Nanoscopic Ultrafast Space-Time-Resolved Spectroscopy

Brixner, Tobias; Abajo, F. Javier García de; Schneider, J.; Pfeiffer, Walter

doi:10.1103/physrevlett.95.093901

Cited by 132 publications

(120 citation statements)

References 21 publications

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“…These metal structures can be realized by e-beam lithography. Solving Maxwell's equations for this geometry shows that plasmonic effects and an optimization procedure of the applied pulses allows to selectively excite single quantum dots 44,45 : For optimizing the pulse envelope of a single pulse E(t, r) towards a field localization at only one quantum dot, we use time-harmonic solutions E ν (ω, r), represented by incident plane waves of polarization directions p, s and incoming direction (indexed as ν) 45 :…”

Section: A Localized Excitationmentioning

confidence: 99%

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

et al. 2012

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We show how coherent, spatially resolved spectroscopy can disentangle complex hybrid wave functions into wave functions of the individual emitters. This way, detailed information on the coupling of the individual emitters, not available in far-field spectroscopy, can be revealed. Here we propose a quantum state tomography protocol that relies on the ability to selectively excite each emitter individually by spatially localized pulses. Simulations of coupled semiconductor GaAs/InAs quantum dots using light fields available in current nanoplasmonics show, that undesired resonances can be removed from measured spectra. The method can be applied on a broad range of coupled emitters to study the internal coupling, including pigments in photosynthesis and artificial light harvesting.

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Section: A Localized Excitationmentioning

confidence: 99%

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

et al. 2012

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“…Combination with femtosecond excitation offers high resolution in space and time (8-15) and opens routes toward novel applications (16,17). In particular, deliberate spatial manipulation of optical near-field distributions was realized with adaptive and coherent control methods (9,(11)(12)(13)(18)(19)(20)(21)(22). In our recent demonstration of adaptive control of nanooptical fields (13), only spatial properties of optical near-field distributions were accessed.…”

mentioning

confidence: 99%

“…For the case of spatial light-field properties, on the other hand, emerging nanooptical techniques (6) have made available spectroscopy beyond the Abbe diffraction limit, as, for example, nanoantenna-assisted addressing of individual molecules (7). Combination with femtosecond excitation offers high resolution in space and time (8)(9)(10)(11)(12)(13)(14)(15) and opens routes toward novel applications (16,17). In particular, deliberate spatial manipulation of optical near-field distributions was realized with adaptive and coherent control methods (9,(11)(12)(13)(18)(19)(20)(21)(22).…”

mentioning

confidence: 99%

Spatiotemporal control of nanooptical excitations

Aeschlimann

Bauer

Bayer

et al. 2010

Proc. Natl. Acad. Sci. U.S.A.

141

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The most general investigation and exploitation of light-induced processes require simultaneous control over spatial and temporal properties of the electromagnetic field on a femtosecond time and nanometer length scale. Based on the combination of polarization pulse shaping and time-resolved two-photon photoemission electron microscopy, we demonstrate such control over nanoscale spatial and ultrafast temporal degrees of freedom of an electromagnetic excitation in the vicinity of a nanostructure. The time-resolved cross-correlation measurement of the local photoemission yield reveals the switching of the nanolocalized optical near-field distribution with a lateral resolution well below the diffraction limit and a temporal resolution on the femtosecond time scale. In addition, successful adaptive spatiotemporal control demonstrates the flexibility of the method. This flexible simultaneous control of temporal and spatial properties of nanophotonic excitations opens new possibilities to tailor and optimize the lightmatter interaction in spectroscopic methods as well as in nanophotonic applications.coherent control | nanophotonics | plasmonics | ultrafast spectroscopy T he interaction of light with matter is of fundamental importance in many areas of nature, science, and engineering, and the dynamics and efficiency of light-induced processes are determined by the properties of the optical field as a function of space and time at the location of interaction. Hence their most general investigation and exploitation would require the generation of light fields that can be specified at will in both their spatial and temporal degrees of freedom at all length and time scales. In the past, significant progress has been made toward realizing either of these two manipulation objectives separately. For temporal field properties, femtosecond laser pulse shaping (1) offers flexible control over the field amplitude, phase, and polarization (2, 3) on an ultrashort time scale. This has been exploited for coherent control over numerous quantum-mechanical systems (4, 5). For the case of spatial light-field properties, on the other hand, emerging nanooptical techniques (6) have made available spectroscopy beyond the Abbe diffraction limit, as, for example, nanoantenna-assisted addressing of individual molecules (7). Combination with femtosecond excitation offers high resolution in space and time (8-15) and opens routes toward novel applications (16,17). In particular, deliberate spatial manipulation of optical near-field distributions was realized with adaptive and coherent control methods (9,(11)(12)(13)(18)(19)(20)(21)(22). In our recent demonstration of adaptive control of nanooptical fields (13), only spatial properties of optical near-field distributions were accessed. In the present work, in contrast, we directly measure and control also the temporal evolution of the nanoscale excitation. This information is obtained and exploited here using time-resolved cross-correlation measurements with one polarization-shaped "pump" light pu...

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“…An important future application of ROAs is coherent spatiotemporal control of optical fields for antenna-enhanced local spectroscopies. Coherent control of near-fields by amplitude and polarization pulse shaping has recently been theoretically proposed [8,9,10,11] and experimentally realized [12]. In extension of such experiments it is envisaged to perform spectroscopy of complex matter in contact with a ROA assembly, which will allow studying ultrafast temporal dynamics with nanoscale spatial resolution [13].…”

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confidence: 99%

Deterministic spatiotemporal control of optical fields in nanoantennas and plasmonic circuits

et al. 2009

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We show that pulse shaping techniques can be applied to tailor the ultrafast temporal response of the strongly confined and enhanced optical near fields in the feed gap of resonant optical antennas (ROAs). Using finite-difference time-domain (FDTD) simulations followed by Fourier transformation, we obtain the impulse response of a nano structure in the frequency domain, which allows obtaining its temporal response to any arbitrary pulse shape. We apply the method to achieve deterministic optimal temporal field compression in ROAs with reduced symmetry and in a twowire transmission line connected to a symmetric dipole antenna. The method described here will be of importance for experiments involving coherent control of field propagation in nanophotonic structures and of light-induced processes in nanometer scale volumes.PACS numbers: 73.21, 84.40.Ba, 84.40.Az Resonant optical antennas (ROA) are metal nano structures that upon illumination with light of welldefined wavelength and polarization exhibit hot spots in which the local optical field is spatially confined and strongly enhanced due to geometry-dependent plasmon resonances [1,2]. When excited by a pulsed laser such hot spots provide the possibility to e.g. investigate nonlinear behavior of materials at moderate pulse energies [2,3,4]. Vice versa, well designed ROAs are able to enhance and direct the radiation of point-like sources that drive the antenna from within a hot spot [5,6] thus providing the basis for enhanced single photon sources [5] and antenna-enhanced local spectroscopy [7]. An important future application of ROAs is coherent spatiotemporal control of optical fields for antenna-enhanced local spectroscopies. Coherent control of near-fields by amplitude and polarization pulse shaping has recently been theoretically proposed [8,9,10,11] and experimentally realized [12]. In extension of such experiments it is envisaged to perform spectroscopy of complex matter in contact with a ROA assembly, which will allow studying ultrafast temporal dynamics with nanoscale spatial resolution [13]. The well-established techniques of femtosecond quantum control [14,15] can be realized on the nanoscale. To reach this goal it is important to understand how the resonant character of nano antennas affects the pulse shape in the feed gap and which degrees of freedom are available to be exploited for coherent control of their near-fields. So far efficient ROAs have been realized using noble metal nano rods which are produced by microfabrication techniques. The plasmon resonances of individual rods are determined by their dimensions and dielectric function [16] or equivalently by length-dependent FabryPerot resonances of a plasmon wave [17] propagating with an effective wavelength [18] along the rod and being reflected at its ends. While a single rod may be considered a monopole antenna [6], dipole antennas are formed by aligning two nano rods end to end thus creating a very small feed gap between the two rods where optical fields are concentrated [2]. The plasmon ...

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Nanoscopic Ultrafast Space-Time-Resolved Spectroscopy

Cited by 132 publications

References 21 publications

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

Reconstruction of the wave functions of coupled nanoscopic emitters using a coherent optical technique

Spatiotemporal control of nanooptical excitations

Deterministic spatiotemporal control of optical fields in nanoantennas and plasmonic circuits

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