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Register a new userSecond-order quantum nonlinear optical processes in single graphene nanostructures and arrays
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Intense efforts have been made in recent years to realize nonlinear optical interactions at the single-photon level. Much of this work has focused on achieving strong third-order nonlinearities, such as by using single atoms or other quantum emitters while the possibility of achieving strong second-order nonlinearities remains unexplored. Here, we describe a novel technique to realize such nonlinearities using graphene, exploiting the strong per-photon fields associated with tightly confined graphene plasmons in combination with spatially nonlocal nonlinear optical interactions. We show that in properly designed graphene nanostructures, these conditions enable extremely strong internal down-conversion between a single quantized plasmon and an entangled plasmon pair, or the reverse process of second harmonic generation. A separate issue is how such strong internal nonlinearities can be observed, given the nominally weak coupling between these plasmon resonances and free-space radiative fields. On one hand, by using the collective coupling to radiation of nanostructure arrays, we show that the internal nonlinearities can manifest themselves as efficient frequency conversion of radiative fields at extremely low input powers. On the other hand, the development of techniques to efficiently couple to single nanostructures would allow these nonlinear processes to occur at the level of single input photons.
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Second order optical nonlinear processes involve the coherent mixing of two electromagnetic waves to generate a new optical frequency, which plays a central role in a variety of applications, such as ultrafast laser systems, rectifiers, modulators, and optical imaging. However, progress is limited in the mid-infrared (MIR) region due to the lack of suitable nonlinear materials. It is desirable to develop a robust system with a strong, electrically tunable second order optical nonlinearity. Here we demonstrate theoretically that AB-stacked bilayer graphene (BLG) can exhibit a giant and tunable second order nonlinear susceptibility chi ^(2) once an in-plane electric field is applied. chi^(2) can be electrically tuned from 0 to ~ {10^5 pm/V}, three orders of magnitude larger than the widely used nonlinear crystal AgGaSe2. We show that the unusually large chi^(2) arises from two different quantum enhanced two-photon processes thanks to the unique electronic spectrum of BLG. The tunable electronic bandgap of BLG adds additional tunability on the resonance of chi^(2), which corresponds to a tunable wavelength ranging from ~2.6 {mu}m to ~3.1 {mu}m for the up-converted photon. Combined with the high electron mobility and optical transparency of the atomically thin BLG, our scheme suggests a new regime of nonlinear photonics based on BLG.
Metal nanostructures can be used to harvest and guide the emission of single photon emitters on-chip via surface plasmon polaritons. In order to develop and characterize photonic devices based on emitter-plasmon hybrid structures a deterministic and scalable fabrication method for such structures is desirable. Here we demonstrate deterministic and scalable top-down fabrication of metal wires onto preselected nitrogen vacancy centers in nanodiamonds using clean room nano-fabrication methods. We observe a life-time reduction of the emitter emission that is consistent with earlier proof-of-principle experiments that used non-deterministic fabrication methods. This result indicates that top-down fabrication is a promising technique for processing future devices featuring single photon emitters and plasmonic nanostructures.
Pristine, undoped graphene has a constant absorption of 2.3 % across the visible to near-infrared (VIS-NIR) region of the electromagnetic spectrum. Under certain conditions, such as nanostructuring and intense gating, graphene can interact more robustly with VIS-NIR light and exhibit a large nonlinear optical response. Here, we explore the optical properties of graphene/LaAlO$_3$/SrTiO$_3$ nanostructures, where nanojunctions formed at the LaAlO$_3$/SrTiO$_3$ interface enable large (~10$^8$ V/m) electric fields to be applied to graphene over a scale of ~10 nm. Upon illumination with ultrafast VIS-NIR light, graphene/LaAlO$_3$/SrTiO$_3$ nanostructures produce broadband THz emission as well as a sum-frequency generated (SFG) response. Strong spectrally sharp, gate-tunable extinction features (>99.99%) are observed in both the VIS-NIR and SFG regions alongside significant intensification of the nonlinear response. The observed gate-tunable strong graphene-light interaction and nonlinear optical response are of fundamental interest and open the way for future exploitation in graphene-based optical devices.
It is shown that non-centrosymmetric materials with bulk second-order nonlinear susceptibility can be used to generate strongly antibunched radiation at an arbitrary wavelength, solely determined by the resonant behavior of suitably engineered coupled microcavities. The proposed scheme exploits the unconventional photon blockade of a coherent driving field at the input of a coupled cavity system, where one of the two cavities is engineered to resonate at both fundamental and second harmonic frequencies, respectively. Remarkably, the unconventional blockade mechanism occurs with reasonably low quality factors at both harmonics, and does not require a sharp doubly-resonant condition for the second cavity, thus proving its feasibility with current semiconductor technology.
Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure an electronic coherence time of 22 +/- 4 fs in graphene. The photocurrent is ideally suited to measure electronic coherence as it is a direct result of quantum path interference, controlled by the delay between two ultrashort two-color laser pulses. The maximum delay for which interference between the population amplitude injected by the first pulse interferes with that generated by the second pulse determines the electronic coherence time. In particular, numerical simulations reveal that the experimental data yield a lower boundary on the electronic coherence time and that coherent dephasing masks a lower coherence time. We expect that our results will significantly advance the understanding of coherent quantum-control in solid-state systems ranging from excitation with weak fields to strongly driven systems.
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