Low-Energy Purification of Crystal Defects by Rydberg Excitons
Department of Chemistry, Purdue University（普渡大学化学系）；Institute for Molecules and Materials, Radboud University（拉德堡德大学分子与材料研究所）；Department of Physics and Astronomy, Purdue University（普渡大学物理与天文学系）；Purdue Quantum Science and Engineering Institute, Purdue University（普渡大学量子科学与工程研究所）
Recent experiments show that optically generated Rydberg excitons in cuprous oxide can neutralize charged impurities, strongly reducing stray electric fields and effectively purifying the crystal. Here, we develop a multichannel theory of Rydberg exciton-impurity scattering that resolves the competing roles of capture, elastic scattering, and inelastic transitions between excitonic states. We find that at high collision energies, as effective under conventional single-photon excitation, purification is reduced relative to Langevin capture. These collisions are accompanied by inelastic redistribution and dominant elastic scattering, including pronounced glory scattering, which suppress purification efficiency. We identify a quantum regime at ultralow collision energies favorable for purification, where only the s-wave contributes: capture is enhanced while elastic and inelastic channels are strongly suppressed. This regime can be accessed via degenerate two-photon excitation of even-parity Rydberg excitons with tunable recoil, additionally enabling the systematic exploration of exciton-impurity scattering over a wide range of collision energies beyond what is readily achievable in atomic counterparts in atomic gas experiments.
We investigate the formation of waveguides for Rydberg excitons in Cu$_\text{2}$O from cylindrical stressors as alternatives to optical traps. We show that the achievable potential depths can easily reach the meV and the trap frequencies the GHz regimes. For Rydberg excitons, we find that it is sufficient to consider only the shift of the band gap, whereas the excitonic binding energies remain almost unchanged.
The quantum confinement of Rydberg excitons is an important step towards exploiting their large nonlinearities for quantum applications. We observe Rydberg excitons in natural nanoparticles of Cu$_2$O. We resolve up to the principal quantum number $n=12$ in a bulk Cu$_2$O crystal and up to $n=6$ in nanoparticles extracted from the same crystal. The exciton transitions in nanoparticles are broadened and their oscillator strengths decrease as $\propto n^{-4}$ compared to those in the bulk (decreasing as $\propto n^{-3}$). We explain our results by including the effect of quantum confinement of e…
We analyze theoretically the Coulomb scattering processes of highly excited excitons in the direct bandgap semiconductor quantum wells. We find that contrary to the interaction of ground state excitons the electron and hole exchange interaction between excited excitons has an attractive character both for $s$- and $p$-type 2D excitons. Moreover, we show that similarly to the three-dimensional (3D) highly excited excitons, the direct interaction of 2D Rydberg excitons exhibits van der Waals type long-range interaction. The results predict the linear growth of the absolute value of exchange inte…
We develop a many-body approach to the behavior of exciton bound states and the conduction electron band edge in a surrounding electron-hole plasma with a focus on the absorption spectrum of Rydberg excitons in cuprous oxide. The interplay of band edge and exciton levels is analyzed numerically, whereby the self-consistent solution is compared to the semiclassical Debye approximation. Our results provide criteria which allow to verify or rule out the different band edge models against future experimental data.
Coherent optical control of individual particles has been demonstrated both for atoms and semiconductor quantum dots. Here we demonstrate the emergence of quantum coherent effects in semiconductor Rydberg excitons in bulk Cu$_2$O. Due to the spectral proximity between two adjacent Rydberg exciton states, a single-frequency laser may pump both resonances with little dissipation from the detuning. As a consequence, additional resonances appear in the absorption spectrum that correspond to dressed states consisting of two Rydberg exciton levels coupled to the excitonic vacuum, forming a V-type th…
We perform a polarization-resolved magnetoluminescence study of excitons in ReS$_2$. We observe that two linearly polarized Rydberg series of excitons are accompanied by two other Rydberg series of dark excitons, brightened by an in-plane magnetic field. All series extrapolate to the same single-electron bandgap, indicating that the observed excitons originate either from the same valley or from two valleys related by the inversion symmetry, and are split by exchange interaction. To interpret our observations of the magnetic brightening, we have to assume the dominant spin-orbit coupling to be…
We show how to compute the magnetooptical functions (absorption, reflection, and transmission) when Rydberg Exciton-Polaritons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field, and the polaritonic effect. Using the Real Density Matrix Approach the analytical expressions for magnetooptical functions are obtained and numerical calculations for Cu$_2$0 crystal are performed. The influence of the strength of applied external magnetic field on the resonance displacement of excitonic spectra is discussed. We report a good agreement with recen…
We show how to compute the electrooptical functions (absorption, reflection, and transmission) when Rydberg Excitons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. With the use of Real Density Matrix Approach numerical calculations applied for Cu$_2$0 crystal are performed. We also examine in detail and explain the dependence of the resonance displacement on the state number and applied electric field strength. We report a good agreement with recently published experimental data.
We report the experimental observation of radiative recombination from Rydberg excitons in a two-dimensional semiconductor, monolayer WSe2, encapsulated in hexagonal boron nitride. Excitonic emission up to the 4s excited state is directly observed in photoluminescence spectroscopy in an out-of-plane magnetic field up to 31 Tesla. We confirm the progressively larger exciton size for higher energy excited states through diamagnetic shift measurements. This also enables us to estimate the 1s exciton binding energy to be about 170 meV, which is significantly smaller than most previous reports. The…
We investigate the influence of a static, uncorrelated distribution of charged impurities on the spectrum of bound excitons in the copper oxide Cu$_{\text{2}}$O. We show that the statistical distribution of Stark shifts and ionisation rates leads to the vanishing of Rydberg resonances into an apparent continuum. The appearance of additional absorption lines due to the broken rotational symmetry, together with spatially inhomogeneous Stark shifts, leads to a modification of the observed line shapes that agree qualitatively with the changes observed in the experiment.
We investigate the infrared optical transitions between excitons of the yellow, green and blue series in the cuprous oxide Cu$_{\mathrm{2}}$O. We show that in many cases the dipole approximation is inadequate and, in particular, that it breaks down in yellow-blue transitions even for moderate principal quantum numbers of $n \approx 10$. The interband matrix elements of the transition operator needed for the evaluation of the excitonic transition strengths are derived from known as well as from fitted band parameters.
We study the effects of Rashba spin-orbit coupling on two-dimensional Rydberg exciton systems. Using analytical and numerical arguments we demonstrate that this coupling considerably modifies the wave functions and leads to a level repulsion that results in a deviation from the Poissonian statistics of the adjacent level distance distribution. This signifies the crossover to non-integrability of the system and hints on the possibility of quantum chaos emerging. Such a behavior strongly differs from the classical realization, where spin-orbit coupling produces highly entangled, chaotic electron…
Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is "dark", although possibly …
We show how to compute the optical functions when Rydberg Excitons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. We use the Real Density Matrix Approach (RDMA), which, combined with Green's function method, enables one to derive analytical expressions for the optical functions. Choosing the susceptibility, we performed numerical calculations appropriate to a Cu$_2$0 crystal. The effect of the coherence is displayed in the line shape. We also examine in details and explain the dependence of the oscillator strength and the resonance p…
We investigate the optical transition selection rules for excitonic Rydberg series formed in massive Dirac cones. The entanglement of the exciton envelop function with the pseudospin texture leads to anomalous selection rules for one-photon generation of excitons, where $d$-orbitals can be excited with the opposite helicity selection rule from the $s$-orbitals in a given valley. The trigonal warping effects in realistic hexagonal lattices further renders more excited states bright, where $p$-orbitals can also be accessed by one-photon excitation with the opposite valley selection rules to the …
We propose a scheme for calculation of optical functions of a semiconductor with Rydberg excitons, for a wide interval of dimensions. We start with 2-dimensional structure, then going to thin films and ending on 3-dimensional bulk crystals. The calculations including the polaritons are performed, the case of large number of polariton branches is discussed and obtained theoretical absorption spectra show good agreement with experimental data.
Rydberg excitons in Cu2O can be an emergent platform for solid-state quantum information processing by utilizing the exaggerated properties of high-lying excited states within the material. To develop practical quantum systems, high-temperature operation is desirable. Here, we study the temperature-dependence of the yellow and green Rydberg exciton resonances in a thin Cu2O crystal via broad-band phonon-assisted absorption spectra between 4 K and 100 K. At 4 K, we can identify the principal quantum number n = 11 yellow and n = 4 green Rydberg exciton states, beyond which we are limited by the …
We propose a solid state maser based on Cu2O, where ensemble of highly excited Rydberg exciton states serves as a gain medium. We show that the system is highly tunable with external electric field, allowing for a wide range of emission frequencies. Numerical simulations of system dynamics are performed to optimize the conditions for efficient masing and estimate the emission power.
Monolayer WSe$_2$ hosts a series of exciton Rydberg states denoted by the principal quantum number n = 1, 2, 3, etc. While most research focuses on their absorption properties, their optical emission is also important but much less studied. Here we measure the photoluminescence from the 1s - 5s exciton Rydberg states in ultraclean monolayer WSe$_2$ encapsulated by boron nitride under magnetic fields from -31 T to 31 T. The exciton Rydberg states exhibit similar Zeeman shifts but distinct diamagnetic shifts from each other. From their luminescence spectra, Zeeman and diamagnetic shifts, we dedu…
We report exciton-mediated coupling between microwave and optical fields in cuprous oxide (Cu$_2$O) at low temperatures. Rydberg excitonic states with principal quantum number up to $n=12$ were observed at 4~K using both one-photon (absorption) and two-photon (second harmonic generation) spectroscopy. Near resonance with an excitonic state, the addition of a microwave field significantly changed the absorption lineshape, and added sidebands at the microwave frequency to the coherent second harmonic. Both effects showed a complex dependence on $n$ and angular momentum, $l$. All of these feature…
We present theoretically calculated optical functions for Cu$_2$O quantum well (QW) with Rydberg excitons in an external, homogeneous electric field parallel to the QW planes for the energy region above the gap, suitable to observe the Franz-Keldysh (FK) oscillations. We quantitatively describe the amplitudes and periodicity of FK modulations and the influence of both Rydberg excitons and confinement effect on this phenomenon.
We show how to compute the nonlinear optical functions (absorption, reflection, and transmission) for a medium with Rydberg excitons, including the effect of the coherence between the electron-hole pair and the electromagnetic field. Using the Real Density Matrix Approach the analytical expressions for nonlinear optical functions are obtained and numerical calculations for Cu$_2$0 crystal are performed. We report a good agreement with recently published experimental data. Propagation of the electromagnetic waves in Rydberg excitons media with nonliner effect is also discussed and the possibili…
The electronic exciton polaron is a hypothetical many-body quasiparticle formed by an exciton dressed with a polarized electron-hole cloud in the Fermi sea (FS). It is predicted to display rich many-body physics and unusual roton-like dispersion. Exciton polarons were recently evoked to explain the excitonic spectra of doped monolayer transition metal dichalcogenides (TMDs), but these studies are limited to the ground state. Excited-state exciton polarons can exhibit richer many-body physics due to their larger spatial extent, but detection is challenging due to their inherently weak signals. …
We study theoretically Rydberg excitons in one-dimensional chains of traps in Cu$_2$O coupled via the van der Waals interaction. The triplet of optically active $p$-shell states acts as an effective spin-$1$ and the interactions between the excitons are strongly spin-dependent. We predict that the system {has the} topological Haldane phase with the diluted antiferromagnetic order, long-range string correlations, and finite excitation gap. We also analyze the effect of the trap geometry and interactions anisotropy on the Rydberg exciton spin states and demonstrate that a rich spin phase diagram…
We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a nonlinear manner. We explore this mechanism theoretically and determine its effects on the optical properties of a semiconductor for the case of degenerate pair-state asymptotes of Rydberg excitons in…
Rydberg excitons are, with their ultrastrong mutual interactions, giant optical nonlinearities, and very high sensitivity to external fields, promising for applications in quantum sensing and nonlinear optics at the single-photon level. To design quantum applications it is necessary to know how Rydberg excitons and other excited states relax to lower-lying exciton states. Here, we present photoluminescence excitation spectroscopy as a method to probe transition probabilities from various excitonic states in cuprous oxide, and we show giant Rydberg excitons at $T=38$ mK with principal quantum n…
The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and molecular physics [1, 2] to quantum optics [3, 4] and technology [5-7]. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up to a micrometer have indeed been observed in cuprous oxide semiconductors [8]. Here, we demonstrate the generation and control of strong exciton interactions in this material by optically producing two…
Moiré excitons are emergent optical excitations in 2D semiconductors with deep moiré superlattice potentials. While these excitations have been realized in several platforms, a system with dynamically tunable moiré potential to tailor the moiré exciton properties is yet to be realized. Here, we present a continuously tunable moiré potential in a monolayer WSe2 that is enabled by its proximity to twisted bilayer graphene (TBG) near the magic-angle. Due to its flat electronic bands, charge distribution is highly localized and forms a triangular lattice in TBG. Tuning the local charge density via…
We have experimentally determined the energies of the ground and first four excited excitonic states of the fundamental optical transition in monolayer WS2, a model system for the growing class of atomically thin two-dimensional semiconductor crystals. From the spectra, we establish a large exciton binding energy of 0.32 eV and a pronounced deviation from the usual hydrogenic Rydberg series of energy levels of the excitonic states. We explain both of these results using a microscopic theory in which the non-local nature of the effective dielectric screening modifies the functional form of the …
We report 65 tesla magneto-absorption spectroscopy of exciton Rydberg states in the archetypal monolayer semiconductor WSe$_2$. The strongly field-dependent and distinct energy shifts of the 2s, 3s, and 4s excited neutral excitons permits their unambiguous identification and allows for quantitative comparison with leading theoretical models. Both the sizes (via low-field diamagnetic shifts) and the energies of the $ns$ exciton states agree remarkably well with detailed numerical simulations using the non-hydrogenic screened Keldysh potential for 2D semiconductors. Moreover, at the highest magn…
The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principle value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, for the fir…
The quantum confiment of Rydberg excitons (REs) in quantum structures opens the way towards considering nonlinear interactions in such systems. We present a theoretical calculation of optical functions in the case of a nonlinear coupling between REs in a quantum well with an electromagnetic wave. Using the Real Density Matrix Approach (RDMA), the analytical expressions for a linear and nonlinear absorption are derived and numerical calculations for Cu$_2$0 quantum wells are performed. The results indicate the conditions in which quantum well confinement states can be observed in linear and non…
Monolayer transition metal dichalcogenide (TMDC) semiconductors exhibit strong excitonic optical resonances which serve as a microscopic, non-invasive probe into their fundamental properties. Like the hydrogen atom, such excitons can exhibit an entire Rydberg series of resonances. Excitons have been extensively studied in most TMDCs (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$), but detailed exploration of excitonic phenomena has been lacking in the important TMDC material molybdenum ditelluride (MoTe$_2$). Here, we report an experimental investigation of excitonic luminescence properties of monolay…
In this study we analyze the transmission spectrum of a thin plate of Cuprous Oxide in the range of the absorption of the yellow exciton states with the coherent transfer matrix method. We demonstrate that, in contrast to the usual analysis using Beer's law, which turns out to be a rather good approximation only in the spectral region of high principal quantum numbers, a consistent quantitative description over the whole spectral range under consideration is possible. This leads to new and more accurate parameters not only for the Rydberg exciton states, but also for the strengths of indirect …
The results of magneto-optical spectroscopy investigations of excitons in a CVD grown monolayer of WSe2 encapsulated in hexagonal boron nitride are presented. The emission linewidth for the 1s state is of 4:7 meV, close to the narrowest emissions observed in monolayers exfoliated from bulk material. The 2s excitonic state is also observed at higher energies in the photoluminescence spectrum. Magneto-optical spectroscopy allows for the determination of the g-factors and of the spatial extent of the excitonic wave functions associated with these emissions. Our work establishes CVD grown monolaye…
Highly excited atoms with an electron moved into a level with large principal quantum number are fascinating hydrogen-like objects. The giant extension of these Rydberg atoms leads to huge interaction effects. Monitoring these interactions has provided novel insights into molecular and condensed matter physics problems on a single quantum level. Excitons, the fundamental optical excitations in semiconductors consisting of a negatively charged electron and a positively charged hole, are the condensed matter analogues of hydrogen. Highly excited excitons with extensions similar to Rydberg atoms …
Experimental and theoretical investigations of excitons in cuprous oxide have revealed a significant fine-structure splitting of the excitonic Rydberg states caused by a strong impact of the valence band structure. We provide a semiclassical interpretation of that splitting by investigating the classical dynamics of the excitonic electron-hole pair beyond the hydrogen-like model. Considering the slow motion of Rydberg excitons in coordinate space compared to the fast dynamics of quasispin and hole spin we use an adiabatic approach and energy surfaces in momentum space for the computation of th…
