Mark E. Siemens

Probing the timescale of the exchange interaction in a ferromagnetic alloy

The underlying physics of all ferromagnetic behavior is the cooperative interaction between individual atomic magnetic moments that results in a macroscopic magnetization. In this work, we use extreme ultraviolet pulses from high-harmonic generation as an element-specific probe of ultrafast, optically driven, demagnetization in a ferromagnetic Fe-Ni alloy (permalloy). We show that for times shorter than the characteristic timescale for exchange coupling, the magnetization of Fe quenches more strongly than that of Ni. Then as the Fe moments start to randomize, the strong ferromagnetic exchange interaction induces further demagnetization in Ni, with a characteristic delay determined by the strength of the exchange interaction. We can further enhance this delay by lowering the exchange energy by diluting the permalloy with Cu. This measurement probes how the fundamental quantum mechanical exchange coupling between Fe and Ni in magnetic materials influences magnetic switching dynamics in ferromagnetic materials relevant to next-generation data storage technologies.

Unraveling quantum pathways using optical 3D Fourier-transform spectroscopy.

Predicting and controlling quantum mechanical phenomena require knowledge of the system Hamiltonian. A detailed understanding of the quantum pathways used to construct the Hamiltonian is essential for deterministic control and improved performance of coherent control schemes. In complex systems, parameters characterizing the pathways, especially those associated with inter-particle interactions and coupling to the environment, can only be identified experimentally. Quantitative insight can be obtained provided the quantum pathways are isolated and independently analysed. Here we demonstrate this possibility in an atomic vapour using optical three-dimensional Fourier-transform spectroscopy. By unfolding the system’s nonlinear response onto three frequency dimensions, three-dimensional spectra unambiguously reveal transition energies, relaxation rates and dipole moments of each pathway. The results demonstrate the unique capacity of this technique as a powerful tool for resolving the complex nature of quantum systems. This experiment is a critical step in the pursuit of complete experimental characterization of a system’s Hamiltonian.

Resonance lineshapes in two-dimensional Fourier transform spectroscopy

We derive an analytical form for resonance lineshapes in two-dimensional (2D) Fourier transform spectroscopy. Our starting point is the solution of the optical Bloch equations for a two-level system in the 2D time domain. Application of the projection-slice theorem of 2D Fourier transforms reveals the form of diagonal and cross-diagonal slices in the 2D frequency data for arbitrary inhomogeneity. The results are applied in quantitative measurements of homogeneous and inhomogeneous broadening of multiple resonances in experimental data.

High-frequency surface acoustic wave propagation in nanostructures characterized by coherent extreme ultraviolet beams

We study ultrahigh frequency surface acoustic wave propagation in nickel-on-sapphire nanostructures. The use of ultrafast, coherent, extreme ultraviolet beams allows us to extend optical measurements of propagation dynamics of surface acoustic waves to frequencies of nearly 50 GHz, corresponding to wavelengths as short as 125 nm. We repeat the measurement on a sequence of nanostructured samples to observe surface acoustic wave dispersion in a nanostructure series for the first time. These measurements are critical for accurate characterization of thin films using this technique.

Ultrafast Extreme Ultraviolet Holography: Dynamic Monitoring of Surface Deformation

We demonstrate femtosecond time-resolved dynamic Gabor holography using highly coherent extreme ultraviolet light generated by high harmonic upconversion of a femtosecond laser. By reflecting this light from an impulsively heated surface, we implement a simple and robust single-reflection geometry for phase-sensitive holographic detection at extreme UV wavelengths. Using this setup, we study the ultrafast deformation and subsequent acoustic oscillations within a thin metal film. These measurements exhibit subpicometer spatial sensitivity in the vertical dimension.

Probing Thermomechanics at the Nanoscale: Impulsively Excited Pseudosurface Acoustic Waves in Hypersonic Phononic Crystals

High-frequency surface acoustic waves can be generated by ultrafast laser excitation of nanoscale patterned surfaces. Here we study this phenomenon in the hypersonic frequency limit. By modeling the thermomechanics from first-principles, we calculate the system’s initial heat-driven impulsive response and follow its time evolution. A scheme is introduced to quantitatively access frequencies and lifetimes of the composite system’s excited eigenmodes. A spectral decomposition of the calculated response on the eigemodes of the system reveals asymmetric resonances that result from the coupling between surface and bulk acoustic modes. This finding allows evaluation of impulsively excited pseudosurface acoustic wave frequencies and lifetimes and expands our understanding of the scattering of surface waves in mesoscale metamaterials. The model is successfully benchmarked against time-resolved optical diffraction measurements performed on one-dimensional and two-dimensional surface phononic crystals, probed using light at extreme ultraviolet and near-infrared wavelengths.

Transient grating measurement of surface acoustic waves in thin metal films with extreme ultraviolet radiation

The authors demonstrate the use of coherent extreme ultraviolet (EUV) light in laser induced transient grating spectroscopy. In this work, the authors study the dispersion of pulsed laser induced surface acoustic waves in a thin uniform nickel film by monitoring the diffraction of 30nm EUV light from the surface. Transient deformation of the sample surface leads to absolute diffracted intensities approaching 10−3 for 1A displacement, an ∼700-fold increase in sensitivity compared with optical probing. EUV probing provides a convenient geometry for observing short wavelength acoustic propagation.

Nanoscale photothermal and photoacoustic transients probed with extreme ultraviolet radiation

We demonstrate the use of extreme ultraviolet (EUV) light for time-resolved measurements of the photothermal and photoacoustic response of materials. By using wavelengths that are 20× shorter than visible light, we demonstrate the potential for dramatically increased sensitivity and signal levels, in some cases by almost two orders of magnitude compared with visible light. This approach will enable probing of surface acoustic dynamics on nano-scale spatial dimensions of 50nm and below, using a small scale coherent EUV sources employing high-harmonic generation.

Optical 2-D Fourier Transform Spectroscopy of Excitons in Semiconductor Nanostructures

Optical 2-D Fourier transform spectroscopy is a powerful technique for studying resonant light-matter interactions, determining the transition structure and monitoring dynamics of optically created excitations. The ability to separate homogeneous and inhomogeneous broadening is one important capability. In this paper, we discuss the use of this technique to study excitonic transitions in semiconductor nanostructures. In quantum wells, the effects of structural disorder is observed as inhomogeneous broadening of the exciton resonances. In quantum dots, the temperature dependence of the homogeneous width gives insight into the nature of the dephasing processes.

Measurement of the M 2 beam propagation factor using a focus-tunable liquid lens

We demonstrate motion-free beam quality M² measurements of stigmatic, simple astigmatic, and general astigmatic (twisted) beams using only a focus-tunable liquid lens and a CCD camera. We extend the variable-focus technique to the characterization of general astigmatic beams by measuring the 10 second-order moments of the power density distribution for the twisted beam produced by passage through multimode optical fiber. Our method measures the same M² values as the traditional variable-distance method for a wide range of laser beam sources, including nearly TEM(00) (M²≈1) and general astigmatic multimode beams (M²≈8). The method is simple and compact, with no moving parts or complex apparatus and measurement precision comparable to the standard variable-distance method.