Multiphoton Absorption and Emission by Interaction of Swift Electrons with Evanescent Light Fields

Abajo, F. Javier García de; Asenjo-Garcı́a, Ana; Kociak, Mathieu

doi:10.1021/nl100613s

Cited by 211 publications

(254 citation statements)

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“…Single-color excitation (upper two panels in Fig. 1c) induces spectra with symmetric sideband peaks separated by the respective photon energy, as previously reported in the context of photon-induced near-field electron microscopy (PINEM) 36,29,30,26,37 and free-electron Rabi-oscillations 8,26 . Coupled to both near-fields, however, the electron spectrum develops a strong asymmetry (lower two panels in Fig.…”

supporting

confidence: 75%

“…Equivalently, the quantum state can be written as a coherent superposition of momentum sidebands 26,29,30 . The action of two fields at frequencies ω and 2ω is now described in terms of two superimposed phase modulations, which for the typically small total energy changes (relative to the initial electron energy) results in the electron quantum state…”

mentioning

confidence: 99%

“…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 .…”

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

et al. 2017

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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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confidence: 99%

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confidence: 99%

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

et al. 2017

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“…27,28 Theoretical accounts have been given by various groups. [29][30][31] Here, we present the imaging aspect of PINEM, in particular, the capability to visualize the optical near field by spatially mapping the photon-electron interaction, and compare it to that by EELS. In EELS, swift electrons induce a transient electric field with a continuous spectrum of frequency and excite plasmons in nearby particles.…”

Section: Introductionmentioning

confidence: 99%

Photon-induced near-field electron microscopy

Barwick

Flannigan

Zewail

2009

Nature

605

639

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Ultrafast electron microscopy in the space and time domains utilizes a pulsed electron probe to directly map structural dynamics of nanomaterials initiated by an optical pump pulse, in imaging, diffraction, spectroscopy, and their combinations. It has demonstrated its capability in the studies of phase transitions, mechanical vibrations, and chemical reactions. Moreover, electrons can directly interact with photons via the near field component of light scattering by nanostructures, and either gain or lose light quanta discretely in energy. By energetically selecting those electrons that exchanged photon energies, we can map this photon-electron interaction, and the technique is termed photon-induced near field electron microscopy (PINEM). Here, we give an account of the theoretical understanding of PINEM. Experimentally, nanostructures such as a sphere, cylinder, strip, and triangle have been investigated. Theoretically, time-dependent Schrödinger and Dirac equations for an electron under light are directly solved to obtain analytical solutions. The interaction probability is expressed by the mechanical work done by an optical wave on a traveling electron, which can be evaluated analytically by the near field components of the Rayleigh scattering for small spheres and thin cylinders, and numerically by the discrete dipole approximation for other geometries. Application in visualization of plasmon fields is discussed.

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“…Barwick et al demonstrated a time-resolved imaging technique for nanostructures with a femtosecond laser in ultrafast electron microscopy (UEM) and termed it photon-induced near-field electron microscopy (PINEM), emphasizing the capability to image the plasmon fields [28,29]. Theoretical accounts have been given by various groups [30][31][32][33]. In particular, the PINEM (image) intensity is approximately proportional to the absolute square of the "field integral," which is defined as the mechanical work performed on the moving electron by the scattered electromagnetic wave (electric field) [34].…”

Section: Introductionmentioning

confidence: 99%

Photon-induced near-field electron microscopy: Mathematical formulation of the relation between the experimental observables and the optically driven charge density of nanoparticles

Park

Zewail

2014

Phys. Rev. A

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Photon-induced near-field electron microscopy (PINEM) enables the visualization of the plasmon fields of nanoparticles via measurement of photon-electron interaction [S. T. Park et al., New J. Phys. 12, 123028 (2010)]. In this paper, the field integral, which is a mechanical work performed on a fast electron by the total electric field, plays a key role in understanding the interaction. Here, we reexamine the field integral and give the physical meaning by decomposing the contribution of the field from the charge-density distribution. It is found that the "near-field integral" (the near-field approximation of the field integral) can be expressed as a convolution of the two-dimensional projection of the optically driven charge-density distribution in the nanoparticle with a broad radial response function. This approach, which we call the "convolution method," is validated by applying it to Rayleigh scattering cases, where previous analytical expressions for the field integrals in near-field approximations are reproduced by the convolution method. The convolution method is applied to discrete dipole approximation calculations of a silver nanorod, and the nature of the induced charge-density distributions of its plasmons is discussed.

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Multiphoton Absorption and Emission by Interaction of Swift Electrons with Evanescent Light Fields

Cited by 211 publications

References 10 publications

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

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

Photon-induced near-field electron microscopy

Photon-induced near-field electron microscopy: Mathematical formulation of the relation between the experimental observables and the optically driven charge density of nanoparticles

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