-
Alloying Controlled Tuning of Interfacial Spin Orbit Interaction and Magnetic Damping in Crystalline FeCo Alloys
Authors:
Hongrui Lao,
Matthias Kronseder,
Zhe Yuan,
Thomas Narr,
Thomas N. G. Meier,
Nadine Mundigl,
Christian H. Back,
Lin Chen
Abstract:
The discovery of intrinsic spin orbit fields in noncentrosymmetric ferromagnets has attracted considerable interest for both fundamental studies and technological applications. However, once such materials are synthesized, the strength of the spin orbit fields is difficult to tune because it is primarily a bulk property. Here, we demonstrate that the interfacial spin orbit interaction (SOI) in sin…
▽ More
The discovery of intrinsic spin orbit fields in noncentrosymmetric ferromagnets has attracted considerable interest for both fundamental studies and technological applications. However, once such materials are synthesized, the strength of the spin orbit fields is difficult to tune because it is primarily a bulk property. Here, we demonstrate that the interfacial spin orbit interaction (SOI) in single crystalline FeCo thin films grown on GaAs(001) can be continuously tuned via alloying. Using spin orbit ferromagnetic resonance, we find that the Lande g factor, the Gilbert damping (alpha), and the interfacial spin orbit fields exhibit a common nonmonotonic dependence on Co concentration. A pronounced minimum occurs near x ~ 0.2 where an ultra low damping alpha ~ 0.0015 is achieved. Furthermore, we observe linear scaling between alpha and (g-2)^2, establishing a direct correlation between interfacial SOI and magnetic relaxation. These results identify alloying as an effective knob to engineer interfacial SOI and damping in single crystalline ferromagnet semiconductor heterostructures.
△ Less
Submitted 28 March, 2026;
originally announced March 2026.
-
Current-tunable room temperature ferromagnetism and current-driven phase transitions
Authors:
Jianping Guo,
Peng Rao,
Xinhao Huang,
Tailai Xu,
Yuxuan Guo,
Jian Shao,
Cheng Sun,
Anton Orekhov,
Thomas N. G. Meier,
Johannes Knolle,
Christian H. Back,
Lin Chen
Abstract:
It is generally assumed that the application of a charge-current in ferromagnetic metals suppresses their ferromagnetic order through trivial Joule heating. Here, we demonstrate that a charge current can instead enhance magnetic ordering. Using a WTe2/Fe3Ge2Te (FGT) stack as a model system, we show that a charge current flowing in WTe2 controls the ferromagnetic properties and magnetic phase trans…
▽ More
It is generally assumed that the application of a charge-current in ferromagnetic metals suppresses their ferromagnetic order through trivial Joule heating. Here, we demonstrate that a charge current can instead enhance magnetic ordering. Using a WTe2/Fe3Ge2Te (FGT) stack as a model system, we show that a charge current flowing in WTe2 controls the ferromagnetic properties and magnetic phase transition of the adjacent FGT via a current-induced effective magnetic-field arising from orbital magnetization. Remarkably, the charge current drives a substantial enhancement of the Curie temperature, boosting it well above room temperature. Furthermore, we show that the charge-current enables controlled tuning of the phase transitions in FGT, which confirms the scaling behaviour of a ferromagnet-paramagnet phase transition. This work provides a pathway for integrating two-dimensional ferromagnets into spintronic functionalities at technologically relevant temperatures and for exploring novel current-driven phenomena in ferromagnetic systems.
△ Less
Submitted 28 March, 2026;
originally announced March 2026.
-
Assessing the classicality of photon echo from excitons in lead halide perovskite nanocrystals
Authors:
George Alkhalil,
Hendrik Rose,
Artur V. Trifonov,
Polina R. Sharapova,
Jan Sperling,
Dmitri R. Yakovlev,
Elena V. Kolobkova,
Maria S. Kuznetsova,
Marc Aßmann,
Manfred Bayer,
Torsten Meier,
Ilya A. Akimov
Abstract:
Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the…
▽ More
Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the photon statistics of PE signals generated by excitons in ensembles of lead halide perovskite CsPbI$_3$ nanocrystals at cryogenic temperature of 2 K using continuous-variable quantum state optical tomography based on homodyne detection. Pronounced Rabi oscillations of the PE amplitude allow us to evaluate the statistics for various pulse areas in the excitation sequence. The damping of the oscillations with increasing pulse area is attributed to spatial excitation inhomogeneity and excitation-induced dephasing. Despite the large ensemble of optically addressed excitons, the efficiency of generated PE signals is low which is attributed to the complex energy level structure of excitons and non-radiative recombination channels in CsPbI$_3$ nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function $g^{(2)}(0)$ and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that $g^{(2)}(0) = 1$, and the characteristic function of the PE signal corresponds to classical behavior. The formation of photon echoes as well as $g^{(2)}(0) = 1$ at the echo time is reproduced by a quantized free-space multimode model. Despite the relatively low efficiency, the photon echo exhibits a high degree of coherence and minimal classical noise, consistent with Poissonian statistics.
△ Less
Submitted 26 May, 2026; v1 submitted 26 March, 2026;
originally announced March 2026.
-
Pressure-driven vibrational and structural peculiarities in the honeycomb layered magnetoelectrics Mn4(B)2O9 (B= Nb, Ta)
Authors:
Rajesh Jana,
Afsal S Shajahan,
Boby Joseph,
Brahmananda Chakraborty,
Irshad K A,
Anuj Upadhyay,
Alka Garg,
Rekha Rao,
Thomas Meier
Abstract:
The high-pressure behavior of two Mn-based honeycomb-structured magnetoelectric materials, Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO), was investigated using Raman spectroscopy, synchrotron x-ray diffraction, and density functional theory (DFT) calculations. In MTO, the application of a small pressure of only 0.5 GPa induces an isostructural transition driven by local symmetry breaking. With further increa…
▽ More
The high-pressure behavior of two Mn-based honeycomb-structured magnetoelectric materials, Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO), was investigated using Raman spectroscopy, synchrotron x-ray diffraction, and density functional theory (DFT) calculations. In MTO, the application of a small pressure of only 0.5 GPa induces an isostructural transition driven by local symmetry breaking. With further increase in pressure, three additional isostructural transitions are observed at about 3.2, 6, and 10 GPa, followed by the onset of a long-range structural transition near 14 GPa, where the ambient P-3c1 phase begins to transform into a P2/c phase. These two phases coexist up to 27 GPa. The Nb analogue, MNO, also exhibits similar isostructural transitions at about 2, 6.6, and 10 GPa. However, the onset of the mixed P2/c and P-3c1 phases occurs at a slightly lower pressure of 12.5 GPa, with phase coexistence extending up to 26.5 GPa. These long-range transitions are supported by pressure-dependent enthalpy changes obtained from DFT calculations. Rietveld refinement reveals pronounced anisotropic lattice compression, with a 42 to 49 percent difference between the c and a axes, leading to a notable reduction in the c/a ratio. This anisotropy may strengthen interlayer coupling and promote magnetic ordering under compression, consistent with the appearance of Raman modes similar to those reported at low temperatures, together with anomalous changes in Raman mode linewidth and intensity. The marked changes in Raman self-energy parameters, anomalies in the reduced pressure-Eulerian strain profile, and the onset of local symmetry breaking at much lower pressures in MTO than in MNO highlight the important role of differences in spin-orbit coupling strength and orbital hybridization associated with Nb5+ and Ta5+ cations.
△ Less
Submitted 17 March, 2026;
originally announced March 2026.
-
Pressure-induced lattice instabilities and phonon softening in the orthorhombically distorted ferrimagnet Ni4Nb2O9
Authors:
Rajesh Jana,
Xinyu Wang,
Takeshi Nakagawa,
Hirofumi Ishii,
Alka Garg,
Rekha Rao,
Thomas Meier
Abstract:
The ambient- and high-pressure behavior of the ferrimagnet Ni4Nb2O9 (orthorhombically distorted honeycomb structure), is investigated using NMR, Raman spectroscopy, and synchrotron XRD. Ambient-pressure NMR measurements reveal, despite its orthorhombic symmetry, the local environment of Ni4Nb2O9 closely resembles that of its trigonal analogue Mn4Nb2O9. In contrast, substantially different paramagn…
▽ More
The ambient- and high-pressure behavior of the ferrimagnet Ni4Nb2O9 (orthorhombically distorted honeycomb structure), is investigated using NMR, Raman spectroscopy, and synchrotron XRD. Ambient-pressure NMR measurements reveal, despite its orthorhombic symmetry, the local environment of Ni4Nb2O9 closely resembles that of its trigonal analogue Mn4Nb2O9. In contrast, substantially different paramagnetic shifts observed in the two compounds reflect their distinct average crystal symmetries, governing orbital overlap and magnetic exchange pathways. Under external pressure, Ni4Nb2O9 exhibits pronounced sensitivity to lattice distortions and phonon instabilities. Three isostructural transitions are identified near 2, 6, and 10 GPa, manifested by mode splitting, frequency shifts, line broadenings, intensity anomalies, and slope changes in the evolution of lattice parameters. At higher pressure, around 13 GPa, signatures of an incipient long-range structural transition from orthorhombic Pbcn to monoclinic P2/c symmetry emerge, signaling the onset of a symmetry-lowering transformation. The anomalous softening of the 192 cm^-1 Raman mode, accompanied by multiple linewidth and spectral-weight anomalies, serve as a key fingerprint of these structural instabilities, linking local symmetry breaking at low pressures to the long-range transition into the P2/c phase. Notably, pronounced linewidth anomalies, strongly anisotropic pressure coefficients, together with a marked enhancement of the intensity of the low-frequency branch over the 2-13 GPa range, point toward a pressure-induced regime influenced by coupled spin, orbital, and lattice degrees of freedom. The close correspondence of transition pressures in Ni4Nb2O9 and those reported for Mn4Nb2O9 highlights a common mechanism rooted in their similar local structural environments, as revealed by NMR.
△ Less
Submitted 2 March, 2026;
originally announced March 2026.
-
Observation of robust spin-phonon coupling and indication of hidden structural transition in the spin-driven ferroelectrics Mn4B_2O_9 (B= Nb, Ta)
Authors:
Rajesh Jana,
Alka Garg,
Rekha Rao,
Thomas Meier
Abstract:
We report detailed Raman spectroscopic and magnetic susceptibility studies on the spin-driven ferroelectric compounds Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO). Both systems exhibit strong spin-phonon coupling below the short-range magnetic ordering temperature (T(sro)=223 K), followed by further renormalization of several Raman modes at the long-range magnetic ordering temperatures (TN = 120 K for MNO an…
▽ More
We report detailed Raman spectroscopic and magnetic susceptibility studies on the spin-driven ferroelectric compounds Mn4Nb2O9 (MNO) and Mn4Ta2O9 (MTO). Both systems exhibit strong spin-phonon coupling below the short-range magnetic ordering temperature (T(sro)=223 K), followed by further renormalization of several Raman modes at the long-range magnetic ordering temperatures (TN = 120 K for MNO and 110 K for MTO). Pronounced anomalies in Raman mode frequencies and linewidths, along with the emergence of octahedral modes between Tsro and TN, indicate a possible low-symmetry structural transition, more evident in MNO and closely linked to magnetic ordering in MTO. Distinct low-temperature evolutions of Raman mode shift, linewidth, and integrated intensity in MNO and MTO highlight the role of the nonmagnetic B-site cation in tuning spin-lattice coupling, driven by differences in spin-orbit coupling and orbital hybridization between Nb5+ (4d) and Ta5+ (5d). By combining Raman spectroscopy with nuclear magnetic resonance, and diffuse reflectance spectroscopy, we further show that Mn-based systems possess a more distorted local structure than their Co analogues, while their electronic structures differ despite comparable band gaps. These results provide a comprehensive understanding of spin-lattice coupling in Mn- and Co-based A4B2O9 magnetoelectric systems.
△ Less
Submitted 5 February, 2026;
originally announced February 2026.
-
Microscopic simulations of the coupled dynamics of cavity photons, excitons, and biexcitons
Authors:
Hendrik Rose,
Stefan Schumacher,
Torsten Meier
Abstract:
The coherent interaction between quantum light and material excitations in semiconductor nanostructures is investigated using a fully quantized microscopic approach that incorporates many-body Coulomb correlations. The simulations demonstrate that the quantum dynamics is influenced by biexciton continuum states and is highly sensitive to both the frequency of the cavity mode and the strength of th…
▽ More
The coherent interaction between quantum light and material excitations in semiconductor nanostructures is investigated using a fully quantized microscopic approach that incorporates many-body Coulomb correlations. The simulations demonstrate that the quantum dynamics is influenced by biexciton continuum states and is highly sensitive to both the frequency of the cavity mode and the strength of the light-matter coupling.
△ Less
Submitted 2 February, 2026;
originally announced February 2026.
-
Electric-current control of anomalous Hall effect
Authors:
Jianping Guo,
Gusthavo M. S. Brizolla,
Peng Rao,
Jian Shao,
Thomas N. G. Meier,
Tailai Xu,
Peirui Ji,
Jonathan Finley,
Jaroslav Fabian,
Johannes Knolle,
Christian Back,
Lin Chen
Abstract:
We demonstrate robust and reversible electric-current control of the anomalous Hall effect (AHE) in a two-dimensional WTe2/Fe3GeTe2 (FGT) stack. Applying a current through Td-WTe2 leads to a giant modulation of the AHE of the adjacent FGT layer, with the relative change of the AHE conductivity exceeding 180%. Control experiments show that i) the observed effect is absent in pure FGT, ii) the modul…
▽ More
We demonstrate robust and reversible electric-current control of the anomalous Hall effect (AHE) in a two-dimensional WTe2/Fe3GeTe2 (FGT) stack. Applying a current through Td-WTe2 leads to a giant modulation of the AHE of the adjacent FGT layer, with the relative change of the AHE conductivity exceeding 180%. Control experiments show that i) the observed effect is absent in pure FGT, ii) the modulation weakens in thicker FGT films, confirming its interfacial origin, and iii) the modulation peaks for bilayer WTe2, indicating that the Berry-curvature dipole (BCD) plays the dominant role in the modulation. We propose that the charge current I generates an out-of-plane magnetization Mz via BCD in WTe2 and Mz modifies the exchange splitting of FGT via the inverse magnetic proximity effect, thereby altering its Berry curvature and nontrivially influencing the AHE. The demonstrated method of AHE control offers new possibilities for magnetism control, i.e., for the study of AHE-transistors as well as electric-current control of quantum magnets, especially magnetic insulators.
△ Less
Submitted 7 January, 2026;
originally announced January 2026.
-
muT2-NMR: Micro-Scale Correlation Relaxometry for in-situ High-Pressure Nuclear Magnetic Resonance
Authors:
Thomas Meier,
Meng Yang,
Yishan Zhou,
Yunhua Fu,
Rui Zhang,
Ziliang Wang,
Tianyao Zheng,
Rajesh Jana,
Takeshi Nakagawa
Abstract:
Over the last decade, frequency-domain in-situ high-pressure nuclear magnetic resonance (NMR) spectroscopy in diamond anvil cells (DACs) has been employed as a structural and electronic probe of condensed matter systems at pressures well into the megabar range. However, extensive spin interactions and sample heterogeneities under pressure often lead to significant spectral overlap, inhibiting inde…
▽ More
Over the last decade, frequency-domain in-situ high-pressure nuclear magnetic resonance (NMR) spectroscopy in diamond anvil cells (DACs) has been employed as a structural and electronic probe of condensed matter systems at pressures well into the megabar range. However, extensive spin interactions and sample heterogeneities under pressure often lead to significant spectral overlap, inhibiting independent observation of chemically similar spin sub-species in the same sample. In this work, we introduce a time-domain relaxometry framework specifically suited for DAC experiments, named muT2-NMR. Experimental flexibility and operational robustness are benchmarked on three hydrogen-rich molecular solids at pressures up to 72 GPa. We demonstrate that muT2-NMR can resolve individual molecular subunits in relaxation space, paving the way for novel high-pressure, high-resolution NMR applications in molecular solids.
△ Less
Submitted 6 January, 2026;
originally announced January 2026.
-
Unexpected increase of intensity-dependent excitonic second- and third-harmonic generation induced by static electric fields
Authors:
Ruixin Zuo,
Matthias Reichelt,
Cong Ngo,
Xiaohong Song,
Weifeng Yang,
Torsten Meier
Abstract:
We compute and analyze the dependence of excitonic second- and third-harmonic generation (SHG/THG) as a function of the optical excitation intensity in the presence of static electric fields by solving the semiconductor Bloch equations. Our simulations are performed for excitation of the strongly bound intralayer exciton of an inversion-symmetric homobilayer of MoS2 with in-plane electric fields.…
▽ More
We compute and analyze the dependence of excitonic second- and third-harmonic generation (SHG/THG) as a function of the optical excitation intensity in the presence of static electric fields by solving the semiconductor Bloch equations. Our simulations are performed for excitation of the strongly bound intralayer exciton of an inversion-symmetric homobilayer of MoS2 with in-plane electric fields. We demonstrate that for resonant excitation at the 1s K-exciton the SHG and the THG show complex dependencies on both the strength of the static field and the peak amplitude of the optical pulse. For sufficiently intense optical excitation, the THG increases and the SHG increases superlinearly with the amplitude of the static field as long as exciton ionization is not yet dominating. Microscopic simulations demonstrate that these dependencies arise from an interplay between several effects including static and transient Stark shifts, exciton ionization, Wannier-Stark localization, off-resonant Rabi oscillations, and a modified interference between optical nonlinearities induced by the intraband acceleration. Our findings offer several new possibilities for controlling the strong-field dynamics of systems with strongly bound excitons.
△ Less
Submitted 7 November, 2025;
originally announced November 2025.
-
Magneto-Chiral Anisotropy in Josephson Diode Effect of All-Metallic Lateral Junctions with Interfacial Rashba Spin-Orbit Coupling
Authors:
Maximilian Mangold,
Lorenz Bauriedl,
Johanna Berger,
Chang Yu-Cheng,
Thomas N. G. Meier,
Matthias Kronseder,
Pertti Hakonen,
Christian H. Back,
Christoph Strunk,
Dhavala Suri
Abstract:
We explore the role of interfacial Rashba spin-orbit coupling (SOC) for the Josephson diode effect in all-metal diffusive Josephson junctions. Devices with Fe/Pt and Cu/Pt weak links between Nb leads reveal a Josephson diode effect in an in-plane magnetic field with magneto-chiral anisotropy according to the point symmetry of Rashba SOC. The Rashba SOC originates from inversion symmetry breaking a…
▽ More
We explore the role of interfacial Rashba spin-orbit coupling (SOC) for the Josephson diode effect in all-metal diffusive Josephson junctions. Devices with Fe/Pt and Cu/Pt weak links between Nb leads reveal a Josephson diode effect in an in-plane magnetic field with magneto-chiral anisotropy according to the point symmetry of Rashba SOC. The Rashba SOC originates from inversion symmetry breaking at the metal-metal interfaces. A control sample with a plain Cu-layer as weak link, in contrast, exhibits an axis-symmetric diode effect. The Fraunhofer patterns display an apparent inverted hysteresis which can be traced back to stray fields resulting from the conventional hysteretic vortex pinning in the Nb contacts.
△ Less
Submitted 27 April, 2026; v1 submitted 2 November, 2025;
originally announced November 2025.
-
Microscopic approach to the quantized light-matter interaction in semiconductor nanostructures: Complex coupled dynamics of excitons, biexcitons, and photons
Authors:
Hendrik Rose,
Stefan Schumacher,
Torsten Meier
Abstract:
We present a microscopic and fully quantized model to investigate the interaction between semiconductor nanostructures and quantum light fields including the many-body Coloumb interaction between photoexcited electrons and holes. Our approach describes the coupled dynamics of the quantum light field and single and double electron-hole pairs, i.e., excitons and biexcitons, and exactly accounts for…
▽ More
We present a microscopic and fully quantized model to investigate the interaction between semiconductor nanostructures and quantum light fields including the many-body Coloumb interaction between photoexcited electrons and holes. Our approach describes the coupled dynamics of the quantum light field and single and double electron-hole pairs, i.e., excitons and biexcitons, and exactly accounts for Coulomb many-body correlations and carrier band dispersions. Using a simplified yet exact approach, we study a one-dimensional two-band system interacting with a single-mode, two-photon quantum state within a Tavis$\unicode{x2013}$Cummings framework. By employing an exact coherent factorization scheme, the computational complexity is reduced significantly enabling numerical simulations. We also derive a simplified model which includes only the bound $1s$-exciton and biexciton states for comparison. Our simulations reveal distinct single- and two-photon Rabi oscillations, corresponding to photon-exciton and exciton-biexciton transitions. We demonstrate, in particular, that biexciton continuum states significantly modify the dynamics in a way that cannot be captured by simplified models which consider only bound states. Our findings emphasize the importance of a comprehensive microscopic modeling in order to accurately describe quantum optical phenomena of interacting electronic many-body systems.
△ Less
Submitted 27 June, 2025;
originally announced June 2025.
-
On the ambient conditions crystal structure of AgSbTe2
Authors:
Baihong Sun,
Sergei Grazhdannikov,
Muhamed Dawod,
Lunhua He,
Jiazheng Hao,
Thomas Meier,
Yansun Yao,
Yaron Amouyal,
Elissaios Stavrou
Abstract:
We present a combined X-ray and neutron diffraction, Raman spectroscopy, and 121Sb NMR studies of AgSbTe2, supported by first-principles calculations aiming to elucidate its crystal structure. While diffraction methods cannot unambiguously resolve the structure, Raman and NMR data, together with electric field gradient calculations, strongly support the rhombohedral R-3m phase. Moreover, the agree…
▽ More
We present a combined X-ray and neutron diffraction, Raman spectroscopy, and 121Sb NMR studies of AgSbTe2, supported by first-principles calculations aiming to elucidate its crystal structure. While diffraction methods cannot unambiguously resolve the structure, Raman and NMR data, together with electric field gradient calculations, strongly support the rhombohedral R-3m phase. Moreover, the agreement between experimental and calculated Raman spectra further corroborates this result, resolving the 60-year sold debate about the exact crystal structure of the AgSbTe2 compound.
△ Less
Submitted 16 June, 2025;
originally announced June 2025.
-
Diffusion Driven Transient Hydrogenation in Metal Superhydrides at Extreme Conditions
Authors:
Yishan Zhou,
Yunhua Fu,
Meng Yang,
Israel Osmond,
Rajesh Jana,
Takeshi Nakagawa,
Owen Moulding,
Jonathan Buhot,
Sven Friedemann,
Dominique Laniel,
Thomas Meier
Abstract:
In recent years, metal hydride research has become one of the driving forces of the high-pressure community, as it is believed to hold the key to superconductivity close to ambient temperature. While numerous novel metal hydride compounds have been reported and extensively investigated for their superconducting properties, little attention has been focused on the atomic and electronic states of hy…
▽ More
In recent years, metal hydride research has become one of the driving forces of the high-pressure community, as it is believed to hold the key to superconductivity close to ambient temperature. While numerous novel metal hydride compounds have been reported and extensively investigated for their superconducting properties, little attention has been focused on the atomic and electronic states of hydrogen, the main ingredient in these novel compounds. Here, we present combined $^{1}H$- and $^{139}La$-NMR data on lanthanum superhydrides, $LaH_{x}$, ($x = 10.2 - 11.1$), synthesized after laser heating at pressures above 160 GPa. Strikingly, we found hydrogen to be in a highly diffusive state at room temperature, with diffusion coefficients in the order of $10^{-6}~cm^2s^{-1}$. We found that this diffusive state of hydrogen results in a dynamic de-hydrogenation of the sample over the course of several weeks, approaching a composition similar to its precursor materials. Quantitative measurements demonstrate that the synthesized superhydrides continuously decompose over time. Transport measurements underline this conclusion as superconducting critical temperatures were found to decrease significantly over time as well. This observation sheds new light on formerly unanswered questions on the long-term stability of metal superhydrides.
△ Less
Submitted 23 August, 2024;
originally announced August 2024.
-
Hexagonal to Monoclinic Phase Transition in Dense Hydrogen Phase III Detected by High-Pressure NMR
Authors:
Meng Yang,
Yishan Zhou,
Rajesh Jana,
Takeshi Nakagawa,
Yunhua Fu,
Thomas Meier
Abstract:
Conclusive crystal structure determination of the high pressure phases of hydrogen remains elusive due to lack of core electrons and vanishing wave vectors, rendering standard high-pressure experimental methods moot. Ab-initio DFT calculations have shown that structural polymorphism might be solely resolvable using high-resolution nuclear magnetic resonance (NMR) spectroscopy at mega-bar pressures…
▽ More
Conclusive crystal structure determination of the high pressure phases of hydrogen remains elusive due to lack of core electrons and vanishing wave vectors, rendering standard high-pressure experimental methods moot. Ab-initio DFT calculations have shown that structural polymorphism might be solely resolvable using high-resolution nuclear magnetic resonance (NMR) spectroscopy at mega-bar pressures, however technical challenges have precluded such experiments thus far. Here, we present in-situ high-pressure high-resolution NMR experiments in hydrogen phase III between 181 GPa and 208 GPa at room temperature. Our spectra suggest that at lower pressures phase III adopts a hexagonal P6122 crystal structure, transitioning into a monoclinic C2/c phase at about 197 GPa. The high resolution spectra are in excellent agreement with earlier structural and spectral predictions and underline the possibility of a subtle P6122 to C2/c phase transition in hydrogen phase III. These experiments show the importance of a combination of ab-initio calculations and low-Z sensitive spectral probes in high-pressure science in elucidating the structural complexity of the most abundant element in our universe.
△ Less
Submitted 27 July, 2024;
originally announced July 2024.
-
Floquet dynamics of ultracold atoms in optical lattices with a parametrically modulated trapping potential
Authors:
Usman Ali,
Martin Holthaus,
Torsten Meier
Abstract:
Experiments with ultracold atoms in optical lattices usually involve a weak parabolic trapping potential which merely serves to confine the atoms, but otherwise remains negligible. In contrast, we suggest a different class of experiments in which the presence of a stronger trap is an essential part of the set-up. Because the trap-modified on-site energies exhibit a slowly varying level spacing, si…
▽ More
Experiments with ultracold atoms in optical lattices usually involve a weak parabolic trapping potential which merely serves to confine the atoms, but otherwise remains negligible. In contrast, we suggest a different class of experiments in which the presence of a stronger trap is an essential part of the set-up. Because the trap-modified on-site energies exhibit a slowly varying level spacing, similar to that of an anharmonic oscillator, an additional time-periodic trap modulation with judiciously chosen parameters creates nonlinear resonances which enable efficient Floquet engineering. We employ a Mathieu approximation for constructing the near-resonant Floquet states in an accurate manner and demonstrate the emergence of effective ground states from the resonant trap eigenstates. Moreover, we show that the population of the Floquet states is strongly affected by the phase of a sudden turn-on of the trap modulation, which leads to significantly modified and rich dynamics. As a guideline for further studies, we argue that the deliberate population of only the resonance-induced effective ground states will allow one to realize Floquet condensates which follow classical periodic orbits, thus providing challenging future perspectives for the investigation of the quantum-classical correspondence.
△ Less
Submitted 3 May, 2024;
originally announced May 2024.
-
Unveiling a Novel Metal-to-Metal Transition in LuH2: Critically Challenging Superconductivity Claims in Lutetium Hydrides
Authors:
Dong Wang,
Ningning Wang,
Caoshun Zhang,
Chunsheng Xia,
Weicheng Guo,
Xia Yin,
Kejun Bu,
Takeshi Nakagawa,
Jianbo Zhang,
Federico Gorelli,
Philip Dalladay-Simpson,
Thomas Meier,
Xujie Lü,
Liling Sun,
Jinguang Cheng,
Qiaoshi Zeng,
Yang Ding,
Ho-kwang Mao
Abstract:
Following the recent report by Dasenbrock-Gammon et al. (2023) of near-ambient superconductivity in nitrogen-doped lutetium trihydride (LuH3-δNε), significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop. Here, we meticulously revisit these claims through comprehensive characterization and investigations. We definitively identify the repor…
▽ More
Following the recent report by Dasenbrock-Gammon et al. (2023) of near-ambient superconductivity in nitrogen-doped lutetium trihydride (LuH3-δNε), significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop. Here, we meticulously revisit these claims through comprehensive characterization and investigations. We definitively identify the reported material as lutetium dihydride (LuH2), resolving the ambiguity surrounding its composition. Under similar conditions (270-295 K and 1-2 GPa), we replicate the reported sharp decrease in electrical resistance with a 30% success rate, aligning with Dasenbrock-Gammon et al.'s observations. However, our extensive investigations reveal this phenomenon to be a novel, pressure-induced metal-to-metal transition intrinsic to LuH2, distinct from superconductivity. Intriguingly, nitrogen doping exerts minimal impact on this transition. Our work not only elucidates the fundamental properties of LuH2 and LuH3 but also critically challenges the notion of superconductivity in these lutetium hydride systems. These findings pave the way for future research on lutetium hydride systems while emphasizing the crucial importance of rigorous verification in claims of ambient temperature superconductivity.
△ Less
Submitted 28 January, 2024; v1 submitted 25 January, 2024;
originally announced January 2024.
-
Temporal sorting of optical multi-wave-mixing processes in semiconductor quantum dots
Authors:
S. Grisard,
A. V. Trifonov,
H. Rose,
R. Reichhardt,
M. Reichelt,
C. Schneider,
M. Kamp,
S. Höfling,
M. Bayer,
T. Meier,
I. A. Akimov
Abstract:
Coherent control of ensembles of light emitters by means of multi-wave mixing processes is key for the realization of high capacity optical quantum memories and information processing devices. In this context, semiconductor quantum dots placed in optical microcavities represent excellent candidates to explore strong light-matter interactions beyond the limits of perturbative non-linear optics and…
▽ More
Coherent control of ensembles of light emitters by means of multi-wave mixing processes is key for the realization of high capacity optical quantum memories and information processing devices. In this context, semiconductor quantum dots placed in optical microcavities represent excellent candidates to explore strong light-matter interactions beyond the limits of perturbative non-linear optics and control the unitary evolution of optically driven quantum systems. In this work, we demonstrate that a sequence of two optical picosecond pulses can be used to establish coherent control over the phase evolution of the ensemble of trions in (In,Ga)As quantum dots independent of their initial quantum state. Our approach is based on coherent transfer between degenerate multi-wave-mixing signals in the strong field limit where Rabi rotations in multi-level systems take place. In particular, we use the two-pulse photon echo sequence to uncover the coherent dynamics of the trion ensemble, whereas the areas of two additional control pulses serve as tuning knobs for adjusting the magnitude and timing of the coherent emission. Furthermore, we make use of the spin degeneracy of ground and excited state of trions to control the polarization state of the emitted signal. Surprisingly, we reveal that the use of optical control pulses, whose durations are comparable to the dephasing time of the ensemble, lifts the temporal degeneracy between wave-mixing processes of different order. This phenomenon is manifested in a significant modification of the temporal shape of the coherent optical response for strong optical fields. Lifting the temporal degeneracy allows to smoothly trace the transition from the perturbative to the regime of Rabi rotations and opens up new possibilities for the optical investigation of complex energy level structures in so far unexplored material systems.
△ Less
Submitted 5 February, 2023;
originally announced February 2023.
-
Non-reciprocity of Vortex-limited Critical Current in Conventional Superconducting Micro-bridges
Authors:
Dhavala Suri,
Akashdeep Kamra,
Thomas N. G. Meier,
Matthias Kronseder,
Wolfgang Belzing,
Christian H. Back,
Christoph Strunk
Abstract:
Non-reciprocity in the critical current has been observed in a variety of superconducting systems and has been called the superconducting diode effect. The origin underlying the effect depends on the symmetry breaking mechanisms at play. We investigate superconducting micro bridges of NbN and also NbN/magnetic insulator (MI) hybrids. We observe a large diode efficiency of $\approx$~30\% when an ou…
▽ More
Non-reciprocity in the critical current has been observed in a variety of superconducting systems and has been called the superconducting diode effect. The origin underlying the effect depends on the symmetry breaking mechanisms at play. We investigate superconducting micro bridges of NbN and also NbN/magnetic insulator (MI) hybrids. We observe a large diode efficiency of $\approx$~30\% when an out-of-plane magnetic field as small as 25~mT is applied. In both NbN and NbN/MI hybrid, we find that the diode effect vanishes when the magnetic field is parallel to the sample plane. Our observations are consistent with the critical current being determined by the vortex surface barrier. Unequal barriers on the two edges of the superconductor strip result in the diode effect. Furthermore, the rectification is observed up to a temperature $\sim$10~K, which makes the device potential for diode based applications over larger temperature range than before.
△ Less
Submitted 13 September, 2022;
originally announced September 2022.
-
High-Pressure Synthesis of Seven Lanthanum Hydrides with a Significant Variability of Hydrogen Content
Authors:
Dominique Laniel,
Florian Trybel,
Bjoern Winkler,
Florian Knoop,
Timofey Fedotenko,
Saiana Khandarkhaeva,
Alena Aslandukova,
Thomas Meier,
Stella Chariton,
Konstantin Glazyrin,
Victor Milman,
Vitali Prakapenka,
Igor A. Abrikosov,
Leonid Dubrovinsky,
Natalia Dubrovinskaia
Abstract:
The lanthanum-hydrogen system has attracted significant attention following the report of superconductivity in LaH10 at near-ambient temperatures and high pressures. Here, we present the results of our single-crystal X-ray diffraction studies on this system, supported by density functional theory calculations, which reveal an unexpected chemical and structural diversity of lanthanum hydrides synth…
▽ More
The lanthanum-hydrogen system has attracted significant attention following the report of superconductivity in LaH10 at near-ambient temperatures and high pressures. Here, we present the results of our single-crystal X-ray diffraction studies on this system, supported by density functional theory calculations, which reveal an unexpected chemical and structural diversity of lanthanum hydrides synthesized in the range of 50 to 180 GPa. Seven lanthanum hydrides were produced, LaH3, LaH~4, LaH4+δ, La4H23, LaH6+δ, LaH9+δ, and LaH10+δ, and the atomic coordinates of lanthanum in their structures determined. The regularities in rare-earth element hydrides unveiled here provide clues to guide the search for other synthesizable hydrides and candidate high-temperature superconductors. The hydrogen content variability in lanthanum hydrides and the samples' phase heterogeneity underline the challenges related to assessing potentially superconducting phase(s) and the nature of electronic transitions in high-pressure hydrides.
△ Less
Submitted 22 August, 2022;
originally announced August 2022.
-
Direct Hydrogen Quantification in High-pressure Metal Hydrides
Authors:
Thomas Meier,
Dominique Laniel,
Florian Trybel
Abstract:
High-pressure metal-hydride (MH) research evolved into a thriving field within condensed matter physics following the realisation of metallic compounds showing phonon mediated near room-temperature superconductivity. However, severe limitations in determining the chemical formula of the reaction products, especially with regards to their hydrogen content, impedes a deep understanding of the synthe…
▽ More
High-pressure metal-hydride (MH) research evolved into a thriving field within condensed matter physics following the realisation of metallic compounds showing phonon mediated near room-temperature superconductivity. However, severe limitations in determining the chemical formula of the reaction products, especially with regards to their hydrogen content, impedes a deep understanding of the synthesized phases and can lead to significantly erroneous conclusions. Here, we present a way to directly access the hydrogen content of MH solids synthesised at high pressures in (laser-heated) diamond anvil cells using nuclear magnetic resonance (NMR) spectroscopy. We show that this method can be used to investigate MH compounds with a wide range of hydrogen content, from MHx with x=0.15 (CuH0.15) to x < 6.4 (H 6+-0.4 S 5).
△ Less
Submitted 8 August, 2022;
originally announced August 2022.
-
Multiple Rabi rotations of trions in InGaAs quantum dots observed by photon echo spectroscopy with spatially shaped laser pulses
Authors:
S. Grisard,
H. Rose,
A. V. Trifonov,
R. Reichhardt,
D. E. Reiter,
M. Reichelt,
C. Schneider,
M. Kamp,
S. Höfling,
M. Bayer,
T. Meier,
I. A. Akimov
Abstract:
We study Rabi rotations arising in intensity-dependent photon echoes from an ensemble of self-assembled InGaAs quantum dots. To achieve a uniform distribution of intensities within the excited ensemble, we introduce flattop intensity profiles of picosecond laser pulses. This allows us to overcome the damping of Rabi rotations imposed by the spatial inhomogeneity of Rabi frequencies by a Gaussian l…
▽ More
We study Rabi rotations arising in intensity-dependent photon echoes from an ensemble of self-assembled InGaAs quantum dots. To achieve a uniform distribution of intensities within the excited ensemble, we introduce flattop intensity profiles of picosecond laser pulses. This allows us to overcome the damping of Rabi rotations imposed by the spatial inhomogeneity of Rabi frequencies by a Gaussian laser profile. Using photon echo polarimetry, we distinguish between the coherent optical responses from exciton and trion ensembles. Here, we demonstrate that a photo-induced charging of the quantum dots leads to a significant reduction of the number of neutral quantum dots under resonant excitation with intensive optical pulses with areas exceeding $\fracπ{2}$. The trion ensemble shows robust Rabi rotations when the area of the refocussing pulse is increased up to 5.5$π$. We analyze the remaining attenuation of Rabi rotations by theoretical modeling of excitation induced dephasing, inhomogeneity of dipole moments, and coupling to acoustic phonons. The latter is identified as the dominating mechanism resulting in a loss of optical coherence during the action of the involved optical pulses.
△ Less
Submitted 20 September, 2022; v1 submitted 16 May, 2022;
originally announced May 2022.
-
Super-Bloch oscillations with parametric modulation of a parabolic trap
Authors:
Usman Ali,
Torsten Meier
Abstract:
Super-Bloch oscillations are the outcome of a relative phase between Bloch oscillations and modulations of the periodic lattice. We analyze the dynamics for a model system in which such a relative phase is intrinsically present due to the position-dependent force provided by a parabolic trap and therefore an external detuning is not required. The relative phase is not unique and the realized dynam…
▽ More
Super-Bloch oscillations are the outcome of a relative phase between Bloch oscillations and modulations of the periodic lattice. We analyze the dynamics for a model system in which such a relative phase is intrinsically present due to the position-dependent force provided by a parabolic trap and therefore an external detuning is not required. The relative phase is not unique and the realized dynamics depends on the initial phase of the modulated parabolic potential. We provide accurate explanations for the different obtained oscillatory transport and spreading regimes by analyzing the spatio-temporal dynamics in real space and by visualizing the relative phase in the k-space dynamics. We also compare our numerical results to an approximate semiclassical analytical expression for the group velocity for a modulated constant force system and find good agreement for coherent oscillations but deviations for oscillations with spreading dynamics which altogether supports the interpretations of our findings.
△ Less
Submitted 26 April, 2022;
originally announced April 2022.
-
Universal Hydrogen Bond Symmetrisation Dynamics Under Extreme Conditions
Authors:
Thomas Meier,
Florian Trybel,
Dominique Laniel,
Saiana Khandarkhaeva,
Takayuki Ishii,
Alena Aslandukova,
Natalia Dubrovinskaia,
Leonid Dubrovinsky
Abstract:
The experimental study of hydrogen bonds and their symmetrisation under extreme conditions is predominantly driven by diffraction methods, despite challenges of localising or probing the hydrogen subsystems directly. Until recently, H-bond symmetrisation has been addressed in terms of either nuclear quantum effects, spin crossovers or direct structural transitions; often leading to contradictory i…
▽ More
The experimental study of hydrogen bonds and their symmetrisation under extreme conditions is predominantly driven by diffraction methods, despite challenges of localising or probing the hydrogen subsystems directly. Until recently, H-bond symmetrisation has been addressed in terms of either nuclear quantum effects, spin crossovers or direct structural transitions; often leading to contradictory interpretations when combined. Here, we present high-resolution \textit{in-situ} $^1$H-NMR experiments in diamond anvil cells investigating a wide range of hydrogen bonded systems at pressure ranges of up to 90 GPa covering their respective H-bond symmetrisation. We found pronounced minima in the pressure dependence of the NMR resonance line-widths associated with a maximum in hydrogen mobility, precursor to a localisation of hydrogen atoms. These minima, independent of of the chemical environment of the linear O -- H-O unit, can be found in a narrow range of oxygen-oxygen distances between 2.44 and 2.45 Å, leading to an average critical oxygen-oxygen distance of $\bar{r}_{\rm OO}^{crit}=2.443(1)$ Å.
△ Less
Submitted 16 January, 2022;
originally announced January 2022.
-
Coherent Contributions to Population Dynamics in a Semiconductor Microcavity
Authors:
J. Paul,
H. Rose,
E. Swagel,
T. Meier,
J. K. Wahlstrand,
A. D. Bristow
Abstract:
Multidimensional coherent spectroscopy (MDCS) is used to separate coherent and incoherent many-body contributions to the population-time dynamics in a GaAs-based semiconductor microcavity encapsulating a single InGaAs quantum well. In a three-pulse four-wave-mixing scheme, the second delay time is the population time that in MDCS probes excited-state coherences and population dynamics. Nonlinear o…
▽ More
Multidimensional coherent spectroscopy (MDCS) is used to separate coherent and incoherent many-body contributions to the population-time dynamics in a GaAs-based semiconductor microcavity encapsulating a single InGaAs quantum well. In a three-pulse four-wave-mixing scheme, the second delay time is the population time that in MDCS probes excited-state coherences and population dynamics. Nonlinear optical interactions can mix these contributions, which are isolated here for the lower- and upper-exciton-polariton through the self- and mutual-interaction features. Results show fast decays and oscillations arising from the coherent response, including a broad stripe along the absorption energy axis, and longer time mutual-interaction features that do not obey a simple population decay model. These results are qualitatively replicated by Bloch equation simulations for the 1s exciton strongly coupled to the intracavity field. The simulations allow for separation of coherent and incoherent Pauli-blocking and Coulomb interaction terms within the chi^(3)-limit, and direct comparison of each feature in one-quantum rephasing and zero-quantum spectra.
△ Less
Submitted 21 February, 2022; v1 submitted 2 December, 2021;
originally announced December 2021.
-
Tailoring Luminescent Properties of SrS:Ce by Modulating Defects: Sr-Deficiency and Na+ Doping
Authors:
Shuqin Chang,
Jipeng Fu,
Xuan Sun,
Guangcan Bai,
Guoquan Liu,
Kaina Wang,
Ligang Xu,
Qi Wei,
Thomas Meier,
Mingxue Tang
Abstract:
Ce3+ doped SrS phosphors with a charge-compensating Na+ for light-emitting diode (LED) applications have been successfully synthesized via a solid-state reaction method, which can be indexed to rock-salt-like crystal structures of Fm-3m space group. SrS:(Ce3+)x(x=0.005-0.05) and SrS:(Ce3+)0.01,(Na+)y(y=0.005-0.030) phosphors were excited by 430nm UV-VIS light, associated to the 5d1-4f1 transition…
▽ More
Ce3+ doped SrS phosphors with a charge-compensating Na+ for light-emitting diode (LED) applications have been successfully synthesized via a solid-state reaction method, which can be indexed to rock-salt-like crystal structures of Fm-3m space group. SrS:(Ce3+)x(x=0.005-0.05) and SrS:(Ce3+)0.01,(Na+)y(y=0.005-0.030) phosphors were excited by 430nm UV-VIS light, associated to the 5d1-4f1 transition of Ce3+. The composition-optimized SrS:(Ce3+)0.01,(Na+)0.015 phosphors showed an intense broad emission band at 430-700nm. The doping of Na+ was probed by solid-state nuclear magnetic resonance. The 430 nm pumped with white LED (w-LED) combining SrS:(Ce3+)0.01,(Na+)0.015 phosphors and Sr2Si5N8:Eu2+ phosphors shows a color-rendering index (Ra) of 89.7. The proposed strategy provides new avenues for design and realization of novel high color quality solid-state lighting emitting diodes (SS-LEDS).
△ Less
Submitted 22 November, 2021;
originally announced November 2021.
-
Absence of proton tunneling during the hydrogen bond symmetrization in $δ$-AlOOH
Authors:
Florian Trybel,
Thomas Meier,
Biao Wang,
Gerd Steinle-Neumann
Abstract:
$δ$-AlOOH is of significant crystallochemical interest due to a subtle structural transition near 10 GPa from a $P2_1nm$ to a $Pnnm$ structure, the nature and origin of hydrogen disorder, the symmetrization of the O-H$\cdots…
▽ More
$δ$-AlOOH is of significant crystallochemical interest due to a subtle structural transition near 10 GPa from a $P2_1nm$ to a $Pnnm$ structure, the nature and origin of hydrogen disorder, the symmetrization of the O-H$\cdots$O hydrogen bond and their interplay. We perform a series of density functional theory based simulations in combination with high-pressure nuclear magnetic resonance experiments on $δ$-AlOOH up to 40 GPa with the goal to better characterize the hydrogen potential and therefore the nature of hydrogen disorder. Simulations predict a phase transition in agreement with our nuclear magnetic resonance experiments at $10-11$ GPa and hydrogen bond symmetrization at $14.7$ GPa. Calculated hydrogen potentials do not show any double-well character and there is no evidence for proton tunneling in our nuclear magnetic resonance data.
△ Less
Submitted 13 October, 2021;
originally announced October 2021.
-
In-situ High Pressure Nuclear Magnetic Resonance Crystallography
Authors:
Thomas Meier,
Alena Aslandukova,
Florian Trybel,
Dominique Laniel,
Takayuki Ishii,
Saiana Khandarkhaeva,
Natalia Dubrovinskaia,
Leonid Dubrovinsky
Abstract:
Our recent developments in in-situ nuclear magnetic resonance (NMR) spectroscopy under extreme conditions led to the observation of a wide variety of physical phenomena not accessible with standard high pressure experimental probes. However, inherent di- or quadrupolar line broadening in diamond anvil cell (DAC) based NMR experiments often limit detailed investigations of local atomic structures,…
▽ More
Our recent developments in in-situ nuclear magnetic resonance (NMR) spectroscopy under extreme conditions led to the observation of a wide variety of physical phenomena not accessible with standard high pressure experimental probes. However, inherent di- or quadrupolar line broadening in diamond anvil cell (DAC) based NMR experiments often limit detailed investigations of local atomic structures, especially if different phases or local environments are coexisting. Here, we present our progress in the development of high resolution NMR experiments in DACs using one and two-dimensional homonuclear decoupling experiments at pressures up to the Mbar regime. Using this technique, spectral resolutions in the order of 1 ppm and below have been achieved, enabling high pressure structural analysis. Several examples will demonstrate the wide applicability of this method for extreme conditions research.
△ Less
Submitted 11 August, 2021;
originally announced August 2021.
-
High-Pressure Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3 Featuring Nitrogen Dimers with Non-Integer Charges and Anion-Driven Metallicity
Authors:
Dominique Laniel,
Bjoern Winkler,
Timofey Fedotenko,
Alena Aslandukova,
Andrey Aslandukov,
Sebastian Vogel,
Thomas Meier,
Maxim Bykov,
Stella Chariton,
Konstantin Glazyrin,
Victor Milman,
Vitali Prakapenka,
Wolfgang Schnick,
Leonid Dubrovinsky,
Natalia Dubrovinskaia
Abstract:
Charged nitrogen dimers are ubiquitous in high-pressure binary metal-nitrogen systems. They are known to possess integer formal charges x varying from one through four. Here, we present the investigation of the binary alkali- and alkaline earth metal-nitrogen systems, Na-N, Ca-N, Sr-N, Ba-N to 70 GPa. We report on compounds-Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3-featuring charged nitrogen dimer…
▽ More
Charged nitrogen dimers are ubiquitous in high-pressure binary metal-nitrogen systems. They are known to possess integer formal charges x varying from one through four. Here, we present the investigation of the binary alkali- and alkaline earth metal-nitrogen systems, Na-N, Ca-N, Sr-N, Ba-N to 70 GPa. We report on compounds-Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3-featuring charged nitrogen dimers with paradigm-breaking non-integer charges, x = 0.67, 0.75 and 1.5. The metallic nature of all four compounds is deduced from ab initio calculations. The conduction electrons occupy the pi* antibonding orbitals of the charged nitrogen dimers that results in anion-driven metallicity. Delocalization of these electrons over the pi* antibonding states enables the non-integer electron count of the dinitrogen species. Anion-driven metallicity is expected to be found among a variety of compounds with homoatomic anions (e.g., polynitrides, carbides, and oxides), with the conduction electrons playing a decisive role in their properties.
△ Less
Submitted 24 May, 2021;
originally announced May 2021.
-
Non-Degenerate Two-Photon Absorption in ZnSe: Experiment and Theory
Authors:
L. Krauss-Kodytek,
W. -R. Hannes,
T. Meier,
C. Ruppert,
M. Betz
Abstract:
We experimentally and theoretically investigate the non-degenerate two-photon absorption coefficient $β(ω_1,ω_2)$ in the prototypical semiconductor ZnSe. In particular, we provide a comprehensive data set on the dependence of $β(ω_1,ω_2)$ on the non-degeneracy parameter $ω_1/ω_2$ with the total frequency sum $ω_1+ω_2$ kept constant. We find a substantial increase of the two-photon absorption stren…
▽ More
We experimentally and theoretically investigate the non-degenerate two-photon absorption coefficient $β(ω_1,ω_2)$ in the prototypical semiconductor ZnSe. In particular, we provide a comprehensive data set on the dependence of $β(ω_1,ω_2)$ on the non-degeneracy parameter $ω_1/ω_2$ with the total frequency sum $ω_1+ω_2$ kept constant. We find a substantial increase of the two-photon absorption strength with increasing $ω_1/ω_2$. In addition, different crystallographic orientations and polarization configurations are investigated. The nonlinear optical response is analyzed theoretically by evaluating the multiband semiconductor Bloch equations including inter- and intraband excitations in the length gauge. The band structure and the matrix elements are taken an eight-band k.p model. The simulation results are in very good agreement with the experiment.
△ Less
Submitted 11 August, 2021; v1 submitted 22 May, 2021;
originally announced May 2021.
-
Proton dynamics in high-pressure ice-VII from density functional theory
Authors:
Florian Trybel,
Michael Cosacchi,
Thomas Meier,
Vollrath Martin Axt,
Gerd Steinle-Neumann
Abstract:
Using a density-functional-theory-based approach, we explore the symmetrization and proton dynamics in ice-VII, for which recent high-pressure NMR experiments indicate significant proton dynamics in the pressure-range of $20-95$ GPa. We directly sample the potential seen by the proton and find a continuous transition from double- to single-well character over the pressure range of 2 to 130 GPa acc…
▽ More
Using a density-functional-theory-based approach, we explore the symmetrization and proton dynamics in ice-VII, for which recent high-pressure NMR experiments indicate significant proton dynamics in the pressure-range of $20-95$ GPa. We directly sample the potential seen by the proton and find a continuous transition from double- to single-well character over the pressure range of 2 to 130 GPa accompanied by proton dynamics in agreement with the NMR experiments.
△ Less
Submitted 23 February, 2021;
originally announced February 2021.
-
Microscopic analysis of high harmonic generation in semiconductors with degenerate bands
Authors:
Le Huu Thong,
Cong Ngo,
Huynh Thanh Duc,
Xiaohong Song,
Torsten Meier
Abstract:
Based on the multiband semiconductor Bloch equations a microscopic approach to high-harmonic generation in crystalline solids which is able to properly describe degenerate bands and band crossings is presented and analyzed. It is well-known that numerical band structure calculations typically provide electronic wave functions with an undetermined k-dependent phase which results in matrix elements…
▽ More
Based on the multiband semiconductor Bloch equations a microscopic approach to high-harmonic generation in crystalline solids which is able to properly describe degenerate bands and band crossings is presented and analyzed. It is well-known that numerical band structure calculations typically provide electronic wave functions with an undetermined k-dependent phase which results in matrix elements which contain arbitrary k-dependent phases. In addition, such approaches usually mix degenerate bands and bands with an energy difference smaller than the numerical precision in an arbitrary way for each point in k-space. These ambiguities are problematic if one considers the dynamics induced by electric fields since the matrix elements of the position operator involve a derivative of the wave functions with respect to k. When the light-matter interaction is described in the length gauge, the problem of arbitrary phases and degenerate subspace mixing of Bloch states is solved by adopting a smooth gauge transformation along the field direction. The results obtained within this method are validated by comparing with calculations in the velocity gauge. Although we obtain in both gauges the same overall result, the length gauge is advantageous since it converges with a smaller number of bands and thus requires significantly less numerical effort than the velocity gauge. Also an unique distinction between inter- and intraband contributions and thus an instructive physical interpretation is possible in the length gauge whereas in the velocity gauge this is unclear. The computed polarization-direction-dependent high-harmonic spectra agree well with experimental data reported for GaAs. Furthermore, it is demonstrated that, under proper conditions, the Berry curvature is largely responsible for the even-order harmonics which are polarized perpendicular to the driving field.
△ Less
Submitted 2 December, 2020;
originally announced December 2020.
-
Nuclear Spin Crossover in Dense Molecular Hydrogen
Authors:
Thomas Meier,
Dominique Laniel,
Miriam Pena-Alvarez,
Florian Trybel,
Saiana Khandarkhaeva,
Alena Krupp,
Jeroen Jacobs,
Natalia Dubrovinskaia,
Leonid Dubrovinsky
Abstract:
The laws of quantum mechanics are often tested against the behaviour of the lightest element in the periodic table, hydrogen. One of the most striking properties of molecular hydrogen is the coupling between molecular rotational properties and nuclear spin orientations, giving rise to the spin isomers ortho- and para-hydrogen. At high pressure, as intermolecular interactions increase significantly…
▽ More
The laws of quantum mechanics are often tested against the behaviour of the lightest element in the periodic table, hydrogen. One of the most striking properties of molecular hydrogen is the coupling between molecular rotational properties and nuclear spin orientations, giving rise to the spin isomers ortho- and para-hydrogen. At high pressure, as intermolecular interactions increase significantly, the free rotation of H2 molecules is increasingly hindered, and consequently a modification of the coupling between molecular rotational properties and the nuclear spin system can be anticipated. To date, high-pressure experimental methods have not been able to observe nuclear spin states at pressures approaching 100 GPa and consequently the effect of high pressure on the nuclear spin statistics could not be directly measured. Here, we present in-situ high-pressure nuclear magnetic resonance data on molecular hydrogen in its hexagonal phase I up to 123 GPa at room temperature. While our measurements confirm the presence of I=1 ortho-hydrogen at low pressures, above 70 GPa, where inter- and intramolecular distances become comparable, we observe a crossover in the nuclear spin statistics from a spin-1 quadrupolar to a spin-1/2 dipolar system, evidencing the loss of spin isomer distinction. These observations represent a unique case of a nuclear spin crossover phenomenon in quantum solids.
△ Less
Submitted 24 July, 2020;
originally announced July 2020.
-
Accurate photon echo timing by optical freezing of exciton dephasing and rephasing in quantum dots
Authors:
A. N. Kosarev,
H. Rose,
S. V. Poltavtsev,
M. Reichelt,
C. Schneider,
M. Kamp,
S. Hoefling,
M. Bayer,
T. Meier,
I. A. Akimov
Abstract:
Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time i…
▽ More
Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a novel concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2pi area. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
△ Less
Submitted 9 June, 2020;
originally announced June 2020.
-
Metallic Hydrogen Sublattice and Proton Mobility in Copper Hydride at High Pressure
Authors:
Thomas Meier,
Florian Trybel,
Giacomo Criniti,
Dominique Laniel,
Saiana Khandarkhaeva,
Egor Koemets,
Timofey Fedotenko,
Konstantin Glazyrin,
Michael Hanfland,
Gerd Steinle-Neumann,
Natalia Dubrovinskaia,
Leonid Dubrovinsky
Abstract:
Atomic and electronic structures of Cu2H and CuH have been investigated by high pressure NMR spectroscopy, X-ray diffraction and ab-initio calculations. Metallic Cu2H was synthesized at a pressure of 40 GPa, and semi-metallic CuH at 90 GPa, found stable up to 160 GPa. Experiments and computations suggest the formation of a metallic 1H-sublattice as well as a high 1H mobility of ~10-7 cm2/s in Cu2H…
▽ More
Atomic and electronic structures of Cu2H and CuH have been investigated by high pressure NMR spectroscopy, X-ray diffraction and ab-initio calculations. Metallic Cu2H was synthesized at a pressure of 40 GPa, and semi-metallic CuH at 90 GPa, found stable up to 160 GPa. Experiments and computations suggest the formation of a metallic 1H-sublattice as well as a high 1H mobility of ~10-7 cm2/s in Cu2H. Comparison of Cu2H and FeH data suggests that deviations from Fermi gas behavior, formation of conductive hydrogen networks, and high 1H mobility could be common features of metal hydrides.
△ Less
Submitted 8 April, 2020;
originally announced April 2020.
-
Realization of all-optical vortex switching in exciton-polariton condensates
Authors:
Xuekai Ma,
Bernd Berger,
Marc Assmann,
Rodislav Driben,
Torsten Meier,
Christian Schneider,
Sven Höfling,
Stefan Schumacher
Abstract:
Vortices are topological objects representing the circular motion of a fluid. With their additional degree of freedom, the 'vorticity', they have been widely investigated in many physical systems and different materials for fundamental interest and for applications in data storage and information processing. Vortices have also been observed in non-equilibrium exciton-polariton condensates in plana…
▽ More
Vortices are topological objects representing the circular motion of a fluid. With their additional degree of freedom, the 'vorticity', they have been widely investigated in many physical systems and different materials for fundamental interest and for applications in data storage and information processing. Vortices have also been observed in non-equilibrium exciton-polariton condensates in planar semiconductor microcavities. There they appear spontaneously or can be created and pinned in space using ring-shaped optical excitation profiles. However, using the vortex state for information processing not only requires creation of a vortex but also efficient control over the vortex after its creation. Here we demonstrate a simple approach to control and switch a localized polariton vortex between opposite states. In our scheme, both the optical control of vorticity and its detection through the orbital angular momentum of the emitted light are implemented in a robust and practical manner.
△ Less
Submitted 6 July, 2019;
originally announced July 2019.
-
Pressure induced Hydrogen-Hydrogen interaction in metallic FeH revealed by NMR
Authors:
Thomas Meier,
Florian Trybel,
Saiana Khandarkhaeva,
Gerd Steinle-Neumann,
Stella Chariton,
Timofey Fedotenko,
Sylvain Petitgirard,
Michael Hanfland,
Konstantin Glazyrin,
Natalia Dubrovinskaia,
Leonid Dubrovinsky
Abstract:
Knowledge of the behavior of hydrogen in metal hydrides is the key for understanding their electronic properties. So far, no experimental methods exist to access these properties beyond 100 GPa, where high-Tc superconductivity emerges. Here, we present an 1H-NMR study of cubic FeH up to 200GPa. We observe a distinct deviation from the ideal metallic behavior between 64 and 110 GPa that suggests pr…
▽ More
Knowledge of the behavior of hydrogen in metal hydrides is the key for understanding their electronic properties. So far, no experimental methods exist to access these properties beyond 100 GPa, where high-Tc superconductivity emerges. Here, we present an 1H-NMR study of cubic FeH up to 200GPa. We observe a distinct deviation from the ideal metallic behavior between 64 and 110 GPa that suggests pressure-induced H-H interactions. Accompanying ab-initio calculations support this interpretation, as they reveal the formation of an intercalating sublattice of electron density, which enhances the hydrogen contribution to the electronic density of states at the Fermi level. This study shows that pressure induced H-H interactions can occur in metal hydrides at much lower compression and larger H-H distances than previously thought and stimulates an alternative pathway in the search for novel high-temperature superconductors.
△ Less
Submitted 8 February, 2019;
originally announced February 2019.
-
Higher-order contributions and non-perturbative effects in the non-degenerate nonlinear optical absorption of direct-gap semiconductors
Authors:
W. -R. Hannes,
T. Meier
Abstract:
The semiconductor Bloch equations for a two-band model including inter- and intraband excitation are used to study the nonlinear absorption of single and multiple light pulses by direct-gap semiconductors. For a consistent analysis the contributions to the absorption originating from both the interband polarization and the intraband current need to be included. In the Bloch equation approach these…
▽ More
The semiconductor Bloch equations for a two-band model including inter- and intraband excitation are used to study the nonlinear absorption of single and multiple light pulses by direct-gap semiconductors. For a consistent analysis the contributions to the absorption originating from both the interband polarization and the intraband current need to be included. In the Bloch equation approach theses contributions as well as different excitation pathways in terms of sequences of inter- and intraband excitations can be evaluated separately which allows for a transparent analysis, the identification of the dominant terms, and analyzing their dependence on the excitation conditions. In the perturbative regime, we obtain analytical expressions for the multi-photon absorption coefficients for continuous-wave excitation. These results are shown to agree well with numerical results for short pulses and/or finite dephasing and relaxation times and we confirm the previously predicted strong enhancement of two-photon absorption for non-degenerate conditions for pulsed excitation. We discuss the dependencies on the light frequencies, initial band populations, and the time delay between the pulses. The frequency dependence of the two-photon absorption coefficient for non-degenerate excitation is evaluated perturbatively in third-order. The higher-order contributions to the optical absorption include three- and four-photon absorption and show a rich frequency dependence including negative regions and dispersive lineshapes. Non-perturbative solutions of the Bloch equations demonstrate a strongly non-monotonous behavior of the intensity-dependent optical absorption for a single incident pulse and in a pump-probe set-up.
△ Less
Submitted 21 December, 2018;
originally announced December 2018.
-
Observation of Nuclear Quantum Effects and Hydrogen Bond Symmetrisation in High Pressure Ice
Authors:
Thomas Meier,
Sylvain Petitgirard,
Saiana Khandarkhaeva,
Leonid Dubrovinsky
Abstract:
Hydrogen bond symmetrisations in H-bonded systems triggered by pressure induced nuclear quantum effects (NQEs) is a long-known concept1 but experimental evidences in high-pressure ices have remained elusive with conventional methods2,3. Theoretical works predicted quantum-mechanical tunneling of protons within water ices to occur at pressures above 30 GPa and the H-bond symmetrisation transition a…
▽ More
Hydrogen bond symmetrisations in H-bonded systems triggered by pressure induced nuclear quantum effects (NQEs) is a long-known concept1 but experimental evidences in high-pressure ices have remained elusive with conventional methods2,3. Theoretical works predicted quantum-mechanical tunneling of protons within water ices to occur at pressures above 30 GPa and the H-bond symmetrisation transition above 60 GPa4. Here, we used 1H-NMR on high-pressure ice up to 90 GPa, and demonstrate that NQEs govern the behavior of the hydrogen bonded protons in ice VII already at significantly lower pressures than previously expected. A pronounced tunneling mode was found to be present up to the highest pressures of 90 GPa, well into the stability field of ice X, where NQEs are not anticipated in a fully symmetrized H-bond network. We found two distinct transitions in the NMR shift data at about 20 GPa and 75 GPa attributed to the step-wise symmetrization of the H-bond (HB), with high-barrier H-Bonds (HBHB) to low-barrier H-bonds (LBHB) and LBHB to symmetric H-bonds (SHB) respectively. These transitions could have major implication on the physical properties of high-pressure ices and planetary interior models. NQEs observed in this chemically simple system over a wide pressure range could prove to be useful in designing a new generation of electronic devices exploiting protonic tunneling.
△ Less
Submitted 19 March, 2018;
originally announced March 2018.
-
Observation and uses of position-space Bloch oscillations in an ultracold gas
Authors:
Zachary A. Geiger,
Kurt M. Fujiwara,
Kevin Singh,
Ruwan Senaratne,
Shankari V. Rajagopal,
Mikhail Lipatov,
Toshihiko Shimasaki,
Rodislav Driben,
Vladimir V. Konotop,
Torsten Meier,
David M. Weld
Abstract:
We report the direct observation and characterization of position-space Bloch oscillations using an ultracold gas in a tilted optical lattice. While Bloch oscillations in momentum space are a common feature of optical lattice experiments, the real-space center-of-mass dynamics are typically too small to resolve. Tuning into the regime of rapid tunneling and weak force, we observe real-space Bloch…
▽ More
We report the direct observation and characterization of position-space Bloch oscillations using an ultracold gas in a tilted optical lattice. While Bloch oscillations in momentum space are a common feature of optical lattice experiments, the real-space center-of-mass dynamics are typically too small to resolve. Tuning into the regime of rapid tunneling and weak force, we observe real-space Bloch oscillation amplitudes of hundreds of lattice sites, in both ground and excited bands. We demonstrate two unique capabilities enabled by tracking of Bloch dynamics in position space: measurement of the full position-momentum phase-space evolution during a Bloch cycle, and direct imaging of the lattice band structure. These techniques, along with the ability to exert long-distance coherent control of quantum gases without modulation, may open up new possibilities for quantum control and metrology.
△ Less
Submitted 6 March, 2018;
originally announced March 2018.
-
Conformation And Mechanical Response of Spray Deposited Single Strand DNA on Gold
Authors:
Remy Pawlak,
J. G. Vilhena,
Antoine Hinaut,
Tobias Meier,
Thilo Glatzel,
Alexis Baratoff,
Fernando Moreno-Herrero,
Enrico Gnecco,
Ruben Perez,
Ernst Meyer
Abstract:
Single molecule force spectroscopy of DNA strands adsorbed at surfaces is a powerful technique used in air or liquid environments to quantify their mechanical properties. Although the force responses are limited to unfolding events so far, single base detection might be possible in more drastic cleanliness conditions such as ultra high vacuum. Here, we report on high resolution imaging and pulling…
▽ More
Single molecule force spectroscopy of DNA strands adsorbed at surfaces is a powerful technique used in air or liquid environments to quantify their mechanical properties. Although the force responses are limited to unfolding events so far, single base detection might be possible in more drastic cleanliness conditions such as ultra high vacuum. Here, we report on high resolution imaging and pulling attempts at low temperature (5K) of a single strand DNA (ssDNA) molecules composed of 20 cytosine bases adsorbed on Au(111) by scanning probe microscopy and numerical calculations. Using electrospray deposition technique, the ssDNA were successfully transferred from solution onto a surface kept in ultra high vacuum. Real space characterizations reveal that the ssDNA have an amorphous structure on gold in agreement with numerical calculations. Subsequent substrate annealing promotes the desorption of solvent molecules, DNA as individual molecules as well as the formation of DNA self assemblies. Furthermore, pulling experiments by force spectroscopy have been conducted to measure the mechanical response of the ssDNA while detaching. A periodic pattern of 0.2 to 0.3nm is observed in the force curve which arises from the stick slip of single nucleotide bases over the gold. Although an intra molecular response is obtained in the force curve, a clear distinction of each nucleotide detachment is not possible due the complex structure of ssDNA adsorbed on gold.
△ Less
Submitted 5 April, 2018; v1 submitted 10 September, 2017;
originally announced September 2017.
-
Anisotropic Excitons and their Contributions to Shift Current Transients in Bulk GaAs
Authors:
Reinold Podzimski,
Huynh Thanh Duc,
Torsten Meier
Abstract:
Shift current transient are obtained for near band gap excitation of bulk GaAs by numerical solutions of the semiconductor Bloch equations in a basis obtained from a 14 band k.p model of the band structure. This approach provides a transparent description of the optically induced excitations in terms of interband, intersubband, and intraband excitations which enables a clear distinction between di…
▽ More
Shift current transient are obtained for near band gap excitation of bulk GaAs by numerical solutions of the semiconductor Bloch equations in a basis obtained from a 14 band k.p model of the band structure. This approach provides a transparent description of the optically induced excitations in terms of interband, intersubband, and intraband excitations which enables a clear distinction between different contributions to the shift current transients and fully includes resonant as well as off-resonant processes. Using a geodesic grid in reciprocal space in our numerical solutions, we are able to include the electron-hole Coulomb attraction in combination with our anisotropic three-dimensional band structure. We obtain an excitonic absorption peak and an enhancement of the continuum absorption and demonstrate that the excitonic wave function contains a significant amount of anisotropy. Optical excitation at the excitonic resonance generates shift current transients of significant strength, however, due to the electron-hole attraction the shift distance is smaller than for above band gap excitation. We thus demonstrate that our approach is able to provide important information on the ultrafast electron dynamics on the atomic scale.
△ Less
Submitted 28 August, 2017;
originally announced August 2017.
-
Towards integrated superconducting detectors on lithium niobate waveguides
Authors:
Jan Philipp Höpker,
Moritz Bartnick,
Evan Meyer-Scott,
Frederik Thiele,
Stephan Krapick,
Nicola Montaut,
Matteo Santandrea,
Harald Herrmann,
Sebastian Lengeling,
Raimund Ricken,
Viktor Quiring,
Torsten Meier,
Adriana Lita,
Varun Verma,
Thomas Gerrits,
Sae Woo Nam,
Christine Silberhorn,
Tim J. Bartley
Abstract:
Superconducting detectors are now well-established tools for low-light optics, and in particular quantum optics, boasting high-efficiency, fast response and low noise. Similarly, lithium niobate is an important platform for integrated optics given its high second-order nonlinearity, used for high-speed electro-optic modulation and polarization conversion, as well as frequency conversion and source…
▽ More
Superconducting detectors are now well-established tools for low-light optics, and in particular quantum optics, boasting high-efficiency, fast response and low noise. Similarly, lithium niobate is an important platform for integrated optics given its high second-order nonlinearity, used for high-speed electro-optic modulation and polarization conversion, as well as frequency conversion and sources of quantum light. Combining these technologies addresses the requirements for a single platform capable of generating, manipulating and measuring quantum light in many degrees of freedom, in a compact and potentially scalable manner. We will report on progress integrating tungsten transition-edge sensors (TESs) and amorphous tungsten silicide superconducting nanowire single-photon detectors (SNSPDs) on titanium in-diffused lithium niobate waveguides. The travelling-wave design couples the evanescent field from the waveguides into the superconducting absorber. We will report on simulations and measurements of the absorption, which we can characterize at room temperature prior to cooling down the devices. Independently, we show how the detectors respond to flood illumination, normally incident on the devices, demonstrating their functionality.
△ Less
Submitted 18 August, 2017;
originally announced August 2017.
-
Damping of Rabi oscillations in intensity-dependent photon echoes from exciton complexes in a CdTe/(Cd,Mg)Te single quantum well
Authors:
S. V. Poltavtsev,
M. Reichelt,
I. A. Akimov,
G. Karczewski,
M. Wiater,
T. Wojtowicz,
D. R. Yakovlev,
T. Meier,
M. Bayer
Abstract:
We study Rabi oscillations detected in the coherent optical response from various exciton complexes in a 20~nm-thick CdTe/(Cd,Mg)Te quantum well using time-resolved photon echoes. In order to evaluate the role of exciton localization and inhomogeneous broadening we use selective excitation with spectrally narrow ps-pulses. We demonstrate that the transient profile of the photon echo from the local…
▽ More
We study Rabi oscillations detected in the coherent optical response from various exciton complexes in a 20~nm-thick CdTe/(Cd,Mg)Te quantum well using time-resolved photon echoes. In order to evaluate the role of exciton localization and inhomogeneous broadening we use selective excitation with spectrally narrow ps-pulses. We demonstrate that the transient profile of the photon echo from the localized trion (X$^-$) and the donor-bound exciton (D$^0$X) transitions strongly depends on the strength of the first pulse. It acquires a non-Gaussian shape and experiences significant advancement for pulse areas larger than $π$ due to non-negligible inhomogeneity-induced dephasing of the oscillators during the optical excitation. Next, we observe that an increase of the area of either the first (excitation) or the second (rephasing) pulse leads to a significant damping of the photon echo signal, which is strongest for the neutral excitons and less pronounced for the donor-bound exciton complex (D$^0$X). The measurements are analyzed using a theoretical model based on the optical Bloch equations which accounts for the inhomogeneity of optical transitions in order to reproduce the complex shape of the photon echo transients. In addition, the spreading of Rabi frequencies within the ensemble due to the spatial variation of the intensity of the focused Gaussian beams and excitation-induced dephasing are required to explain the fading and damping of Rabi oscillations. By analyzing the results of the simulation for the X$^-$ and the D$^0$X complexes we are able to establish a correlation between the degree of localization and the transition dipole moments determined as $μ($X$^-$)=73~D and $μ($D$^0$X)=58~D.
△ Less
Submitted 16 June, 2017;
originally announced June 2017.
-
Magnetic Flux Tailoring through Lenz Lenses in Toroidal Diamond Indenter Cells: A New Pathway to High Pressure Nuclear Magnetic Resonance
Authors:
Thomas Meier,
Nan Wang,
Dario Mager,
Jan G. Korvink,
Sylvain Petigirard,
Leonid Dubrovinsky
Abstract:
A new pathway to nuclear magnetic resonance spectroscopy in high pressure diamond anvil cells is introduced, using inductively coupled broadband passive electro-magnetic lenses to locally amplify the magnetic flux at the isolated sample, leading to an increase in sensitivity. The lenses are adopted for the geometrical restrictions imposed by a toroidal diamond indenter cell, and yield high signal-…
▽ More
A new pathway to nuclear magnetic resonance spectroscopy in high pressure diamond anvil cells is introduced, using inductively coupled broadband passive electro-magnetic lenses to locally amplify the magnetic flux at the isolated sample, leading to an increase in sensitivity. The lenses are adopted for the geometrical restrictions imposed by a toroidal diamond indenter cell, and yield high signal-to-noise ratios at pressures as high as 72 GPa, at initial sample volumes of only 230 pl. The corresponding levels of detection, LODt, are found to be up to four orders of magnitude lower compared to formerly used solenoidal micro-coils in diamond anvil cells, as shown by Proton-NMR measurements on paraffin oil. This approach opens up the field of ultra-high pressure sciences for one of the most versatile spectroscopic methods available in a pressure range unprecedended up to now.
△ Less
Submitted 24 May, 2017;
originally announced June 2017.
-
Entropy-limited topological protection of skyrmions
Authors:
J. Wild,
T. N. G. Meier,
S. Pöllath,
M. Kronseder,
A. Bauer,
A. Chacon,
M. Halder,
M. Schowalter,
A. Rosenauer,
J. Zweck,
J. Müller,
A. Rosch,
C. Pfleiderer,
C. H. Back
Abstract:
Magnetic skyrmions are topologically protected whirls that decay through singular magnetic configurations known as Bloch points. We have used Lorentz transmission electron microscopy to infer the energetics associated with the topological decay of magnetic skyrmions far from equilibrium in the chiral magnet Fe$_{1-x}$Co$_x$Si. We observed that the life time $τ$ of the skyrmions depends exponential…
▽ More
Magnetic skyrmions are topologically protected whirls that decay through singular magnetic configurations known as Bloch points. We have used Lorentz transmission electron microscopy to infer the energetics associated with the topological decay of magnetic skyrmions far from equilibrium in the chiral magnet Fe$_{1-x}$Co$_x$Si. We observed that the life time $τ$ of the skyrmions depends exponentially on temperature, $τ\sim τ_0 \, e^{ΔE/k_B T}$. The prefactor $τ_0$ of this Arrhenius law changes by more than 30 orders of magnitude for small changes of magnetic field reflecting a substantial reduction of the life time of skyrmions by entropic effects and thus an extreme case of enthalpy-entropy compensation. Such compensation effects, being well-known across many different scientific disciplines, affect topological transitions and thus topological protection on an unprecedented level.
△ Less
Submitted 9 May, 2017; v1 submitted 4 May, 2017;
originally announced May 2017.
-
Dynamical defects in rotating magnetic skyrmion lattices
Authors:
S. Pöllath,
J. Wild,
L. Heinen,
T. N. G. Meier,
M. Kronseder,
L. Tutsch,
A. Bauer,
H. Berger,
C. Pfleiderer,
J. Zweck,
A. Rosch,
C. H. Back
Abstract:
The chiral magnet Cu$_{2}$OSeO$_{3}$ hosts a skyrmion lattice, that may be equivalently described as a superposition of plane waves or lattice of particle-like topological objects. A thermal gradient may break up the skyrmion lattice and induce rotating domains raising the question which of these scenarios better describes the violent dynamics at the domain boundaries. Here we show that in an inho…
▽ More
The chiral magnet Cu$_{2}$OSeO$_{3}$ hosts a skyrmion lattice, that may be equivalently described as a superposition of plane waves or lattice of particle-like topological objects. A thermal gradient may break up the skyrmion lattice and induce rotating domains raising the question which of these scenarios better describes the violent dynamics at the domain boundaries. Here we show that in an inhomogeneous temperature gradient caused by illumination in a Lorentz Transmission Electron Microscope different parts of the skyrmion lattice can be set into motion with different angular velocities. Tracking the time dependence we show that the constant rearrangement of domain walls is governed by dynamic 5-7 defects arranging into lines. An analysis of the associated defect density is described by Frank's equation and agrees well with classical 2D-Monte Carlo simulations. Fluctuations of boundaries show surge-like rearrangement of skyrmion clusters driven by defect rearrangement consistent with simulations treating skyrmions as point particles. Our findings underline the particle character of the skyrmion.
△ Less
Submitted 3 May, 2017; v1 submitted 24 April, 2017;
originally announced April 2017.
-
Transient photon echoes from donor-bound excitons in ZnO epitaxial layers
Authors:
S. V. Poltavtsev,
A. N. Kosarev,
I. A. Akimov,
D. R. Yakovlev,
S. Sadofev,
J. Puls,
S. P. Hoffmann,
M. Albert,
C. Meier,
T. Meier,
M. Bayer
Abstract:
The coherent optical response from 140~nm and 65~nm thick ZnO epitaxial layers is studied using transient four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D$^0$X$_\text{A}$) at temperature of 1.8~K we evaluate optical coherence times $T_2=33-50$~p…
▽ More
The coherent optical response from 140~nm and 65~nm thick ZnO epitaxial layers is studied using transient four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D$^0$X$_\text{A}$) at temperature of 1.8~K we evaluate optical coherence times $T_2=33-50$~ps corresponding to homogeneous linewidths of $13-19~μ$eV, about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is determined mainly by the population decay with time $T_1=30-40$~ps, while pure dephasing is negligible in the studied high quality samples even for strong optical excitation. Temperature increase leads to a significant shortening of $T_2$ due to interaction with acoustic phonons. In contrast, the loss of coherence of the donor-bound B exciton (D$^0$X$_\text{B}$) is significantly faster ($T_2=3.6$~ps) and governed by pure dephasing processes.
△ Less
Submitted 16 February, 2017;
originally announced February 2017.
-
High resolution two-dimensional optical spectroscopy of electron spins
Authors:
M. Salewski,
S. V. Poltavtsev,
I. A. Yugova,
G. Karczewski,
M. Wiater,
T. Wojtowicz,
D. R. Yakovlev,
I. A. Akimov,
T. Meier,
M. Bayer
Abstract:
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses has still remained a chal…
▽ More
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses has still remained a challenge. Here, we analyze two-dimensional Fourier spectra for resonant optical excitation of resident electrons to localized trions or donor-bound excitons in semiconductor nanostructures subject to a transverse magnetic field. Particular attention is devoted to Raman coherence spectra which allow one to accurately evaluate tiny splittings of the electron ground state and to determine the relaxation times in the electron spin ensemble. A stimulated step-like Raman process induced by a sequence of two laser pulses creates a coherent superposition of the ground state doublet which can be retrieved only optically due to selective excitation of the same sub-ensemble with a third pulse. This provides the unique opportunity to distinguish between different complexes that are closely spaced in energy in an ensemble. The related experimental demonstration is based on photon echo measurements in an n-type CdTe/(Cd,Mg)Te quantum well structure detected by a heterodyne technique. The difference in the sub-$μ$eV range between the Zeeman splittings of donor-bound electrons and electrons localized at potential fluctuations can be resolved even though the homogeneous linewidth of the optical transitions is larger by two orders of magnitude.
△ Less
Submitted 17 August, 2017; v1 submitted 7 January, 2017;
originally announced January 2017.
-
Two-dimensional symbiotic solitons and vortices in binary condensates with attractive cross-species interaction
Authors:
Xuekai Ma,
Rodislav Driben,
Boris A. Malomed,
Torsten Meier,
Stefan Schumacher
Abstract:
We consider a two-dimensional (2D) two-component spinor system with cubic attraction between the components and intra-species self-repulsion, which may be realized in atomic Bose-Einstein condensates, as well as in a quasi-equilibrium condensate of microcavity polaritons. Including a 2D spatially periodic potential, which is necessary for the stabilization of the system against the critical collap…
▽ More
We consider a two-dimensional (2D) two-component spinor system with cubic attraction between the components and intra-species self-repulsion, which may be realized in atomic Bose-Einstein condensates, as well as in a quasi-equilibrium condensate of microcavity polaritons. Including a 2D spatially periodic potential, which is necessary for the stabilization of the system against the critical collapse, we use detailed numerical calculations and an analytical variational approximation (VA) to predict the existence and stability of several types of 2D symbiotic solitons in the spinor system. Stability ranges are found for symmetric and asymmetric symbiotic fundamental solitons and vortices, including hidden-vorticity (HV) modes, with opposite vorticities in the two components. The VA produces exceptionally accurate predictions for the fundamental solitons and vortices. The fundamental solitons, both symmetric and asymmetric ones, are completely stable, in either case when they exist as gap solitons or regular ones. The symmetric and asymmetric vortices are stable if the inter-component attraction is stronger than the intra-species repulsion, while the HV modes have their stability region in the opposite case.
△ Less
Submitted 13 September, 2016; v1 submitted 28 June, 2016;
originally announced June 2016.