Deeply nonlinear excitation of self-normalized short spin waves.

Spin waves are ideal candidates for wave-based computing, but the construction of magnetic circuits is blocked by a lack of an efficient mechanism to excite long-running exchange spin waves with normalized amplitudes. Here, we solve the challenge by exploiting a deeply nonlinear phenomenon for forward volume spin waves in 200-nm-wide nanoscale waveguides and validate our concept using microfocused Brillouin light scattering spectroscopy. An unprecedented nonlinear frequency shift of more than 2 GHz is achieved, corresponding to a magnetization precession angle of 55° and enabling the excitation of spin waves with wavelengths down to 200 nm. The amplitude of the excited spin waves is constant and independent of the input microwave power due to the self-locking nonlinear shift, enabling robust adjustment of the spin-wave amplitudes in future on-chip magnonic integrated circuits.

Control of the Bose-Einstein Condensation of Magnons by the Spin Hall Effect.

Previously, it has been shown that rapid cooling of yttrium-iron-garnet-platinum nanostructures, preheated by an electric current sent through the Pt layer, leads to overpopulation of a magnon gas and to subsequent formation of a Bose-Einstein condensate (BEC) of magnons. The spin Hall effect (SHE), which creates a spin-polarized current in the Pt layer, can inject or annihilate magnons depending on the electric current and applied field orientations. Here we demonstrate that the injection or annihilation of magnons via the SHE can prevent or promote the formation of a rapid cooling-induced magnon BEC. Depending on the current polarity, a change in the BEC threshold of -8% and +6% was detected. These findings demonstrate a new method to control macroscopic quantum states, paving the way for their application in spintronic devices.

Bose-Einstein condensation of quasiparticles by rapid cooling.

The fundamental phenomenon of Bose-Einstein condensation has been observed in different systems of real particles and quasiparticles. The condensation of real particles is achieved through a major reduction in temperature, while for quasiparticles, a mechanism of external injection of bosons by irradiation is required. Here, we present a new and universal approach to enable Bose-Einstein condensation of quasiparticles and to corroborate it experimentally by using magnons as the Bose-particle model system. The critical point to this approach is the introduction of a disequilibrium of magnons with the phonon bath. After heating to an elevated temperature, a sudden decrease in the temperature of the phonons, which is approximately instant on the time scales of the magnon system, results in a large excess of incoherent magnons. The consequent spectral redistribution of these magnons triggers the Bose-Einstein condensation.

Propagation of Spin-Wave Packets in Individual Nanosized Yttrium Iron Garnet Magnonic Conduits.

Modern-day CMOS-based computation technology is reaching its fundamental limitations. The emerging field of magnonics, which utilizes spin waves for data transport and processing, proposes a promising path to overcome these limitations. Different devices have been demonstrated recently on the macro- and microscale, but the feasibility of the magnonics approach essentially relies on the scalability of the structure feature size down to the extent of a few 10 nm, which are typical sizes for the established CMOS technology. Here, we present a study of propagating spin-wave packets in individual yttrium iron garnet (YIG) conduits with lateral dimensions down to 50 nm. Space and time-resolved microfocused Brillouin-light-scattering (BLS) spectroscopy is used to characterize the YIG nanostructures and measure the spin-wave decay length and group velocity directly. The revealed magnon transport at the scale comparable to the scale of CMOS proves the general feasibility of magnon-based data processing.

Electronic states of o-nitrobenzaldehyde: a combined experimental and theoretical study.

The experimental UV/vis absorption spectrum of ortho-nitrobenzaldehyde (o-NBA) has been assigned by means of MS-CASPT2/CASSCF, TD-DFT, and RI-CC2 theoretical computations. Additional information on the nature of the absorbing bands was obtained by comparing the o-NBA spectrum with that of related compounds, as, e.g., nitrobenzene and benzaldehyde. For wavelengths larger than approximately 280 nm, the absorption spectrum of o-NBA is dominated by a series of weak n pi* absorptions from the NO2 and CHO groups. These weak transitions are followed in energy by a more intense band, peaking at 250 nm and arising from charge transfer pi pi* excitations involving mainly benzene and nitro orbitals. Finally, the most intense band centered at 220 nm has its origin in the overlap of two different absorptions: the first one localized in the NO2 substituent and the second one arising from a charge transfer excitation involving the NO2 and the CHO fragments, respectively.

On the mechanism of intramolecular sensitization of photocleavage of the 2-(2-nitrophenyl)propoxycarbonyl (NPPOC) protecting group.

A spectroscopic study of a variety of covalently linked thioxanthone(TX)-linker-2-(2-nitrophenyl)propoxycarbonyl(NPPOC)-substrate conjugates is presented. Herein, the TX chromophore functions as an intramolecular sensitizer to the NPPOC moiety, a photolabile protecting group used in photolithographic DNA chip synthesis. The rate of electronic energy transfer between TX and NPPOC was quantified by means of stationary fluorescence as well as nanosecond and femtosecond time-resolved laser spectroscopy. A dual mechanism of triplet-triplet energy transfer has been observed comprising a slower mechanism involving the T1(pipi*) state of TX with linker-length-dependent time constants longer than 20 ns and a fast mechanism with linker-length-dependent time constants shorter than 3 ns. Evidence is provided that the latter mechanism is due to energy transfer from the T2(npi*) state which is in fast equilibrium with the fluorescent S1(pipi*) state. In the case of direct linkage between the aromatic rings of TX and NPPOC, the spectroscopic properties are indicative of one united chromophore which, however, still shows the typical NPPOC cleavage reaction triggered by intramolecular hydrogen atom transfer to the nitro group.

Photochemical Z-->E isomerization of a hemithioindigo/hemistilbene omega-amino acid.

The molecule HTI, which combines hemithioindigo and hemistilbene molecular parts, allows reversible switching between two isomeric states. Photochromic behaviour of the HTI molecule is observed by irradiation with UV/Vis light. The photochemical reaction, a Z/E isomerization around the central double bond connecting the two molecular parts, is investigated by transient absorption and emission spectroscopy. For a special HTI molecule, namely, an omega-amino acid, the Z-->E isomerization process occurs on a timescale of 30 ps. In the course of the reaction fast processes on the 1-10 ps timescale are observed which point to motions of the molecule on the potential-energy surface of the excited state. The combination of transient absorption experiments in the visible spectral range with time-resolved fluorescence and infrared measurements reveal a photochemical pathway with three intermediate states. Together with a theoretical modelling procedure the experiments point to a sequential reaction scheme and give indications of the nature of the involved intermediates.

Comparing a photoinduced pericyclic ring opening and closure: differences in the excited state pathways.

The photochromicity of fulgimides rests on the existence of open (E) and closed ring (C) isomers. As predicted by the Woodward-Hoffmann rules both isomers can photochemically be interconverted. This interconversion has been studied by femtosecond fluorescence and transient absorption spectroscopy. For either direction (E --> C cyclization and C --> E cycloreversion) a biphasic fluorescence decay on the 0.1-1 ps time scale is observed. The longer time constants of the decays equal the formation times of the photoproducts. The time constants retrieved (0.06 and 0.4 ps for E --> C, 0.09 and 2.4 ps for C --> E) and the associated spectral signatures differ substantially. This indicates that no common excited-state pathway for the two directions exists, as one would infer from a simple Woodward-Hoffmann consideration. These findings support recent quantum dynamic calculations on the excited-state topology of fulgimides.