Plasmon Dephasing in Single Gold Nanorods Observed By Ultrafast Time-Resolved Near-Field Optical Microscopy

Nishiyama, Yoshio; Imaeda, Keisuke; Imura, Kohei; Okamoto, Hiromi

doi:10.1021/acs.jpcc.5b03341

Cited by 39 publications

(53 citation statements)

References 44 publications

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“…In contrast, the TPPL from the gold nanoantenna presents a very different behaviour, and three regimes can be identified: (i) for δ ≲ 50 fs, the TPPL increases as the pulse duration decreases; (ii) for 100 ≲ δ ≲ 300 fs, the TPPL is almost constant; (iii) for δ ≳ 300 fs, the dependence on the inverse of δ is recovered. Regimes (ii) and (iii) were already studied in the study by Biagioni et al [18] and are consistent with the established model in which the TPE process in gold involves two successive single-photon absorptions, mediated by a real transition with lifetime T 1 in the few hundreds to thousands femtosecond range [18,19,32,37]. For nanoantennas resonant in the spectral region of the excitation spectrum, the LSPR acts as the intermediate state, enhancing the TPE process [32,37].…”

Section: The Initial Coherent Regimesupporting

confidence: 84%

“…Stockman et al [23] and Stockman [24] first linked the field of coherent control to the study of optical nanoantennas with the objective of simultaneously achieving nanometre and femtosecond control of optical fields. Experimental demonstrations of such control principle include: the phase and polarization manipulation of nanooptical fields in the incoherent regime [25,26]; the simultaneous high space and time resolution imaging of surface plasmon dynamics in the coherent and incoherent regimes [27][28][29][30][31][32][33]; and the phase-dependent control of the propagation of LSPRs through nanoparticle arrays caused by different amounts of dispersion acquired in different propagation directions [34,35].…”

Section: Introductionmentioning

confidence: 99%

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Selective excitation of individual nanoantennas by pure spectral phase control in the ultrafast coherent regime

et al. 2020

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Coherent control is an ingenious tactic to steer a system to a desired optimal state by tailoring the phase of an incident ultrashort laser pulse. A relevant process is the two-photon–induced photoluminescence (TPPL) of nanoantennas, as it constitutes a convenient route to map plasmonic fields, and has important applications in biological imaging and sensing. Unfortunately, coherent control of metallic nanoantennas is impeded by their ultrafast femtosecond dephasing times so far limiting control to polarization and spectral optimization. Here, we report that phase control of the TPPL in resonant gold nanoantennas is possible. We show that, by compressing pulses shorter than the localized surface plasmon dephasing time (<20 fs), a very fast coherent regime develops, in which the two-photon excitation is sensitive to the phase of the electric field and can therefore be controlled. Instead, any phase control is gone when using longer pulses. Finally, we demonstrate pure phase control by resorting to a highly sensitive closed-loop strategy, which exploits the phase differences in the ultrafast coherent response of different nanoantennas, to selectively excite a chosen antenna. These results underline the direct and intimate relation between TPPL and coherence in gold nanoantennas, which makes them interesting systems for nanoscale nonlinear coherent control.

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Section: The Initial Coherent Regimesupporting

confidence: 84%

Section: Introductionmentioning

confidence: 99%

Selective excitation of individual nanoantennas by pure spectral phase control in the ultrafast coherent regime

et al. 2020

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“…At the same time, for many applications such an intrinsic property of LSPR as its dephasing time plays a crucial role. For this reason, it is intensively studied . It is well known that plasmonic oscillations are damped out due to both radiative and non‐radiative processes.…”

Section: Introductionmentioning

confidence: 99%

“…For this reason, it is intensively studied. [7][8][9][10][11] It is well known [12] that plasmonic oscillations are damped out due to both radiative and non-radiative processes. Radiative processes dominate for comparatively big NPs.…”

Section: Introductionmentioning

confidence: 99%

Influence of Silver Nanoparticles Crystallinity on Localized Surface Plasmons Dephasing Times

Toropov

Леонов

Vartanyan

2017

Physica Status Solidi (b)

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The dephasing time of localized surface plasmons is a crucial parameter that defines the quality of resonance and achievable electromagnetic field enhancement near metal nanoparticles. Lattice irregularities of as‐deposited supported metal nanoparticles shorten the plasmon dephasing time and degrade the resonance quality. To study the crystallinity influence on the plasmon dephasing time in more detail, silver nanoparticles in the form of a granular film were produced on dielectric substrates via physical vapor deposition in a vacuum chamber. The samples are characterized using Vis–NIR spectroscopy and transmission electron microscopy. The persistent spectral hole burning technique is applied to study the annealing influence on the dephasing time of localized surface plasmons of the particular resonance frequency. After annealing, the improved crystallinity of nanoparticles leads to a twofold dephasing time increase. This conclusion is supported by the electron diffraction patterns. The role of the improved crystallinity among concurrent effects of annealing is discussed.

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“…13,14 Many studies determined the coherence time of surface plasmons in resonant nanoantennas to be in the fs range and therefore at the limit of the time resolution achievable by broadband laser systems. 20,[65][66][67][68] In our group we recently carried out a series of experiments aimed at detecting, understanding and making use of the ultrafast resonant response of plasmonic nanoantennas. 33,35,36 These experiments rely on the detection of nonlinear optical signals from the nanoantennas, such as SHG and two-photon induced photoluminescence (TPPL).…”

Section: Plasmonic Antennas For Ultrafast Nanophotonicsmentioning

confidence: 99%

Ultrafast Meets Ultrasmall: Controlling Nanoantennas and Molecules

2016

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We present a review on the advances of pulse control and ultrafast coherent excitation of both plasmonic nanoantennas and individual molecular systems, primarily based on the achievements in our group. Essential concepts from coherent control of ultrashort broadband laser pulses are combined with nanoscale diffraction limited detection and imaging of single photon emitters, i.e. the central area of this work is where ultrafast meets ultrasmall. First, the critical role of dedicated pulse shaping and phase control is discussed, which is crucial to realize free of spatio-temporal coupling Fourier limited pulses inside a high numerical aperture microscope at the diffraction limited spot. Next we apply this scheme to plasmonic antennas, exploiting broadband two-photon excitation, to determine amplitude and phase of plasmonic resonances, to achieve ultrafast switching of nanoscale hotspots, and multicolor second harmonic detection for imaging applications. Subsequently we address single molecules with phase-shaped pulses to control the electronic state population and retrieve single molecule vibrational dynamics response. We compare the response of a molecule to phase-locked with free phase multipulse excitation. Furthermore, we discuss phase control of excited state energy transfer in photosynthetic molecular complexes. Finally we combine nanoscale plasmonics with single molecule detection, to attain strong enhancement of both excitation and emission, with fluorescence lifetime shortening to the ps range. In conclusion, we anticipate that this review on ultrafast plasmonics and single emitter control will provide a useful view of the status of ultrafast nanophotonics and its application potential.

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Plasmon Dephasing in Single Gold Nanorods Observed By Ultrafast Time-Resolved Near-Field Optical Microscopy

Cited by 39 publications

References 44 publications

Selective excitation of individual nanoantennas by pure spectral phase control in the ultrafast coherent regime

Selective excitation of individual nanoantennas by pure spectral phase control in the ultrafast coherent regime

Influence of Silver Nanoparticles Crystallinity on Localized Surface Plasmons Dephasing Times

Ultrafast Meets Ultrasmall: Controlling Nanoantennas and Molecules

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