arXiv subjects

Chris Sturm

Publications and source records attributed to Chris Sturm.

13 recordsLinked to original sources

arXiv2023

Determination of acoustic phonon anharmonicities via second-order Raman scattering in CuI

We demonstrate the determination of anharmonic acoustic phonon properties via second-order Raman scattering exemplarily on copper iodide single crystals. The origin of multi-phonon features from the second-order Raman spectra was assigned by the support of the calculated 2-phonon density of states. In this way, the temperature dependence of acoustic phonons was determined down to 10\,K. To determine independently the harmonic contributions of respective acoustic phonons, density functional theory (DFT) in quasi-harmonic approximation was used. Finally, the anharmonic contributions were determined. The results are in agreement with earlier publications and extend CuI's determined acoustic phonon properties to lower temperatures with higher accuracy. This approach demonstrates that it is possible to characterize the acoustic anharmonicities via Raman scattering down to zero-temperature renormalization constants of at least 0.1\,cm$^{-1}$.

cond-mat.mtrl-sci↗

arXiv2023

The anisotropic Beer-Lambert law in $\beta$-Ga$_{2}$O$_{3}$: Spectral and polarization dependent absorption and photoresponsivity

Due to its low symmetry, $\beta$-Ga$_{2}$O$_{3}$ exhibits a strongly anisotropic optical response. As a result, the absorption spectra change with the polarization state of the incoming photons. To understand this phenomenon, here we calculate the complete electromagnetic wave equation solutions as a function of linear polarization angle and photon energy for $\beta$-Ga$_{2}$O$_{3}$ using its previously measured complex dielectric function tensor. The significant off-diagonal terms in this tensor can result in a non-exponential decay in the photon flux, indicating that the Beer-Lambert law is not generally valid in this anisotropic material. However, for above-band-gap spectral regions which depend on crystallographic orientations (> 5.8 eV (001 plane),>5.2 eV (010 plane)) an effective absorption coefficient well approximates the photon flux decay with depth. On the other hand, near the optical absorption edge (4.9 - 5.8 eV (001 plane),4.65 - 5.2 eV (010 plane)) the photon flux decay exhibits a sum of two exponential decays, such that two effective absorption coefficients are necessary to model the loss behavior versus the absorption depth. This behavior manifests from the presence of dichroism in $\beta$-Ga$_{2}$O$_{3}$. A single effective absorption coefficient can only be recovered for this energy range by augmenting the isotropic Beer-Lambert law with a critical penetration depth and polarization dependence. Using these results, we calculate the polarization-dependent photoresponsivity spectra for light polarized along different crystallographic directions.

cond-mat.mtrl-sci↗

arXiv2023

Anisotropic excitonic photocurrent in $β$-Ga$_{2}$O$_{3}$

Polarization dependent photocurrent spectra are measured on a (001) $β$-Ga$_{2}$O$_{3}$ Schottky photodetector, where the linear polarization of light is rotated within the ab plane. Three spectral peaks at 4.92 eV, 5.15 eV, and 5.44 eV are observed that vary in intensity with the optical polarization direction. The peak transition energies are consistent with excitons previously reported in $β$-Ga$_{2}$O$_{3}$ due to interband transitions modified by the valence band p-orbital anisotropy and the electron-hole Coulombic attraction. The measured polarization-dependence of the photocurrent matches our predictions based on electromagnetic simulations of anisotropic absorption using the complex dielectric function tensor extracted from previous ellipsometry studies. These results illustrate the dominance of excitonic absorption and photocurrent in $β$-Ga$_{2}$O$_{3}$ both below and above the band gap, demonstrate a combined theoretical/experimental understanding of anisotropic photocarrier generation, and validate previous atomistic band structure calculations in this low-symmetry ultra-wide band gap semiconductor.

cond-mat.mtrl-sci↗

arXiv2022

Dielectric function of CuBr$_\mathrm{x}$I$_{1-\mathrm{x}}$ alloy thin films

We study the dielectric function of CuBr$_\mathrm{x}$I$_{1-\mathrm{x}}$ thin film alloys using spectroscopic ellipsometry in the spectral range between 0.7 eV to 6.4 eV, in combination with first-principles calculations based on density functional theory. Through the comparison of theory and experiment, we attribute features in the dielectric function to electronic transitions at specific k-points in the Brillouin zone. The observed bandgap bowing as a function of alloy composition is discussed in terms of different physical and chemical contributions. The band splitting at the top of the valence band due to spin-orbit coupling is found to decrease with increasing Br-concentration, from a value of 660 meV for CuI to 150 meV for CuBr. This result can be understood considering the contribution of copper d-orbitals to the valence band maximum as a function of the alloy composition.

cond-mat.mtrl-sci↗

arXiv2019

Control of Magnetic Order in Spinel ZnFe$_2$O$_4$ Thin Films Through Intrinsic Defect Manipulation

We present a systematic study of the magnetic properties of semiconducting ZnFe$_2$O$_4$ thin films fabricated by pulsed laser deposition at low and high oxygen partial pressure and annealed in oxygen and argon atmosphere, respectively. The magnetic response is enhanced by annealing the films at 250$^{\circ}$C and diminished at annealing temperatures above 300$^{\circ}$C. The initial increase is attributed to the formation of oxygen vacancies after argon treatment, evident by the increase in the low energy absorption at $\sim$ 0.9 eV involving Fe$^{2+}$ cations. The weakened magnetic response is related to a decline in disorder with a cation redistribution toward a normal spinel configuration. The structural renormalization is consistent with the decrease and increase in oscillator strength of respective electronic transitions involving tetrahedrally (at $\sim$ 3.5 eV) and octahedrally (at $\sim$ 5.7 eV) coordinated Fe$^{3+}$ cations.

physics.app-ph↗

arXiv2016

Exceptional points in anisotropic planar microcavities

Planar microcavities allow the control and manipulation of spin-polarization, manifested in phenomena like the optical spin Hall effect due to the intrinsic polarization mode splitting. Here, we study a transparent microcavity with broken rotational symmetry, realized by aligning the optical axis of a uniaxial cavity material in the cavity plane. We demonstrate that the in-plane optical anisotropy gives rise to exceptional points in the dispersion relation, which occur pair-wise, are circularly polarized, and are cores of polarization vortices. These exceptional points are a result of the non-Hermitian character of the system, and are in close relationship to singular optical axes in absorptive biaxial systems.

physics.optics↗

arXiv2016

Raman tensor elements of $β\text{-Ga}_2\text{O}_3$

The Raman spectrum and particularly the Raman scattering intensities of monoclinic $β\text{-Ga}_2\text{O}_3$ are investigated by experiment and theory. The low symmetry of $β\text{-Ga}_2\text{O}_3$ results in a complex dependence of the Raman intensity for the individual phonon modes on the scattering geometry which is additionally affected by birefringence. We measured the Raman spectra in dependence on the polarization direction for backscattering on three crystallographic planes of $β\text{-Ga}_2\text{O}_3$ and modeled these dependencies using a modified Raman tensor formalism which takes birefringence into account. The spectral position of all 15 Raman-active phonon modes and the Raman tensor elements of 13 modes were determined and are compared to results from ab-initio calculations.

cond-mat.mtrl-sci↗

arXiv2016

Dipole Analysis of the Dielectric Function of Colour Dispersive Materials: Application to Monoclinic Ga$_2$O$_3$

We apply a generalized model for the determination and analysis of the dielectric function of optically anisotropic materials with colour dispersion to phonon modes and show that it can also be generalized to excitonic polarizabilities and electronic band-band transitions. We take into account that the tensor components of the dielectric function within the cartesian coordinate system are not independent from each other but are rather projections of the polarization of dipoles oscillating along directions defined by the, non-cartesian, crystal symmetry and polarizability. The dielectric function is then composed of a series of oscillators pointing in different directions. The application of this model is exemplarily demonstrated for monoclinic ($β$-phase) Ga$_2$O$_3$ bulk single crystals. Using this model, we are able to relate electronic transitions observed in the dielectric function to atomic bond directions and orbitals in the real space crystal structure. For thin films revealing rotational domains we show that the optical biaxiality is reduced to uniaxial optical response.

cond-mat.mtrl-sci↗

arXiv2016

Carrier density driven lasing dynamics in ZnO nanowires

We report on the temporal lasing dynamics of high quality ZnO nanowires using time-resolved micro-photoluminescence technique. The temperature dependence of the lasing characteristics and of the corresponding decay constants demonstrate the formation of an electron-hole plasma to be the underlying gain mechanism in the considered temperature range from 10 K to 300 K. We found that the temperature dependent emission onset-time ($t_{\text{on}}$) strongly depends on the excitation power and becomes smallest in the lasing regime, with values below 5 ps. Furthermore, the observed red shift of the dominating lasing modes in time is qualitatively discussed in terms of the carrier density induced change of the refractive index dispersion after the excitation laser pulse. This theory is supported by extending an existing model for the calculation of the carrier density dependent complex refractive index for different temperatures. This model coincides with the experimental observations and reliably describes the evolution of the refractive index after the excitation laser pulse.

physics.optics↗

arXiv2016

The Singular Optical Axes in Biaxial Crystals and Analysis of Their Spectral Dispersion Effects in $β$-Ga$_2$O$_3$

We classify and distinguish optically biaxial materials, which can have triclinic, monoclinic or orthorhombic crystal symmetry, by the degeneracy of the indices of refraction of their four singular optical axes (Windungsachsen) in the absorption regime. We provide explicit analytical solutions for angular orientations of the singular optical axes in monoclinic crystals and orthorhombic crystals. As a model material we analyze monoclinic gallia ($β$-Ga$_2$O$_3$) and discuss in detail the dispersion (i.e. the spectral variation of the angular position) of its singular optical axes. For a certain energy range ($E \approx 7.23$-$7.33$ eV) we find quasi-uniaxial symmetry. At two energies ($E \approx 8.14$ eV and $E \approx 8.37$ eV) we find triaxial spectral points for which one regular optical axis and two singular optical axes exist. Concurrently a Stokes analysis of the spectral dependence of the electrical field eigenvectors is made and discussed for various crystal orientations. For a singular optical axis $|S_3|=1$; for the two degenerate singular axes at the triaxial point the Stokes vector is undefined. For a certain energy ($E=6.59$ eV), the $\langle 010 \rangle$-orientation is close to a singular optical axis, $|S_3|=0.977$. The analysis provided here is prototypical for the treatment of the optical properties of optically biaxial functional materials in the absorption and gain regimes.

cond-mat.mtrl-sci↗

arXiv2015

Cavity Polariton Condensate in a Disordered Environment

We report on the influence of disorder on an exciton-polariton condensate in a ZnO based bulk planar microcavity and compare experimental results with a theoretical model for a non-equilibrium condensate. Experimentally, we detect intensity fluctuations within the far-field emission pattern even at high condensate densities which indicates a significant impact of disorder. We show that these effects rely on the driven dissipative nature of the condensate and argue that they can be accounted for by spatial phase inhomogeneities induced by disorder, which occur even for increasing condensate densities realized in the regime of high excitation power. Thus, non-equilibrium effects strongly suppress the stabilization of the condensate against disorder, contrarily to what is expected for equilibrium condensates in the high density limit. Numerical simulations based on our theoretical model reproduce the experimental data.

cond-mat.mes-hall↗

arXiv2015

Dielectric tensor of monoclinic Ga$_2$O$_3$ single crystals in the spectral range $0.5 - 8.5\,$eV

The dielectric tensor of $β$-Ga$_2$O$_3$ was determined by generalized spectroscopic ellipsometry in a wide spectral range from $0.5\,\mathrm{eV}$ to $8.5\,\mathrm{eV}$ as well as by calculation including quasiparticle bands and excitonic effects. The dielectric tensors obtained by both methods are in excellent agreement with each other and the observed transitions in the dielectric function are assigned to the corresponding valence bands. It is shown that the off-diagonal element of the dielectric tensor reaches values up to $|\varepsilon_{xz} | \approx 0.30 $ and cannot be neglected. Even in the transparent spectral range where it is quite small ($|\varepsilon_{xz} | < 0.02 $) it causes a rotation of the dielectric axes around the symmetry axis of up to $20^\circ$.

cond-mat.mtrl-sci↗

arXiv2013

Realization of a double barrier resonant tunneling diode for cavity polaritons

We report on the realization of a double barrier resonant tunneling diode for cavity polaritons, by lateral patterning of a one-dimensional cavity. Sharp transmission resonances are demonstrated when sending a polariton flow onto the device. We use a non-resonant beam can be used as an optical gate and control the device transmission. Finally we evidence distortion of the transmission profile when going to the high density regime, signature of polariton-polariton interactions.

cond-mat.mes-hall↗