Quantum fluctuations of the electromagnetic field are known to produce the atomic Lamb shift. We here reveal their iconic signature in semiconductor physics, through the blue-shift they produce to optically bright excitons, thus lifting the energy of these excitons above their dark counterparts. The electromagnetic field here acts in its full complexity: in addition to the longitudinal part via interband \textit{virtual Coulomb} processes, the transverse part -- which has been missed up to now -- also acts via resonant and nonresonant \textit{virtual photons}. These two parts beautifully combine to produce a bright exciton blue-shift independent of the exciton wave-vector direction. Our work readily leads to a striking prediction: long-lived excitons must have a small bright-dark splitting. Although the analogy between exciton and hydrogen atom could lead us to see the bright exciton shift as a Lamb shift, this is not fully so: the atom shift entirely comes from virtual photons, whereas the Coulomb interaction also contributes to the exciton shift through the so-called "electron-hole exchange".
Excitons - the particle-hole bound states - composed of localized electron-hole states in semiconducting systems are crucial to explaining the optical spectrum. Spectroscopic measurements can contain signatures of these two particle bound states and can be particularly useful in determining the characteristics of these excitons. We formulate an expression for evaluating the angle-resolved photoemission spectrum arising from the ionization of excitons given their steady-state distribution in a semiconductor. We show that the spectrum contains information about the direct/indirect band gap natur…
Mostly, optical spectroscopies are used to investigate the physics of excitons, whereas their electrical evidences are hardly explored. Here, we examined a forward bias activated differential capacitance response of GaInP-AlGaInP based multi-quantum well laser diodes to trace the presence of excitons using electrical measurements. Occurrence of negative activation energy after light emission is understood as thermodynamical signature of steady state excitonic population under intermediate range of carrier injections. Similar corroborative results are also observed in an InGaAs-GaAs quantum dot…
Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS$_2$. We show that photoexcited excitons may be measured and quantified as satellite bands, as well as leading to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton- Floquet phenomenon induced by an exciton time-dependent bosonic field, which is orders of magnitude stronger than l…
With the both spin and valley degrees of freedom, the low-lying excitonic spectra of photo-excited transition-metal dichalcogenide monolayers (TMDC-MLs) are featured by rich fine structures, comprising the intra-valley bright exciton states as well as various intra- and inter-valley dark ones. The latter states can be classified as those of the spin- and momentum-forbidden dark excitons according to the violated optical selection rules. Because of the optical invisibility, the two types of the dark states are in general hardly observed and even distinguished in conventional spectroscopies alth…
The vertical stacking of two-dimensional materials into heterostructures gives rise to a plethora of intriguing optoelectronic properties and presents an unprecedented potential for technological development. While much progress has been made combining different monolayers of transition metal dichalgonenides (TMDs), little is known about TMD-based heterostructures including organic layers of molecules. Here, we present a joint theory-experiment study on a TMD/tetracene heterostructure demonstrating clear signatures of spatially separated interlayer excitons in low temperature photoluminescence…
ARPES signatures of trions in van der Waals materials
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）；Stockholm University（斯德哥尔摩大学）；Georg-August-Universität Göttingen（格奥尔格·奥古斯特哥廷根大学）
The seminal work by T. Kazimierczuk et al. [Nature 514, 343 (2014)] has shown the existence of highly excited exciton states in a regime, where the correspondence principle is applicable and quantum mechanics turns into classical mechanics, however, any interpretation of exciton spectra based on a classical approach to excitons is still missing. Here, we close this gap by computing and comparing quantum mechanical and semiclassical recurrence spectra of cuprous oxide. We show that the quantum mechanical recurrence spectra exhibit peaks, which, by application of semiclassical theories and a sca…
Exciton dynamics, lifetimes and scattering are directly related to the exciton dispersion, or bandstructure. While electron and phonon bandstructures are well understood and can be easily calculated from first principles, the exciton bandstructure is commonly conflated with the underlying electronic bandstructure, where the exciton dispersion is assumed to follow the same dispersion as the electron and hole bands from which it is composed (i.e., the effective mass model). Here, we present a general theory of exciton bandstructure within both ab initio and model Hamiltonian approaches. We show …
Atomistic van der Waals heterostacks are ideal systems for high-temperature exciton condensation because of large exciton binding energies and long lifetimes. Charge transport and electron energy-loss spectroscopy showed first evidence of excitonic many-body states in such two-dimensional materials. Pure optical studies, the most obvious way to access the phase diagram of photogenerated excitons have been elusive. We observe several criticalities in photogenerated exciton ensembles hosted in MoSe2-WSe2 heterostacks with respect to photoluminescence intensity, linewidth, and temporal coherence …
Resonant Raman signatures of bright and momentum-dark exciton coupled by intervalley phonon scattering in monolayer WSe2
University of Münster（明斯特大学）；Center for Soft Nanoscience (SoN), University of Münster（明斯特大学软纳米科学中心）；Technical University of Munich（慕尼黑工业大学）；Walter Schottky Institut and Physics Department, Technical University of Munich（慕尼黑工业大学沃尔特·肖特基研究所与物理系）；MCQST, München（慕尼黑量子科学与技术中心）
Monolayer transition metal dichalcogenides (TMDs) have been in focus of current research, among others due to their remarkable exciton landscape consisting of bright and dark excitonic states. Although dark excitons are not directly visible in optical spectra, they have a large impact on exciton dynamics and hence their understanding is crucial for potential TMD-based applications. Here, we study brightening mechanisms of dark excitons via interaction with phonons and in-plane magnetic fields. We show clear signatures of momentum- and spin-dark excitons in WS$_2$, WSe$_2$ and MoS$_2$, while th…
Excitons, Coulomb-bound electron-hole pairs, are the fundamental excitations governing the optoelectronic properties of semiconductors. While optical signatures of excitons have been studied extensively, experimental access to the excitonic wave function itself has been elusive. Using multidimensional photoemission spectroscopy, we present a momentum-, energy- and time-resolved perspective on excitons in the layered semiconductor WSe$_2$. By tuning the excitation wavelength, we determine the energy-momentum signature of bright exciton formation and its difference from conventional single-parti…
Moiré superlattices open an unprecedented opportunity for tailoring interactions between quantum particles and their coupling to electromagnetic fields. Strong superlattice potential generates moiré minibands of excitons -- bound pairs of electrons and holes that reside either in a single layer (intralayer excitons) or two separate layers (interlayer excitons). The twist-angle-controlled interlayer hybridization of carriers can also mix the two types of excitons to combine the strengths of both. Here, we report a direct observation of spatially mixed moiré excitons in angle-aligned WSe2/WS2 an…
It is shown that the strong Coulomb coupling in intrinsic suspended semiconducting transition metal dichalcogenides can exceed the critical value needed for an excitonic ground state. The dipole-allowed optical excitations then correspond to intra-excitonic transitions such that the optically bright excitonic transitions near the Dirac points have a $p$-like symmetry whereas the $s$-like states are dipole forbidden. The large intrinsic coupling strength seems to be a generic property of the semiconducting transition metal dichalcogenides and strong Coulomb-coupling signatures in the form of th…
2D coherent spectroscopy signatures of exciton condensation in Ta$_2$NiSe$_5$
Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Songshan Lake Materials Laboratory（松山湖材料实验室）；Department of Physics, University of Fribourg（弗里堡大学物理系）；Jožef Stefan Institute（约热·斯特凡研究所）；Faculty of Mathematics and Physics, University of Ljubljana（卢布尔雅那大学数学与物理学院）
We have developed an ab-initio-based fully-quantum numerically-accurate methodology for the simulation of the exciton dynamics and time- and frequency-resolved fluorescence spectra of the cavity-controlled two-dimensional materials at finite temperature and applied this methodology to the single-layer WSe2 system. This allowed us to establish dynamical and spectroscopic signatures of the polaronic and polaritonic effects as well as uncover their characteristic timescales in the relevant range of temperatures.
We have investigated the electronic and optical properties of (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ (x= 0 - 0.375) and (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$ (y= 0 - 0.375) epitaxial thin-films, in which the bandwidth is systematically tuned via chemical substitutions of Sr ions by Ca and Ba. Transport measurements indicate that the thin-film series exhibits insulating behavior, similar to the J$_{eff}$= 1/2 spin-orbit Mott insulator Sr$_2$IrO$_4$. As the average A-site ionic radius increases from (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ to (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$, optical conductivity spectra in the near-infra…
