Control of Ultrafast Electron Dynamics with Shaped Femtosecond Laser Pulses: From Atoms to Solids

Wollenhaupt, M.; Bayer, Tim; Baumert, Thomas

doi:10.1007/978-3-319-20173-3_4

Cited by 13 publications

(10 citation statements)

References 136 publications

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“…Femtosecond polarization pulse shaping [1][2][3][4][5] is an established experimental technique which provides access to the spatial nature of the light-matter interaction by control of the instantaneous ellipticity of the laser pulse. Control by polarization-shaped femtosecond laser pulses has been demonstrated in numerous experiments including coherent manipulation of two-photon absorption in atomic rubidium [6] and optimization of the ion yield in the multi-photon ionization of potassium dimers [7].…”

Section: Introductionmentioning

confidence: 99%

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Control of photoelectron momentum distributions by bichromatic polarization-shaped laser fields

et al. 2017

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Bichromatic polarization-shaped femtosecond laser pulses are used to control three-dimensional photoelectron momentum distributions (3D-EDs) from resonance enhanced multi-photon ionization of potassium atoms. The light fields consisting of two spectral bands with different ellipticity are produced using an ultrafast polarization pulse shaper equipped with a custom polarizer in the Fourier plane. The tomographically reconstructed 3D-EDs from ionization with counterrotating circularly or orthogonal linearly polarized bichromatic laser pulses show different angular momentum superposition states at four distinct photoelectron energies. The analysis of the measured 3D-EDs reveals that the underlying physical mechanism is based on the interplay of ionization pathway selection via quantum mechanical selection rules for optical transitions and intrapulse frequency mixing of the spectral bands with different ellipticity. multiple ionization pathways by energetic separation of different angular momentum target states. Control of the ionization pathway along with energy-and angle-resolved detection allows us, on the one hand, to generate individual angular momentum free electron wave packets using CNR-CP bichromatic pulses and, on the other hand, to create unusual angular momentum superposition states using O-LP bichromatic pulses. In the experiment, bichromatic polarization-tailored fields are produced using a f 4 polarization pulse shaper [35] equipped with a custom polarizer in the Fourier plane [36,37]. Multiple photoelectron momentum images are recorded employing a velocity map imaging (VMI) spectrometer [38] and subsequently combined to reconstruct the 3D-EDs using a tomography algorithm [39][40][41]. Positive and negative time delays between the two colors are introduced to discriminate resonant from non-resonant ionization and to observe signatures from spin-orbit wave packets (SOWPs) in the 3D-EDs. A similar setup was recently used to produce electron vortices with a sequence of two one-color CNR-CP femtosecond laser pulses [42]. In that experiment, the minimal time delay in the sequence was given by the pulse length in order to avoid the creation of linear polarization in the overlapping interval. However, CNR-CP bichromatic fields, consisting of temporally overlapping left-(L-CP) and right-handed circularly (R-CP) polarized disjoined spectral bands do not create linearly polarized light. This feature allows us to observe photoelectrons from REMPI by overlapping bichromatic CNR-CP pulses such that frequency mixing between photons of opposite helicity can occur. For example, we demonstrate that 3D-EDs from three-photon ionization with two red L-CP photons and one blue R-CP photon are observed in a specific kinetic energy window.We start in section 2 with a theoretical discussion of the 3D-EDs from 1+2 REMPI with bichromatic polarization-shaped laser pulses. Section 3 introduces the experimental strategy based on the combination of polarization pulse shaping and tomographic photoelectron imaging. The experimental ...

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Section: Introductionmentioning

confidence: 99%

“…and the corresponding CGCs, summed over all relevant helicity combinations as described by equation(4). The weighted energy distributions are shown in table 1(b) for the CNR-CP and in table 2(b) for the O-LP case.…”

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Control of photoelectron momentum distributions by bichromatic polarization-shaped laser fields

et al. 2017

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“…(2). A rich variety of tailored quantum states is accessible by variation of the relative phase and amplitudes of such bichromatic fields, and a further design of such momentum state synthesis may be realized by optical pulse-shaping techniques 39 .…”

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Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

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We introduce a framework for the preparation, coherent manipulation and characterization of free-electron quantum states, experimentally demonstrating attosecond pulse trains for electron microscopy. Specifically, we employ phaselocked single-color and two-color optical fields to coherently control the electron wave function along the beam direction. We establish a new variant of quantum state tomography -"SQUIRRELS" -to reconstruct the density matrices of freeelectron ensembles and their attosecond temporal structure. The ability to tailor and quantitatively map electron quantum states will promote the nanoscale study of electron-matter entanglement and the development of new forms of ultrafast electron microscopy and spectroscopy down to the attosecond regime.Optical, electron and x-ray microscopy and spectroscopy reveal specimen properties via spatial and spectral signatures imprinted onto a beam of radiation or electrons. Leaving behind the traditional paradigm of idealized, simple probe beams, advanced optical techniques increasingly harness tailored probes, or even their quantum properties and probe-sample entanglement. The rise of structured illumination microscopy 1 , pulse shaping 2 , and multidimensional 3 and quantum-optical spectroscopy 4 exemplify this development. Similarly, electron microscopy explores the use of shaped electron beams exhibiting particular spatial symmetries 5 or angular momentum 6,7 , and novel measurement schemes involving quantum aspects of electron probes have been proposed 8,9 . Ultrafast imaging and spectroscopy with electrons and x-rays are the basis for an ongoing revolution in the understanding of dynamical processes in matter on atomic scales [10][11][12][13] . The underlying technology heavily rests on laser science for the 2 generation and characterization of ever-shorter femtosecond electron 10,14 and xray [15][16][17] probe pulses, with examples in optical pulse compression 18 and streaking spectroscopy [19][20][21] . The temporal structuring of electron probe beams is facilitated by time-dependent fields in the radio-frequency [22][23][24] , terahertz 18,25 or optical domains. Promising a further leap in temporal resolution, recent findings suggest that ultrafast electron diffraction and microscopy with optically phasecontrolled and sub-cycle, attosecond-structured wave functions may be feasible 8,[26][27][28][29][30] . Specifically, light-field control may translate the temporal resolution of ultrafast transmission electron microscopy (UTEM) 31,32 and electron diffraction (UED) 10,33 , currently at about 200 fs 34 and 20 fs 14,23 , respectively, to the range of attoseconds 26,27,35 . However, such future technologies call for means to both prepare and fully analyze the corresponding quantum states of free electrons.Here, we demonstrate the coherent control and attosecond density modulation of free-electron quantum states using multiple phase-locked optical interactions. Moreover, we introduce quantum state tomography for free electrons, providing crucial e...

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“…The presented scheme offers full control over all bichromatic parameters such as the frequency ratio, the amplitude ratio, the bandwidth and the polarization state of both colors. Moreover, the additional phase modulation modality provides us with the complete toolbox of femtosecond pulse shaping [35, 55,56] individually applicable to each color. The output waveform can be controlled by tuning the CEP or by adjusting the relative phase and time delay between the two colors with zeptosecond precision [15].…”

Section: Discussionmentioning

confidence: 99%

Ultrashort polarization-tailored bichromatic fields from a CEP-stable white light supercontinuum

et al. 2017

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We apply ultrafast polarization shaping to an ultrabroadband carrier envelope phase (CEP) stable white light supercontinuum to generate polarization-tailored bichromatic laser fields of low-order frequency ratio. The generation of orthogonal linearly and counter-rotating circularly polarized bichromatic fields is achieved by introducing a composite polarizer in the Fourier plane of a 4 f polarization shaper. The resulting Lissajous-and propeller-type polarization profiles are characterized experimentally by cross-correlation trajectories. The scheme provides full control over all bichromatic parameters and allows for individual spectral phase modulation of both colors. Shaper-based CEP control and the generation of tailored bichromatic fields is demonstrated. These bichromatic CEP-stable polarization-shaped ultrashort laser pulses provide a versatile class of waveforms for coherent control experiments.

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Control of Ultrafast Electron Dynamics with Shaped Femtosecond Laser Pulses: From Atoms to Solids

Cited by 13 publications

References 136 publications

Control of photoelectron momentum distributions by bichromatic polarization-shaped laser fields

Control of photoelectron momentum distributions by bichromatic polarization-shaped laser fields

Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

Ultrashort polarization-tailored bichromatic fields from a CEP-stable white light supercontinuum

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