SearcharxivSearch

arXiv subjects

Paul Herrmann

Publications and source records attributed to Paul Herrmann.

6 recordsLinked to original sources

Nonlinear Circular Dichroism Reveals the Local Berry Curvature

Light-matter interactions are governed by conservation laws of energy and momentum. For harmonic generation in crystalline solids, energy conservation imposes that $m$ incoming photons with energy $\hbar \omega_0$ are combined to form one photon at energy $m\hbar \omega_0$. Linear momentum conservation governs phase matching, whereas angular momentum conservation connects the angular momentum carried by photons to the discrete rotational symmetry of the crystal lattice. As a consequence, circular harmonic generation exerts a torque on the lattice and, conversely, a macroscopic rotation of the crystal induces a nonlinear rotational Doppler shift. These cornerstone laws of nonlinear optics rely on macroscopic symmetry arguments, and therefore provide little insight into the microscopic origin of angular momentum transfer. Here we uncover a direct connection between angular momentum conservation in nonlinear optics and the electronic quantum geometry, by proving that the transferred angular momentum from light to the crystal is proportional to the local Berry curvature at one optical resonance. This relation is encoded in the nonlinear harmonic circular dichroism, which we measure experimentally in an atomically thin semiconductor. With this, we extend our understanding of nonlinear optics, and we establish a method for the all-optical control and read-out of the local Berry curvature.

cond-mat.mes-hall

Direct measurement of broken time-reversal symmetry in centrosymmetric and non-centrosymmetric atomically thin crystals with nonlinear Kerr rotation

Time-reversal symmetry, together with space-inversion symmetry, is one of the defining properties of crystals, underlying phenomena such as magnetism, topology and non-trivial spin textures. Transition metal dichalcogenides (TMDs) provide an excellent tunable model system to study the interplay between time-reversal and space-inversion symmetry, since both can be engineered on demand by tuning the number of layers and via all-optical bandgap modulation. In this work, we modulate and study time-reversal symmetry using third harmonic Kerr rotation in mono- and bilayer TMDs. By illuminating the samples with elliptically polarized light, we achieve spin-selective bandgap modulation and consequent breaking of time-reversal symmetry. The reduced symmetry modifies the nonlinear susceptibility tensor, causing a rotation of the emitted third harmonic polarization. With this method, we are able to probe broken time-reversal symmetry in both non-centrosymmetric (monolayer) and centrosymmetric (bilayer) crystals. Furthermore, we discuss how the detected third harmonic rotation angle directly links to the spin-valley locking in monolayer TMDs and to the spin-valley-layer locking in bilayer TMDs. Thus, our results define a powerful approach to study broken time-reversal symmetry in crystals regardless of space-inversion symmetry, and shed light on the spin, valley and layer coupling of atomically thin semiconductors.

physics.optics

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci

Valley Polarization-Electric Dipole Interference and Nonlinear Chiral Selection Rules in Monolayer WSe$_2$

In monolayer transition metal dichalcogenides time-reversal symmetry, combined with space-inversion symmetry, defines the spin-valley degree of freedom. As such, engineering and control of time-reversal symmetry by optical or magnetic fields constitutes the foundation of valleytronics. Here, we propose a new approach for the detection of broken time-reversal symmetry and valley polarization in monolayer WSe$_2$ based on second harmonic generation. Our method can selectively and simultaneously generate and detect a valley polarization at the $\pm K$ valleys of transition metal dichalcogenides at room temperature. Furthermore, it allows to measure the interference between the real and imaginary parts of the intrinsic (electric dipole) and valley terms of the second order nonlinear susceptibility. This work demonstrates the potential and unique capabilities of nonlinear optics as a probe of broken time-reversal symmetry and as a tool for ultrafast and non-destructive valleytronic operations.

physics.optics

Nonlinear Dispersion Relation and Out-of-Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long-lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, we study second and third harmonic generation in MoSSe and WSSe Janus monolayers. We use polarization-resolved spectroscopy to map the full second-order susceptibility tensor of MoSSe, including its out-of-plane components. In addition, we measure the effective third-order susceptibility, and the second-order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe at room and cryogenic temperatures. Our work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next-generation on-chip multifaceted photonic devices.

cond-mat.mes-hall

Discrete dispersion scan setup for measuring few-cycle laser pulses in the mid-infrared

In this work, we demonstrate a discrete dispersion scan scheme using a low number of flat windows to vary the dispersion of laser pulses in discrete steps. Monte Carlo simulations indicate that the pulse duration can be retrieved accurately with less than 10 dispersion steps, which we verify experimentally by measuring few-cycle pulses and material dispersion curves at 3 and 10 micrometer wavelength. This minimal measuring scheme using only five optical components without the need for high-precision positioners and interferometric alignment can be readily implemented in many wavelength ranges and situations.

physics.optics