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Giant Electron–Phonon Coupling Detected Under Surface Plasmon Resonance in Au Film

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Giant Electron–Phonon Coupling Detected Under Surface Plasmon Resonance in Au Film 4590 Vol. 44, No. 18 / 15 September 2019 / Optics Letters Letter Giant electron–phonon coupling detected under surface plasmon resonance in Au film 1,2 3 3 1,2, FENG HE, NATHANIAL SHEEHAN, SETH R. BANK, AND YAGUO WANG * 1Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712, USA 2Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, USA 3Department of Electrical and Computer Engineering, The University of Texas at Austin, Austin, Texas 78758, USA *Corresponding author: [email protected] Received 4 July 2019; revised 22 August 2019; accepted 23 August 2019; posted 23 August 2019 (Doc. ID 371563); published 13 September 2019 Surface plasmon resonance (SPR) is a powerful tool to am- small change in reflectance/transmittance and can hardly be plify coherent phonon signals in metal films. In a 40 nm Au captured by regular coherent phonon spectroscopy. film excited with a 400 nm pump, we observed an abnor- Surface plasmon resonance (SPR) has been proven a power- mally large electron–phonon coupling constant of about ful tool to enhance the detection of CPs in metal films 17 3 8 × 10 W∕ m K, almost 40× larger than those reported [2,17–19] and dielectrics [14]. SPR is the coherent excitation in noble metals, and even comparable to transition metals. of a delocalized charge wave that propagates along an interface. We attribute this phenomenon to quantum confinement SPPs, which are the evanescent waves from the coupling be- and interband excitation. With SPR, we also observed tween light and SP in metals, can create a strongly enhanced two coherent phonon modes in a GaAs/AlAs quantum well electric field at the metal/air interface [20]. The most conven- thin film. Our finding provides a new approach to generate ient way to couple the light with the SP wave (collective elec- high-frequency acoustic phonons in noble metals and to tronic modes) is using a prism or a grating. The two most study their nonlinear nature of propagation. © 2019 popular prism coupling geometries are the Kretschmann con- Optical Society of America figuration Fig. 1(a)] and the Otto configuration [20]. To excite SPR, the wave vector k of incident light must satisfy the fol- https://doi.org/10.1364/OL.44.004590 x lowing criteria [20]: pffiffiffiffiffi ω ω ε ε 1∕2 ε sin θ m α kx P ksp ε ε , (1) c c m α Au nanostructures, e.g., films and nanoparticles, are the most ε ε ε studied plasmonic materials for terahertz emission [1], gas de- where P, m, α are the dielectric constant of the prism, metal, ω tection and biosensing [2–8], electromechanical devices [9], and material under detection, respectively. is the photon fre- 2π∕λ λ photothermal therapy [10], photoacoustic imaging [11], etc. quency of incident light, which is equal to , where is the θ The localized surface plasmons (SPs) and propagating surface wavelength of the incident light. is the incident angle and c is plasmon polaritons (SPPs) in Au nanostructures are highly tun- the speed of light in vacuum. To satisfy Eq. (1), the real part of able by manipulating the structure geometry and shape. Au the dielectric constant of the metal must be negative, and its nanostructures can also be easily hybridized with a wide range magnitude must be greater than that of the material under of semiconductors, dielectrics, and organic materials [10–14]to detection. This criterion can be satisfied at interfaces of noble enhance their performance. Under light excitation, electrons metals (Au, Ag, Al) with many common semiconductors. As first absorb photon energy and then pass it to phonons (quan- shown in Fig. 1(b) in an Au film, when the incident angle tized lattice vibration). The electron–phonon (e–ph) coupling of probe beam is close to the SPR angle, dR∕dθ becomes very determines how fast the energy is deposited into phonons from large and a small disturb of the SPR angle will induce large the electrons and hence is critical for many applications. Noble reflectivity changes [21]. When CPs travel into the region of metals like Au and Ag usually possess a small e–ph coupling the surface plasmon, the collective oscillation of atoms will constant (∼1016 W∕ m3K), much less than some transition modulate the local dielectric constant and slightly alter the metals, such as Ni and Co (∼1017 W∕ m3K). For most of the SPR angle. Owing to the large dR∕dθ, the reflectivity change studies, to extract the e–ph coupling constant of Au nanostruc- from coherent phonons can be amplified substantially. It has tures, the electronic decay signals from femtosecond pump- been reported that the coherent phonon signals in metal films probe experiments were used [15]. The obtained e–ph coupling could be enhanced by 10–100 times [14,17,18]. Recently, constant is a value averaged over all phonon modes. Rarely a surface plasmon has been utilized to detect coherent thermal measured is the e–ph coupling between electrons and specific phonons in gold film up to 1 THz [19]. phonon modes [16] that requires excitation/detection of coher- In this work, we incorporate the Kretschmann configuration ent phonons (CPs). CPs in Au nanofilms produce an extremely into a coherent phonon spectrometer to excite SPR and detect 0146-9592/19/184590-04 Journal © 2019 Optical Society of America Letter Vol. 44, No. 18 / 15 September 2019 / Optics Letters 4591 was obtained, which was then transferred onto a 25 nm Au film deposited directly on a prism. A home-built coherent phonon spectrometer used laser pulses out of a mode-locked Ti:Sapphire femtosecond laser (Spitfire ACE, Spectra Physics, 800 nm wavelength, 100 fs pulse duration, 5 kHz repetition rate). For the pump, a sec- ond-harmonic-generation crystal (beta-barium borate, BBO) was used to double the photon energy to 3.1 eV. All experi- ments were carried out in a “front pump back probe” configu- ration, where the pump irradiates from the air/sample interface and the probe detects from the prism side. A 15 cm lens was used to focus both the pump and probe beams, with spot sizes (diameter at the 1∕e2 intensity level) of 245 μm and 60 μm, respectively. The pump fluence was fixed at 1.27 mJ∕cm2. The rotational stage on which the samples sat was used to control the incident angle of the probe beam. All devices were synchronized through a home-built LabView program for real-time data acquisition [22,23]. Fig. 1. (a) SPR generated in Kretschmann configuration. The red- First, we measured the angle-resolved static reflectance of shaded region represents the SPP excited resonantly (ksp kx). a 40 nm Au thin film in the Kretschmann configuration A p-polarized probe beam incident from prism side along the SPR [Figs. 1(a) and 1(b)]. The reflectance displays a minimum value angle θ0; (b) angle-resolved static reflectance change at different angles. around 41.3°, marked by angle a, at which the criteria of Four angles marked as a, b, c, d were chosen to perform coherent Eq. (1) is satisfied and SPR excitation occurs. For comparison, phonon measurements; (c) time-resolved ΔR∕R signals measured in four incident angles (a, b, c, d) were selected to perform co- a 40 nm Au film with a coherent phonon spectrometer, at four differ- herent phonon measurements, where a is the SPR angle, b and ent incident angles marked in (b); (d) coherent echoes after removing c are angles located in the linear dR∕dθ regions on two sides of electronic background. Orange-dashed lines mark the duration of sin- the dip, and d lies in a region far away from the SPR angle. gle acoustic echo. Blue-dashed lines mark the separation time between As shown in the inset of Fig. 1(c), we generated coherent two echoes. acoustic phonons by heating the air/Au interface with a weakly focused pump beam and detecting from the prism side with a p-polarized probe beam. The pump beam size is about ∼4 CPs in a bare Au film. We observed an abnormally large e–ph times larger than the probe beam. Figure 1(c) shows the tran- coupling constant of about 8 × 1017 W∕ m3K, almost 40× sient reflectivity changes at four different incident angles, larger than those previously reported in Au films, and even marked in Fig. 1(b). At all angles, ΔR∕R shows a sharp positive comparable to transition metals. SPR-enhanced detection of peak around time zero, which is due to the excitation of the hot CPs in semiconductors has not been reported. In semiconduc- electrons, and the decaying processes reveal hot electron relax- tor, CPs are usually detected through the stimulated Raman ation via electron–electron and e–ph coupling. The angle a light scattering mechanism; hence, only the phonons with wave gives the highest peak signal, which is reasonable because of Δ ∕ vectors kphonon 0 ∼ 2kprobe can be detected. With SPR, the the resonant condition. R R peaks at angles b and c have detected reflectivity change of the probe beam comes from the almost the same height because of their similar dR∕dθ values. interference between the surface plasmon and coherent pho- Angle d shows the smallest ΔR∕R peak due to its off-resonant nons; therefore, a broader band of CPs might be detected. condition. Compared to angle d, the ΔR∕R peak at angle a is In this study, substantial CP enhancement is also demonstrated enhanced by more than 75 times. in a GaAs/AlAs superlattice (SL), when the incident light fol- After removing the electronic background, we can see echo- lows an angle close to the SPR angle.
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