Graphene is an attractive material for optoelectronics and photodetection applications because it offers a broad spectral bandwidth and fast response times. However, weak light absorption and the absence of a gain mechanism that can generate multiple charge carriers from one incident photon have limited the responsivity of graphene-based photodetectors to ∼10(-2) A W(-1). Here, we demonstrate a gain of ∼10(8) electrons per photon and a responsivity of ∼10(7) A W(-1) in a hybrid photodetector that consists of monolayer or bilayer graphene covered with a thin film of colloidal quantum dots. Strong and tunable light absorption in the quantum-dot layer creates electric charges that are transferred to the graphene, where they recirculate many times due to the high charge mobility of graphene and long trapped-charge lifetimes in the quantum-dot layer. The device, with a specific detectivity of 7 × 10(13) Jones, benefits from gate-tunable sensitivity and speed, spectral selectivity from the short-wavelength infrared to the visible, and compatibility with current circuit technologies.

The ability to manipulate optical fields and the energy flow of light is central to modern information and communication technologies, as well as quantum information processing schemes. However, because photons do not possess charge, a way of controlling them efficiently by electrical means has so far proved elusive. A promising way to achieve electric control of light could be through plasmon polaritons—coupled excitations of photons and charge carriers—in graphene. In this two-dimensional sheet of carbon atoms, it is expected that plasmon polaritons and their associated optical fields can readily be tuned electrically by varying the graphene carrier density. Although evidence of optical graphene plasmon resonances has recently been obtained spectroscopically, no experiments so far have directly resolved propagating plasmons in real space. Here we launch and detect propagating optical plasmons in tapered graphene nanostructures using near-field scattering microscopy with infrared excitation light. We provide real-space images of plasmon fields, and find that the extracted plasmon wavelength is very short—more than 40 times smaller than the wavelength of illumination. We exploit this strong optical field confinement to turn a graphene nanostructure into a tunable resonant plasmonic cavity with extremely small mode volume. The cavity resonance is controlled in situ by gating the graphene, and in particular, complete switching on and off of the plasmon modes is demonstrated, thus paving the way towards graphene-based optical transistors. This successful alliance between nanoelectronics and nano-optics enables the development of active subwavelength-scale optics and a plethora of nano-optoelectronic devices and functionalities, such as tunable metamaterials, nanoscale optical processing, and strongly enhanced light–matter interactions for quantum devices and biosensing applications.

Controlling the energy flow processes and the associated energy relaxation rates of a light emitter is of high fundamental interest, and has many applications in the fields of quantum optics, photovoltaics, photodetection, biosensing and light emission. While advanced dielectric and metallic systems have been developed to tailor the interaction between an emitter and its environment, active control of the energy flow has remained challenging. Here, we demonstrate in-situ electrical control of the relaxation pathways of excited erbium ions, which emit light at the technologically relevant telecommunication wavelength of 1.5 µm. By placing the erbium at a few nanometres distance from graphene, we modify the relaxation rate by more than a factor of three, and control whether the emitter decays into either electron-hole pairs, emitted photons or graphene near-infrared plasmons, confined to <15 nm to the sheet. These capabilities to dictate optical energy transfer processes through electrical control of the local density of optical states constitute a new paradigm for active (quantum) photonics.Spontaneous emission constitutes a canonical example of energy flow from an excited light emitter into its environment, where energy relaxation takes place via photon emission. Alternatively, for an emitter in the vicinity of a solid, energy relaxation can occur through channels involving electronic excitations, such as electron-hole pairs and collective charge oscillations (plasmons). Tailoring spontaneous emission by modifying the local density of optical states (LDOS), which governs the emitter-environment interactions [1,2], has been achieved using, amongst others, optical cavities [3][4][5][6], photonic crystals [7,8], and metallic nanostructures [9]. In these systems the LDOS available for the light emitters is typically a fixed property that depends only on the type and geometry of the material system. Here, we control electrically and in-situ the local density of optical states and therefore the energy relaxation rate of a nearby emitter, by employing graphene. Specifically, we demonstrate in-situ tuning of the magnitude and character of the energy transfer pathways from optically excited erbium ions -emitters for near-infrared light that are used as a gain medium in telecommunication applications [10,13]. This control enables new avenues in a range of fields, covering photovoltaics [11,12] The ability to control in-situ the LDOS requires a material for which the optical excitations that occur for a specific emission energy can be modified. Because graphene is gapless and it has a Fermi energy that is electrostatically tunable up to optical energies of ∼1 eV, it can effectively behave as a semiconductor, a dielectric, or a metal. Here, we propose to use these material characteristics to electrically control the relaxation rate and energy transfer processes of a dipolar emitter at subwavelength distance from the graphene. The concept of our experiment is shown in Fig. 1a, schematically representing the gate-tunable ener...

Multi-µJ narrow-bandwidth (≈ 10 cm(-1)) picosecond pulses, broadly tunable in the visible-UV range (320-520 nm), are generated by spectral compression of femtosecond pulses emitted by an amplified Ti:sapphire system. Such pulses provide the ideal Raman pump for broadband femtosecond stimulated Raman spectroscopy, as here demonstrated on a heme protein.

The photoresponse of graphene at mid-infrared frequencies is of high technological interest and is governed by fundamentally different underlying physics than the photoresponse at visible frequencies, as the energy of the photons and substrate phonons involved have comparable energies. Here, we perform a spectrally resolved study of the graphene photoresponse for mid-infrared light by measuring spatially resolved photocurrent over a broad frequency range (1000-1600 cm(-1)). We unveil the different mechanisms that give rise to photocurrent generation in graphene on a polar substrate. In particular, we find an enhancement of the photoresponse when the light excites bulk or surface phonons of the SiO2 substrate. This work paves the way for the development of graphene-based mid-infrared thermal sensing technology.

We study plasmonic nanoantennas for molecular sensing in the mid-infrared made of heavily doped germanium, epitaxially grown with a bottom-up doping process and featuring free carrier density in excess of 1020 cm−3. The dielectric function of the 250 nm thick germanium film is determined, and bow-tie antennas are designed, fabricated, and embedded in a polymer. By using a near-field photoexpansion mapping technique at λ = 5.8 μm, we demonstrate the existence in the antenna gap of an electromagnetic energy density hotspot of diameter below 100 nm and confinement volume 105 times smaller than λ3

Cell membranes are intrinsically heterogeneous, as the local protein and lipid distribution is critical to physiological processes. Even in template systems embedding a single protein type, like purple membranes, there can be a different local response to external stimuli or environmental factors, resulting in heterogeneous conformational changes. Despite the dramatic advances of microspectroscopy techniques, the identification of the conformation heterogeneity is still a challenging task. Tip-enhanced infrared nanospectroscopy is here used to identify conformational changes connected to the hydration state of the transmembrane proteins contained in a 50 nm diameter cell membrane area, without the need for fluorescent labels. In dried purple membrane monolayers, areas with fully hydrated proteins are found among large numbers of molecules with randomly distributed hydration states. Infrared nanospectroscopy results are compared to the spectra obtained with diffraction-limited infrared techniques based on the use of synchrotron radiation, in which the diffraction limit still prevents the observation of nanoscale heterogeneity.

By use of resonantly-enhanced mechanical photoexpansion technique we have performed mid-infrared vibrational spectroscopy and imaging on the nanoscale of individual purple membranes deposited on ultraflat gold substrate. The observed Amide I and Amide II bands of proteins are in good agreement with the far-field infrared transmission spectra previously collected on large numbers of membranes. A comparison between the near-field signal of single purple membranes and that of two overlapping membranes is presented. The results are discussed by adopting simple thermal and electromagnetic considerations