further, we explicitly show that in such a design the time of polariton scattering towards the Dirac points can be drastically decreased which can be used, for instance, in engineering novel classes of polariton lasers with subs…
We demonstrate the feasibility of the time-linear scaling formulation of the $GW$ method [Phys. Rev. Lett. {\bf 124}, 076601 (2020)] for {\it ab initio} simulations of optically driven two-dimensional materials. The time-dependent $GW$ equations are derived and solved numerically in the basis of Bloch states. We address carrier multiplication and relaxation in photo-excited graphene and find deviations from the typical exponential behavior predicted by the Markovian Boltzmann approach. For resonantly pumped semiconductor we discover a self-sustained screening cascade leading to the Mott transi…
Van der Waals heterostructures built by vertically stacked transition metal dichalcogenides (TMDs) exhibit a rich energy landscape including interlayer and intervalley excitons. Recent experiments demonstrated an ultrafast charge transfer in TMD heterostructures. However, the nature of the charge transfer process has remained elusive. Based on a microscopic and material-realistic exciton theory, we reveal that phonon-mediated scattering via strongly hybridized intervalley excitons governs the charge transfer process that occurs on a sub-100fs timescale. We track the time-, momentum-, and energ…
Auger-ionized carriers in a one-dimensional semiconductor are predicted to result in a strong band-gap renormalization. Isolated single-walled carbon nanotubes (SWCNT) under high-intensity laser irradiation exhibit strong nonlinear photoluminescence (PL) due to exciton-exciton annihilation (EEA). The presence of exciton disassociation during the rapid Auger-ionization caused by EEA would lead to a strong nonlinear absorption. By simultaneously measuring SWCNT PL and optical absorption of isolated SWCNT clusters in the PL saturation regime, we give evidence that Auger-ionized excitons do not di…
When a two-level quantum dot and a plasmonic metal nanoantenna are resonantly coupled by the electromagnetic near field, the system can exhibit a Fano resonance, resulting in a transparency dip in the optical spectrum of the coupled system. We calculate the nonlinear response of such a system, for illumination both by continuous-wave and ultrafast pulsed lasers, using both a cavity quantum electrodynamics and a semiclassical coupled-oscillator model. For the experimentally relevant case of meV thermal broadening of the quantum-dot transition, we predict that femtosecond pulsed illumination can…
Molecular materials have emerged as highly tunable materials for photovoltaic and light-harvesting applications. The most severe challenge of this class of materials is the trapping of charge carriers in bound electron-hole pairs, which severely limits the free charge carrier generation. Here, we demonstrate a significant modification of the exciton dynamics of thin films of endohedral metallofullerene complexes upon alkali metal intercalation. For the exemplary case of Sc$_3$N@C$_{80}$ thin films, we show that potassium intercalation results in an additional relaxation channel for the optical…
Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 fs is due to the excitation of graphene excitons, and the slow process at 1.4 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron tra…
We present a detailed investigation of ultrafast (subpicosecond) exciton dynamics in the lattice model of a donor/acceptor heterojunction. Exciton generation by means of a photoexcitation, exciton dissociation, and further charge separation are treated on equal footing. The experimentally observed presence of space-separated charges at $\lesssim 100$ fs after the photoexcitation is usually attributed to ultrafast transitions from excitons in the donor to charge transfer and charge separated states. Here, we show, however, that the space-separated charges appearing on $\lesssim 100$-fs time sca…
We study theoretically the fluctuation properties of acoustic phonons created in a semiconductor quantum dot after ultrafast optical excitation. An excitation with a single ultrafast pulse creates an exciton confined to the quantum dot, which is coupled to longitudinal acoustic phonons. This leads to the formation of a polaron in the quantum dot accompanied by the emission of a phonon wave packet. We show that the fluctuations of the lattice displacement associated with the wave packet after a single laser pulse excitation in resonance with the exciton transition are always larger than their r…
Quantum kinetic equations of motion for the description of the exciton spin dynamics in II-VI diluted magnetic semiconductor quantum wells with laser driving are derived. The model includes the magnetic as well as the nonmagnetic carrier-impurity interaction, the Coulomb interaction, Zeeman terms, and the light-matter coupling, allowing for an explicit treatment of arbitrary excitation pulses. Based on a dynamics-controlled truncation scheme, contributions to the equations of motion up to second order in the generating laser field are taken into account. The correlations between the carrier an…
Van der Waals (vdW) materials, weakly bound layered compounds, have received enormous interest as they offer a malleable playground for a wide range of physical properties in thermal, electronic and optical devices. In particular, owing to their inherent deep subwavelength light confinement, they support a variety of light-matter interactions phenomena such as plasmons, excitons and phonons conveyed as polaritonic modes. Specifically, semiconductor vdW materials such as WSe_2 are particularly attractive for photonic and quantum integrated technologies since they sustain VIS-NIR exciton-polarit…
Transient reflectivity measurements of thin films, ranging from 6 to 40 nm in thickness, of the topological insulator Bi2Se3 revealed a strong dependence of the carrier relaxation time on the film thickness. For thicker films the relaxation dynamics are similar to those of bulk Bi2Se3, where the contribution of the bulk insulating phase dominates over that of the surface metallic phase. The carrier relaxation time shortens with decreasing film thickness, reaching values comparable to those of noble metals. This effect may result from the hybridization of Dirac cone states at the opposite surfa…
We demonstrate that time-delayed nonlinear effects in exciton-polaritons can be used to construct neural networks where information is coded in optical pulses arriving consecutively on the sample. The highly nonlinear effects are induced by time-dependent interactions with the excitonic reservoir. These nonlinearities allow to create a nonlinear XOR logic gate that can perform operations on the picosecond timescale. An optoelectronic neural network based on the constructed logic gate performs classification of spoken digits with a high accuracy rate.
We examine a mechanism by which excitons undergo ultrafast relaxation in common monolayer transition metal dichalcogenides. It is shown that at densities $\approx$ 1$\times$ 10$^{11}$ cm$^{-2}$ and temperatures $ \le 60$ K, excitons in well known monolayers (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$) exist as point-like structureless electron-hole quasi-particles. We evaluate the average rate of exciton energy relaxation due to acoustic phonons via the deformation potential and the piezoelectric coupling mechanisms and examine the effect of spreading of the excitonic wavefunction into the region p…
We present quantitative ultrafast interferometric pump-probe microscopy capable of tracking of photoexcitations with sub 10 nm spatial precision in three dimensions with 15 fs temporal resolution, through retrieval of the full transient photoinduced complex refractive index. We use this methodology to study the spatiotemporal dynamics of the quantum coherent photophysical process of ultrafast singlet exciton fission. Measurements on microcrystalline pentacene films grown on glass (SiO$_2$) and boron nitride (hBN) reveal a 25 nm, 70 fs expansion of the joint-density-of-states along the crystal …
Time- and angle-resolved photoemission spectroscopy (trARPES) is a powerful spectroscopic method to measure the ultrafast electron dynamics directly in momentum-space. However, band gap materials with exceptional strong Coulomb interaction such as monolayer transition metal dichlacogenides (TMDC) exhibit tightly bound excitons, which dominate their optical properties. This rises the question whether excitons, in particular their formation and relaxation dynamics, can be detected in photoemission. Here, we develope a fully microscopic theory of the temporal dynamics of excitonic time- and angle…
Direct observation of ultrafast defect-bound and free exciton dynamics in defect-engineered WS$_2$ monolayers
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory（橡树岭国家实验室纳米材料科学中心）；Center for Integrated Nanotechnologies, Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室集成纳米技术中心）；Honda Research Institute USA Inc.（本田美国研究院）；Department of Materials Science and Engineering, University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校材料科学与工程系）
We perform a $\mathbf{k \cdot p}$ theory analysis of the spectra of the lowest energy and excited states of the excitons in few-layer atomically thin films of InSe taking into account in-plane electric polarizability of the film and the influence of the encapsulation environment. For the thinner films, the lowest-energy state of the exciton is weakly indirect in momentum space, with its dispersion showing minima at a layer-number-dependent wave number, due to an inverted edge of a relatively flat topmost valence band branch of the InSe film spectrum and we compute the activation energy from th…
Transient reflectivity (TR) from thin films (6 - 40 nm thick) of the topological insulator Bi2Se3 reveal ultrafast carrier dynamics, which suggest the existence of both radiative and non-radiative recombination between electrons residing in the upper cone of initially unoccupied high energy Dirac surface states (SS) and holes residing in the lower cone of occupied low energy Dirac SS. The modeling of measured TR traces allowed us to conclude that recombination is induced by the depletion of bulk electrons in films below ~20 nm thick due to the charge captured on the surface defects. We predict…
Heterostructures comprising van der Waals (vdW) stacked transition metal dichalcogenide (TMDC) monolayers are a fascinating class of two-dimensional (2D) materials with unique properties. The presence of interlayer excitons, where the electron and the hole remain spatially separated in the two layers due to ultrafast charge transfer, is an intriguing feature of these heterostructures. Inevitably, the efficiency of 2D heterostructure devices is critically dependent on the charge transfer dynamics. However, the role of the relative rotation angle of the constituent layers on this charge transfer…
Localized excitons play a vital role in the optical response of monolayers of transition metal dichalcogenides and can be exploited as single photon sources for quantum information technology. While the optical properties of such localized excitons are vastly studied, the ultrafast capture process of delocalized excitons into localized potentials is largely unexplored. We perform quantum kinetic calculations of exciton capture via acoustic and optical phonons showing that efficient capture takes place on an ultrafast time scale. The polaron formation in the low-temperature limit leads to highe…
Increasing the speed limits of conventional electronics requires innovative approaches to manipulate other quantum properties of electrons besides their charge. An alternative approach utilizes the valley degree of freedom in low-dimensional semiconductors. Here we demonstrate that the valley degeneracy of exciton energies in transition metal dichalcogenide monolayers may be lifted by coherent optical interactions on timescales corresponding to few tens of femtoseconds. The optical Stark and Bloch-Siegert effects generated by strong nonresonant circularly-polarized light induce valley-selectiv…
Van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS2 p-n type-II heter…
Ultrafast terahertz spectroscopy accesses the {\em dark} excitonic ground state in resonantly-excited (6,5) SWNTs via internal, direct dipole-allowed transitions between lowest lying dark-bright pair state $\sim$6 meV. An analytical model reproduces the response which enables quantitative analysis of transient densities of dark excitons and {\em e-h} plasma, oscillator strength, transition energy renormalization and dynamics. %excitation-induced renormalization. Non-equilibrium, yet stable, quasi-1D quantum states with dark excitonic correlations rapidly emerge even with increasing off-resonan…
The conducting polymer polyaniline (PANI) has a wide range of optoelectronic applications due to its unique electronic and optical characteristics. Although extensive works have been performed to understand the equilibrium properties, the nature of the charge type that governs its non-equilibrium optical response has been barely understood; a number of studies have debated the nature of photo-generated charge type in PANI, specifically whether it is polaron or exciton based. Here, we report experimental evidence that the charge relaxation dynamics of PANI are dominated by excitons. Utilizing u…
Transient reflectivity (TR) measured at laser photon energy 1.51 eV from the indirectly intersurface coupled topological insulator Bi2-xMnxSe3 films (12 nm thick) revealed a strong dependence of the rise-time and initial decay-time constants on photoexcited carrier density and Mn content. In undoped samples (x = 0), these time constants are exclusively governed by electron-electron and electron-phonon scattering, respectively, whereas in films with x = 0.013 - 0.27 ultrafast carrier dynamics are completely controlled by photoexcited electron trapping by ionized Mn2+ acceptors and their dimers.…
We present results on both the intensity and phase-dynamics of the transient non-linear optical response of a single quantum dot (SQD). The time evolution of the Four Wave Mixing (FWM) signal on a subpicosecond time scale is dominated by biexciton effects. In particular, for the cross-polarized excitation case a biexciton bound state is found. In this latter case, mean-field results are shown to give a poor description of the non-linear optical signal at small times. By properly treating exciton-exciton effects in a SQD, coherent oscillations in the FWM signal are clearly demonstrated. These o…
We report a femtosecond mid-infrared study of the broadband low-energy response of individually separated (6,5) and (7,5) single-walled carbon nanotubes. Strong photoinduced absorption is observed around 200 meV, whose transition energy, oscillator strength, resonant chirality enhancement and dynamics manifest the observation of quasi-1D intra-excitonic transitions. A model of the nanotube 1s-2p cross section agrees well with the signal amplitudes. Our study further reveals saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs.
Manifestation of chiral excitons on surfaces of topological insulator thin film with magnetically induced energy gap in the surface spectrum in magnetooptical Kerr and Faraday effects is analyzes. Excitonic contribution to a surface optical conductivity tensor is calculated. Chiral excitons contrary to conventional ones resonantly contribute to Hall conductivity due to lack of the symmetry between the states with opposite angular momentum. They can lead to considerable enhancement of Faraday angle and ellipticity of transmitted electromagnetic wave. Chiral excitons cause decrease of Kerr angle…
We present a novel optical transient absorption and reflection microscope based on a diffraction-limited pump pulse in combination with a wide-field probe pulse, for the spatio-temporal investigation of ultrafast population transport in thin films. The microscope achieves a temporal resolution down to 12 fs and simultaneously provides sub-10 nm spatial accuracy. We demonstrate the capabilities of the microscope by revealing an ultrafast excited-state exciton population transport of up to 32 nm in a thin film of pentacene and by tracking the carrier motion in p-doped silicon. The use of few-cyc…
The recent identification of strongly bound excitons in room temperature anatase TiO$_2$ single crystals and nanoparticles underscores the importance of bulk many-body effects in samples used for applications. Here, for the first time, we unravel the interplay between many-body interactions and correlations in highly-excited anatase TiO$_2$ nanoparticles using ultrafast two-dimensional deep-ultraviolet spectroscopy. With this approach, under non-resonant excitation, we disentangle the optical nonlinearities contributing to the bleach of the lowest direct exciton peak. This allows us to clock t…
A new degree of freedom, the valley pseudospin, emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2) and has attracted great scientific interest. The capability to manipulate the valley pseudospin, in analogy to the control of spin in spintronics, can open up exciting opportunities in valleytronics. Here we demonstrate that an ultrafast and ultrahigh valley pseudomagnetic field can be generated using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Employing ultrafast pump-probe spectroscopy, we observed …
The transient acoustic response of a free-standing, polycrystalline thin Au film upon femtosecond optical excitation has been studied by time-resolved Debye-Scherrer X-ray diffraction using ultrashort Cu K$_α$ X-ray pulses from a laser-driven plasma X-ray source. The temporal strain evolution has been determined from the transient shifts of multiple Bragg diffraction peaks. The experimental data are in good agreement with the results of calculations based on the two-temperature model and an acoustic model assuming uni-axial strain propagation in the laser-excited thin film.
Layered van-der-Waals materials with hexagonal symmetry offer an extra degree of freedom to their electrons, the so called valley index or valley pseudospin. This quantity behaves conceptually like the electron spin and the term valleytronics has been coined. In this context, the group of semiconducting transition-metal dichalcogenides (TMDC) are particularly appealing, due to large spin-orbit interactions and a direct bandgap at the K points of the hexagonal Brillouin zone. In this work, we present investigations of excitonic transitions in mono- and multilayer WSe$_2$ and MoSe$_2$ materials …
We investigate the usefulness and viability of the scheme developed by Viola and Lloyd [Phys. Rev. A 58, 2733 (1998)] to control dephasing in the context of exciton-based quantum computation with self-assembled quantum dots. We demonstrate that optical coherence of a confined exciton qubit exposed to phonon-induced dephasing can be substantially enhanced through the application of a simple periodic sequence of control pulses. The shape of the quantum dot has a significant effect on the dephasing properties. Remarkably, we find that quantum dots with parameters optimized for implementing quantu…
Time-resolved soft-X-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe$_2$. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels reveals a delayed core-hole renormalization due to screening by excited quasi-free carriers, revealing an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectr…
While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ va…
The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including NMR, quantum communication, and quantum computation. Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics. Valley exciton polarization has been created in the transition metal dichalcogenide (TMDC) monolayers using excitation by circularly polarized light and has been detected both optically and…
We use time-resolved x-ray resonant magnetic scattering (tr-XRMS) at the Co M$_{2,3}$- and Tb O$_1$-edges to study ultrafast demagnetization in an amorphous Co$_{88}$Tb$_{12}$ alloy with stripe domains. Combining the femtosecond temporal with nanometer spatial resolution of our experiment, we demonstrate that the equilibrium spin texture of the thin film remains unaltered by the optical pump-pulse on ultrashort timescales ($<$1 ps). However, after $\simeq$ 4 ps, we observe the onset of a significant domain wall broadening, which we attribute to a reduction of the uniaxial magnetic anisotropy o…
The origin of charge density waves (CDW) in TiSe$_2$ has long been debated, mainly due to the difficulties in identifying the timescales of how and when the excitonic pairing and electron-phonon coupling (EPC) come into play. Without a proper time resolution and microscopic mechanism, one has to assume simultaneous appearance of CDW and periodic lattice distortions (PLD). Here, we accomplish a complete separation of exciton and PLD dynamics and unravel their interplay in the ultrafast time domain in our real-time time-dependent density functional theory simulations. We find that laser pulses k…
