Imprinting photon orbital angular momentum during laser-assisted photoemission from quantum wells.

We study theoretically the transfer of the light field orbital angular momentum (OAM) to propagating electrons upon photoemission from quantum well states. Irradiation with a Laguerre-Gaussian mode laser pulse elevates the quantum well state into a laser-dressed Volkov state that can be detected in an angular and energy-resolved manner while varying the characteristics of the driving fields. We derive the photoemission cross section for this process using the S-matrix theory and illustrate how the OAM is embodied in the photoelectron angular pattern with the aid of numerical calculations. The results point to a new type of time-resolved spectroscopy, in which the electronic orbital motion is addressed exclusively, with the potential for a new insight in spin-orbitally or orbitally coupled systems.

Band-Resolved Double Photoemission Spectroscopy on Correlated Valence Electron Pairs in Metals.

Correlated valence electrons in Ag and Cu are investigated using double photoemission spectroscopy driven by a high-order harmonic light source. Electron pairs consisting of two d electrons as well as pairs with one sp and one d electron are resolved in the two-dimensional energy spectrum. Surprisingly, the intensity ratio of sp-d to d-d pairs from Ag is 3 times higher than in the self-convoluted density of states. Our results directly show the band-resolved configurations of electron pairs in solids and emphasize a band-dependent picture for electron correlation even in these paradigmatic metals.

Photoluminescence of Nitrogen-Vacancy Centers by Ultraviolet One- and Two-Photon Excitation of Fluorescent Nanodiamonds.

Fluorescent nanodiamonds contain nitrogen-vacancy (NV) centers as quantum defects. When exposed to a continuous-wave 325 nm laser or a femtosecond 344 nm laser, the particles emit red fluorescence from NV0 centers at ∼620 nm. Power dependence measurements of the emission strength revealed a predominantly linear behavior at the laser peak intensity lower than 1 GW·cm-2, contributed mainly by photoexcitation of electrons from the valence band of diamond to the NV0 centers, followed by relaxation via electron-hole recombination. In the higher power regions, however, nonresonant two-photon interband excitation of the diamond matrix dominates the photoluminescence processes. Best fits of the experimental data to semiempirical models revealed an ionization coefficient of ∼1 cm-1 for the one-photon valence-to-defect excitation and a saturation intensity of 180 ± 60 GW·cm-2 for the two-photon interband excitation. The study provides new insight into the photoionization of NV0 centers and the interband excitation properties of diamond in the UV region.

Ultrafast coupled charge and spin dynamics in strongly correlated NiO.

Charge excitations across an electronic band gap play an important role in opto-electronics and light harvesting. In contrast to conventional semiconductors, studies of above-band-gap photoexcitations in strongly correlated materials are still in their infancy. Here we reveal the ultrafast dynamics controlled by Hund's physics in strongly correlated photoexcited NiO. By combining time-resolved two-photon photoemission experiments with state-of-the-art numerical calculations, an ultrafast (≲10 fs) relaxation due to Hund excitations and related photo-induced in-gap states are identified. Remarkably, the weight of these in-gap states displays long-lived coherent THz oscillations up to 2 ps at low temperature. The frequency of these oscillations corresponds to the strength of the antiferromagnetic superexchange interaction in NiO and their lifetime vanishes slightly above the Néel temperature. Numerical simulations of a two-band t-J model reveal that the THz oscillations originate from the interplay between local many-body excitations and antiferromagnetic spin correlations.

Electromagnetic Functionalization of Wide-Bandgap Dielectric Oxides by Boron Interstitial Doping.

A surge in interest of oxide-based materials is testimony for their potential utility in a wide array of device applications and offers a fascinating landscape for tuning the functional properties through a variety of physical and chemical parameters. In particular, selective electronic/defect doping has been demonstrated to be vital in tailoring novel functionalities, not existing in the bulk host oxides. Here, an extraordinary interstitial doping effect is demonstrated centered around a light element, boron (B). The host matrix is a novel composite system, made from discrete bulk LaAlO3 :LaBO3 compounds. The findings show a spontaneous ordering of the interstitial B cations within the host LaAlO3 lattices, and subsequent spin-polarized charge injection into the neighboring cations. This leads to a series of remarkable cation-dominated electrical switching and high-temperature ferromagnetism. Hence, the induced interstitial doping serves to transform a nonmagnetic insulating bulk oxide into a ferromagnetic ionic-electronic conductor. This unique interstitial B doping effect upon its control is proposed to be as a general route for extracting/modifying multifunctional properties in bulk oxides utilized in energy and spin-based applications.

Evaluation of dermal thermal damage by multiphoton autofluorescence and second-harmonic-generation microscopy.

We attempt to characterize the degree of skin thermal damage by using multiphoton microscopy to characterize dermal thermal damage. Our results show that dermal collagen and elastic fibers display different susceptibility to thermal injury. Morphologically, dermal collagen starts to denature at 60 degrees C while fracture and aggregation of elastic fibers do not occur until 65 degrees C. With increasing temperatures, the structures of both elastic and collagen fibers deteriorate. While second-harmonic-generation (SHG) imaging is helpful in identifying the denaturation temperature of collagen, autofluorescence (AF) imaging can help to identify the structural alternations of tissue at higher temperatures when SHG signals have decayed. We also employ a ratiometric approach based on the AF-to-SHG index of dermis (ASID) to characterize the degree of dermal thermal damage. Use of the ASID index can bypass the difficulty in analyzing inhomogeneous dermal fibers and show that dermal collagen starts to denature at 60 degrees C. Our results suggest that with additional developments, multiphoton microscopy has potential to be developed into an effective in vivo imaging technique to monitor and characterize dermal thermal damage.

Magnetic dichroism from optically excited quantum well states.

We demonstrate magnetic dichroism from optically excited states in two-photon photoemission. Using ultrathin cobalt films grown on Cu(001), we observe unoccupied quantum well states which give rise to a sizable intensity change in photoemission under magnetization reversal. The simultaneous comparison of both circular and linear magnetic dichroism in the same system permits us to check fundamental symmetry requirements and allows us to explicitly elucidate the common origin of both effects. Based on our observations we argue that the observed effect is related to spin-orbit coupling in the intermediate quantum well states.