The remagnetization process after ultrafast demagnetization can be described by relaxation mechanisms between the spin, electron, and lattice reservoirs. Thereby, collective spin excitations in form of spin waves and their angular momentum transfer play an important role on the longer timescales. In this work, we address the question whether the magnitude of demagnetization-the so-called quenching-affects the coherency and the phase of the excited spin waves.
View Article and Find Full Text PDFExcitons are realizations of a correlated many-particle wave function, specifically consisting of electrons and holes in an entangled state. Excitons occur widely in semiconductors and are dominant excitations in semiconducting organic and low-dimensional quantum materials. To efficiently harness the strong optical response and high tuneability of excitons in optoelectronics and in energy-transformation processes, access to the full wavefunction of the entangled state is critical, but has so far not been feasible.
View Article and Find Full Text PDFAltermagnets are an emerging elementary class of collinear magnets. Unlike ferromagnets, their distinct crystal symmetries inhibit magnetization while, unlike antiferromagnets, they promote strong spin polarization in the band structure. The corresponding unconventional mechanism of time-reversal symmetry breaking without magnetization in the electronic spectra has been regarded as a primary signature of altermagnetism but has not been experimentally visualized to date.
View Article and Find Full Text PDFWe design and experimentally demonstrate an optical switch based on the interference of plasmonic modes in whispering gallery mode (WGM) antennas. Simultaneous excitation of even and odd WGM modes, enabled by a small symmetry breaking via non-normal illumination, allows switching the plasmonic near field between opposite sides of the antenna, depending on the excitation wavelength used in a wavelength range of 60 nm centered around 790 nm. This proposed switching mechanism is experimentally demonstrated by combining photoemission electron microscopy (PEEM) with a tunable wavelength femtosecond laser source in the visible and infrared.
View Article and Find Full Text PDFThe discovery of the electrons' chiral induced spin selective transmission (CISS) through chiral molecules has opened the pathway for manipulating spin transport in nonmagnetic structures on the nanoscale. CISS has predominantly been explored in structurally helical molecules on surfaces, where the spin selectivity affects only the spin polarization of the electrons along their direction of propagation. Here, we demonstrate a spin selective electron transmission for the point-chiral molecule 3-methylcyclohexanone (3-MCHO) adsorbed on the chiral Cu(643) surface.
View Article and Find Full Text PDFThe strength of light-matter interaction in condensed matter is fundamentally linked to the orientation and oscillation strength of the materials' optical transition dipoles. Structurally anisotropic materials, e.g.
View Article and Find Full Text PDFThe prosperity and lifestyle of our society are very much governed by achievements in condensed matter physics, chemistry and materials science, because new products for sectors such as energy, the environment, health, mobility and information technology (IT) rely largely on improved or even new materials. Examples include solid-state lighting, touchscreens, batteries, implants, drug delivery and many more. The enormous amount of research data produced every day in these fields represents a gold mine of the twenty-first century.
View Article and Find Full Text PDFUnderstanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers.
View Article and Find Full Text PDFWe investigated the surface and bulk properties of the pristine (110) surface of silver using threshold photoemission by excitation with light of 5.9 eV. Using a momentum microscope, we identified two distinct transitions along the Γ[over ¯]Y[over ¯] direction of the crystal.
View Article and Find Full Text PDFOrbital angular momentum of light is a core feature in photonics. Its confinement to surfaces using plasmonics has unlocked many phenomena and potential applications. Here, we introduce the reflection from structural boundaries as a new degree of freedom to generate and control plasmonic orbital angular momentum.
View Article and Find Full Text PDFPhase transitions between different aggregate states are omnipresent in nature and technology. Conventionally, a crystalline phase melts upon heating as we use ice to cool a drink. Already in 1903, Gustav Tammann speculated about the opposite process, namely melting upon cooling.
View Article and Find Full Text PDFSurface plasmon polaritons carrying orbital angular momentum are of great fundamental and applied interest. However, common approaches for their generation are restricted to having a weak dependence on the properties of the plasmon-generating illumination, providing a limited degree of control over the amount of delivered orbital angular momentum. Here we experimentally show that by tailoring local and global geometries of vortex generators, a change in helicity of light imposes arbitrary large switching in the delivered plasmonic angular momentum.
View Article and Find Full Text PDFControlling self-assembled nanostructures on bulk insulators at room temperature is crucial towards the fabrication of future molecular devices, e.g., in the field of nanoelectronics, catalysis and sensor applications.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
October 2020
The high flexibility of organic molecules offers great potential for designing the optical properties of optically active materials for the next generation of optoelectronic and photonic applications. However, despite successful implementations of molecular materials in today's display and photovoltaic technology, many fundamental aspects of the light-to-charge conversion in molecular materials have still to be uncovered. Here, we focus on the ultrafast dynamics of optically excited excitons in C thin films depending on the molecular coverage and the light polarization of the optical excitation.
View Article and Find Full Text PDFWe use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS and graphene. This heterostructure combines the benefits of a direct-gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electrons remain in the WS layer.
View Article and Find Full Text PDFWe compare the decay of plasmons and "conventional" hot electrons within the same series of gold/metal oxide interfaces. We found an accelerated decay of hot electrons at gold-metal oxide interfaces with decreasing band gap of the oxide material. The decay is accelerated by the increased phase space for electron scattering caused by additional interfacial states.
View Article and Find Full Text PDFWe unravel the underlying near-field mechanism of the enhancement of the magneto-optical activity of bismuth-substituted yttrium iron garnet films (Bi:YIG) loaded with gold nanoparticles. The experimental results show that the embedded gold nanoparticles lead to a broadband enhancement of the magneto-optical activity with respect to the activity of the bare Bi:YIG films. Full vectorial near- and far-field simulations demonstrate that this broadband enhancement is the result of a magneto-optically enabled cross-talking of orthogonal localized plasmon resonances.
View Article and Find Full Text PDFHeusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, CoMnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs.
View Article and Find Full Text PDFOrganic photovoltaic devices operate by absorbing light and generating current. These two processes are governed by the optical and transport properties of the organic semiconductor. Despite their common microscopic origin-the electronic structure-disclosing their dynamical interplay is far from trivial.
View Article and Find Full Text PDFThe quest for a spin-polarized organic light-emitting diode (spin-OLED) is a common goal in the emerging fields of molecular electronics and spintronics. In this device, two ferromagnetic (FM) electrodes are used to enhance the electroluminescence intensity of the OLED through a magnetic control of the spin polarization of the injected carriers. The major difficulty is that the driving voltage of an OLED device exceeds a few volts, while spin injection in organic materials is only efficient at low voltages.
View Article and Find Full Text PDFThe successful implementation of nanoscale materials in next generation optoelectronic devices crucially depends on our ability to functionalize and design low dimensional materials according to the desired field of application. Recently, organic adsorbates have revealed an enormous potential to alter the occupied surface band structure of tunable materials by the formation of tailored molecule-surface bonds. Here, we extend this concept of adsorption-induced surface band structure engineering to the unoccupied part of the surface band structure.
View Article and Find Full Text PDFElectron-electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening.
View Article and Find Full Text PDFMagnetization dynamics on a femtosecond timescale has been observed for a huge variety of magnetic structures. However, the influence of different excitation photon energies has not been studied in detail yet. In our time-resolved magneto-optical Kerr effect setup we excite a Nickel bulk system with 1.
View Article and Find Full Text PDF