arXiv subjects

D. Fröhlich

Publications and source records attributed to D. Fröhlich.

7 recordsLinked to original sources

arXiv2025

Coherence of dipole-forbidden Rydberg excitons in Cu$_2$O measured by polarization- and time-resolved multi-photon spectroscopy

Quantum applications of solid state systems base upon generation and control of coherent electronic excitations. Prominent examples are exciton states in semiconductors excitable by photons. The high oscillator strength of electric-dipole (ED) allowed exciton states favors their efficient coherent generation, but limits also their lifetime. ED-forbidden exciton states with long recombination times might maintain long-lived coherence, especially in highly-quality crystals with suppressed exciton scattering. Here, we propose a multi-photon technique combining two-photon excitation with difference frequency generation (2PE-DFG) for time-resolved measurements of exciton coherence. The technique utilizes polarization tomography for state-selective control in both the pump and probe processes. Its potential is demonstrated by measuring the coherent dynamics of the ED-forbidden $S$ and $D$ excitons in Cu$_2$O crystals. The excited states of the Rydberg excitons with principal quantum number $n=2$, $3$, and $4$ have short dephasing times of a few picoseconds, limited by their relaxation to lower lying states. The dephasing time reaches 3 ns for the $1S$ state. In an external magnetic field up to 10 T, the $1S$ exciton splits into a triplet so that quantum beats are observed after coherent excitation, for which three distinct regimes are found depending on the chosen polarization tomography scheme. These results establish the 2PE-DFG technique as a powerful tool to assess the coherent dynamics of ED-forbidden excitons.

cond-mat.mtrl-sci↗

arXiv2020

Magneto-Stark and Zeeman effect as origin of second harmonic generation of excitons in Cu$_2$O

We report on the experimental and theoretical investigation of magnetic-field-induced second harmonic generation (SHG) and two-photon absorption (TPA) of excited exciton states ($n \geq 3$) of the yellow series in Cu$_2$O. In this centrosymmetric material, SHG can occur due to constructive interplay of electric dipole and electric quadrupole/magnetic dipole transitions for light propagating along the low-symmetry directions [111] or [112]. By application of a magnetic field in Voigt configuration, SHG gets also allowed for excitation along the [110]-axis and even the high-symmetry cubic direction [001]. Combining a symmetry analysis and a microscopic theory, we uncover the two key contributions to the magnetic-field-induced SHG: the Zeeman effect and the magneto-Stark effect. We demonstrate systematic dependencies of the SHG intensity on the linear polarization angles of the ingoing fundamental laser and the outgoing SHG beam. In general, the resulting contour plots in combination with a symmetry analysis allow one to determine uniquely the character of involved transitions. Moreover, we can separate in magnetic field the Zeeman and the magneto-Stark effect through appropriate choice of the experimental geometry and polarization configuration. We present a microscopic theory of the second harmonic generation of excitons in a centrosymmetric cubic semiconductor taking into account the symmetry and the band structure of cuprous oxide. Based on the developed microscopic theory we identify the main contributions to the second-order nonlinear susceptibility of $S$-, $P$- and $D$-excitons. We analyze the redistribution of SHG intensities between the excitonic states both in the absence and presence of the magnetic field and show good agreement with the experimental data. With increasing exciton principal quantum number the magneto-Stark effect overpowers the influence of the Zeeman effect.

cond-mat.mes-hall↗

arXiv2017

Rydberg excitons in the presence of an ultralow-density electron-hole plasma

We use two-color pump-probe spectroscopy to study Rydberg excitons in Cu$_2$O in the presence of free carriers injected by above-band-gap excitation. Already at plasma densities $ρ_\text{eh}$ below one hundredth electron-hole pair per \textmu m$^{3}$, the Rydberg exciton absorption lines are bleached while their energies remain constant, until they finally disappear, starting from the highest observed principal quantum number $n_\text{max}$. As confirmed by calculations, the band gap is reduced by many-particle effects caused by free carriers scaling as $ρ_\text{eh}^{1/2}$. An exciton line looses oscillator strength when the band edge approaches the exciton energy vanishing completely at the crossing point. We quantitatively describe this plasma blockade by introducing an effective Bohr radius that determines the energy distance to the shifted band edge. In combination with the negligible associated decoherence this opens the possibility to control the Rydberg exciton absorption through the plasma-induced band gap modulation.

cond-mat.mtrl-sci↗

arXiv2017

Scaling laws of Rydberg excitons

Rydberg atoms have attracted considerable interest due to their huge interaction among each other and with external fields. They demonstrate characteristic scaling laws in dependence on the principal quantum number $n$ for features such as the magnetic field for level crossing. While bearing striking similarities to Rydberg atoms, fundamentally new insights may be obtained for Rydberg excitons, as the crystal environment gives easy optical access to many states within an exciton multiplet. Here we study experimentally and theoretically the scaling of several characteristic parameters of Rydberg excitons with $n$. From absorption spectra in magnetic field we find for the first crossing of levels with adjacent principal quantum numbers a $B_r \propto n^{-4}$ dependence of the resonance field strength, $B_r$, due to the dominant paramagnetic term unlike in the atomic case where the diamagnetic contribution is decisive. By contrast, in electric field we find scaling laws just like for Rydberg atoms. The resonance electric field strength scales as $E_r \propto n^{-5}$. We observe anticrossings of the states belonging to multiplets with different principal quantum numbers. The energy splittings at the avoided crossings scale as $n^{-4}$ which we relate to the crystal specific deviation of the exciton Hamiltonian from the hydrogen model. We observe the exciton polarizability in the electric field to scale as $n^7$. In magnetic field the crossover field strength from a hydrogen-like exciton to a magnetoexciton dominated by electron and hole Landau level quantization scales as $n^{-3}$. The ionization voltages demonstrate a $n^{-4}$ scaling as for atoms. The width of the absorption lines remains constant before dissociation for high enough $n$, while for small $n \lesssim 12$ an exponential increase with the field is found. These results are in excellent agreement with theoretical calculations.

cond-mat.mtrl-sci↗

arXiv2017

High resolution study of the yellow excitons in Cu$_2$O subject to an electric field

We have used high resolution transmission spectroscopy to study the exciton level spectrum in Cu$_2$O subject to a longitudinal external electric field, i.e., in the geometry where the transmitted light is propagating along the field direction. Different experimental configurations given by the field orientation relative to the crystal and the light polarization have been explored. We focus on the range of small principal quantum numbers $n \leq 7$. The number of exciton states belonging to a particular principal quantum number increases with $n$, leading to an enhanced complexity of the spectra. Still, in particular for $n = 3 \ldots 5$ a spectral separation of the different lines is feasible and identification as well as assignment of the dominant state character are possible. We find a strong dependence of the spectra on the chosen light propagation direction and polarization configuration, reflecting the inadequacy of the hydrogen model for describing the excitons. With increasing the field excitonic states with different parity become mixed, leading to optical activation of states that are dark in zero field. As compared with atoms, due to the reduced Rydberg energy states with different $n$ can be brought into resonance in the accessible electric field strength range. When this occurs, we observe mostly crossing of levels within the experimental accuracy showing that the electron and hole motion remains regular. The observed features are well described by detailed calculations accounting for the spin-orbit coupling, the cubic anisotropy effects, and the symmetry-imposed optical selection rules.

cond-mat.mtrl-sci↗

arXiv2016

Signatures of Quantum Coherence in Rydberg Excitons

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 three-level system, but driven only by one laser light source. We show that the level of pure dephasing in this system is extremely low. These observations are a crucial step towards coherently controlled quantum technologies in a bulk semiconductor.

cond-mat.mes-hall↗

arXiv2015

Observation of high angular momentum excitons in cuprous oxide

The recent observation of dipole-allowed $P$-excitons up to principal quantum numbers of $n=25$ in cuprous oxide has given insight into exciton states with unprecedented spectral resolution. While so far the exciton description as a hydrogen-like complex has been sufficient for cubic crystals, we demonstrate here distinct deviations: The breaking of rotational symmetry leads to mixing of high angular momentum $F$- and $H$-excitons with the $P$-excitons so that they can be observed in absorption. The $F$-excitons show a three-fold splitting that depends systematically on $n$, in agreement with theoretical considerations. From detailed comparison of experiment and theory we determine the cubic anisotropy parameter of the Cu$_2$O valence band.

cond-mat.mtrl-sci↗