We demonstrate sensitive electric field measurements by coherent homodyne amplification of the electric field induced second harmonic generation (E-FISH) technique. In the process of E-FISH, an applied electric field breaks the centrosymmetry of an otherwise homogeneous medium, in turn promoting the generation of the second harmonic frequency of an incident field. Due to weak third-order hyperpolarizability and the requirement of an applied field to break the symmetry, the E-FISH technique has been mainly used to study high fields, also requiring a strong optical field and sensitive detection. Here we superimpose the E-FISH signal with an auxiliary beam, also termed a local oscillator (LO), at double the incident frequency. Coherent superposition of the LO and the E-FISH output (LOE-FISH) allows for a homodyne amplification of the otherwise weak nonlinear signal. We have demonstrated an increase of signal-to-noise by a factor of seven, which results in a measurement time reduction of a factor of 49. This technique, LOE-FISH, has a number of advantages: detection with intensified detectors is not required. Furthermore, instead of millijoule pulsed lasers, we can work with microjoule pulsed lasers, which allows measuring at repetition rates of megahertz and opens single shot and real-time capability. The LOE-FISH technique increases in sensitivity at lower electric field values. Our work is a demonstration of the principle. Already with our first results from the demonstration, one can see the high potential of LOE-FISH.
Employing electro-optic sampling (EOS) with ultrashort probe pulses, recent experiments showed direct measurements of quantum vacuum fields and their correlations on subcycle timescales. Here, we propose a quantum-enhanced EOS where bright photon-number entangled twin beams are used to derive conditioned nonclassical probes. In the case of the quantum vacuum, this leads to a sixfold improvement in the signal-to-noise ratio over the classically probed EOS. In addition, engineering of the conditioning protocol yields a reliable way to extract higher-order moments of the quantum noise distribution and robust discrimination of the input quantum states, for instance, a vacuum and a few-photon cat state. These improvements open a viable route toward robust tomography of quantum fields in space-time, an equivalent of homodyne detection in energy-momentum space, and the possibility of precise experiments in real-space quantum electrodynamics.
The nonlinear transformation of fluctuations by frequency broadening is found to produce strong anti-correlations in the spectral output. This effect is investigated by dispersive Fourier transform measurements. We exploit the anti-correlations in order to cancel the intensity noise in a subsequent sum-frequency mixing step. This principle allows for the generation of tunable visible pulses by cascaded nonlinear mixing whilst maintaining the same intensity noise performance as the input pulses. In addition, we demonstrate that the power fluctuations occurring in the process of passive stabilization of the carrier-envelope phase locking via difference frequency generation may be cancelled by an analogous strategy.
Recent demonstrations of passively phase-locked fiber-based combs motivate broadband characterization of the noise associated with the stabilized carrier-envelope offset frequency. In our study, we analyze the phase noise of a 100 MHz Er:fiber system in a wide range spanning from microhertz to the Nyquist frequency. An interferometric detection method enables analysis of the high-frequency output of an f-to-2f interferometer. The dominant contribution of a broadband white noise floor at high frequencies attests quantum-limited performance. An out-of-loop measurement of the carrier-envelope phase reveals its jitter to be as low as 250 mrad when integrated over 12 orders of magnitude of the radio-frequency spectrum.
'Blinking', or 'fluorescence intermittency', refers to a random switching between 'ON' (bright) and 'OFF' (dark) states of an emitter; it has been studied widely in zero-dimensional quantum dots and molecules, and scarcely in one-dimensional systems. A generally accepted mechanism for blinking in quantum dots involves random switching between neutral and charged states (or is accompanied by fluctuations in charge-carrier traps), which substantially alters the dynamics of radiative and non-radiative decay. Here, we uncover a new type of blinking effect in vertically stacked, two-dimensional semiconductor heterostructures, which consist of two distinct monolayers of transition metal dichalcogenides (TMDs) that are weakly coupled by van der Waals forces. Unlike zero-dimensional or one-dimensional systems, two-dimensional TMD heterostructures show a correlated blinking effect, comprising randomly switching bright, neutral and dark states. Fluorescence cross-correlation spectroscopy analyses show that a bright state occurring in one monolayer will simultaneously lead to a dark state in the other monolayer, owing to an intermittent interlayer carrier-transfer process. Our findings suggest that bilayer van der Waals heterostructures provide unique platforms for the study of charge-transfer dynamics and non-equilibrium-state physics, and could see application as correlated light emitters in quantum technology.
The interaction of intense near- and mid-infrared laser pulses with rare gases has produced bursts of radiation with spectral content extending into the extreme ultraviolet and soft x-ray region of electromagnetic spectrum. On the other end of the spectrum, laser-driven gas plasmas has been shown to produce coherent sub-harmonic optical waveforms, covering from terahertz (THz) to mid- and near-infrared frequency spectral band. Both processes can be enhanced via a combination of a driving field and its second harmonic. Despite this striking similarity, only limited experimental and theoretical attempts have been made to address these two regimes simultaneously. Here we present systematic experiments and a unifying picture of these processes, based on our extension of the semi-classical three-step model. Further understanding of the generation and coherent control of time-synchronized transients with photon energies from meV to 1 keV can lead to numerous technological advances and to an intriguing possibilities of ultra-broadband investigations into complex condensed matter systems.
The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.
This review discusses the progress and ongoing efforts in optical refrigeration. Optical refrigeration is a process in which phonons are removed from a solid by anti-Stokes fluorescence. The review first summarizes the history of optical refrigeration, noting the success in cooling rare-earth-doped solids to cryogenic temperatures. It then examines in detail a four-level model of rare-earth-based optical refrigeration. This model elucidates the essential roles that the various material parameters, such as the spacing of the energy levels and the radiative quantum efficiency, play in the process of optical refrigeration. The review then describes the experimental techniques for cryogenic optical refrigeration of rare-earth-doped solids employing non-resonant and resonant optical cavities. It then examines the work on laser cooling of semiconductors, emphasizing the differences between optical refrigeration of semiconductors and rare-earth-doped solids and the new challenges and advantages of semiconductors. It then describes the significant experimental results including the observed optical refrigeration of CdS nanostructures. The review concludes by discussing the engineering challenges to the development of practical optical refrigerators, and the potential advantages and uses of these refrigerators.
We report a robust method of coherent detection of broadband THz pulses using terahertz induced second-harmonic (TISH) generation in a laser induced air plasma together with a controlled second harmonic optical bias. We discuss a role of the bias field and its phase in the process of coherent detection. Phase-matching considerations subject to plasma dispersion are also examined.
We investigated the effect of rare earth impurities on the cooling efficiency of Yb³âº:LiYF4 (Yb:YLF). The refrigeration performance of two single crystals, doped with 5%-at. Yb and with identical history but with different amount of contaminations, have been compared by measuring the cooling efficiency curves. Spectroscopic and elemental analyses of the samples have been carried out to identify the contaminants, to quantify their concentrations and to understand their effect on the cooling efficiencies. A model of energy transfer processes between Yb and other rare earth ions is suggested, identifying Erbium and Holmium as elements that produce a detrimental effect on the cooling performance.
Fluorides/chemistry , Lithium Compounds/chemistry , Optical Phenomena , Refrigeration , Ytterbium/chemistry , Yttrium/chemistry , Crystallization , Energy Transfer , Ions , Models, Theoretical , Spectrometry, Fluorescence , Spectroscopy, Near-Infrared
A 7% Yb:YLF crystal is laser cooled to 131 ± 1 K from room temperature by placing it inside the external cavity of a high power InGaAs/GaAs VECSEL operating at 1020 nm with 0.15 nm linewidth. This is the lowest temperature achieved in the intracavity geometry to date and presents major progress towards realizing an all-solid-state compact optical cryocooler.
We report on bulk optical refrigeration of Yb:YLF crystal to a temperature of ~124 K, starting from the ambient. This is achieved by pumping the E4-E5 Stark multiplet transition at ~1020 nm. A lower temperature of 119±1 K (~-154C) with available cooling power of 18 mW is attained when the temperature of the surrounding crystal is reduced to 210 K. This result is within only a few degrees of the minimum achievable temperature of our crystal and signifies the bulk solid-state laser cooling below the National Institute of Standards and Technology (NIST)-defined cryogenic temperature of 123 K.
We present analytical considerations of "self-mode-locked" operation in a typical vertical external-cavity surface-emitting laser (VECSEL) cavity geometry by means of Kerr lens action in the semiconductor gain chip. We predict Kerr-lens mode-locked operation for both soft- and hard-apertures placed at the optimal intra-cavity positions. These predictions are experimentally verified in a Kerr-lens mode-locked VECSEL capable of producing pulse durations of below 500 fs at 1 GHz repetition rate.
Minimum achievable temperature of ~110 K is measured in a 5% doped Yb:YLF crystal at λ = 1020 nm, corresponding to E4-E5 resonance of Stark manifold. This measurement is in excellent agreement with the laser cooling model and was made possible by employing a novel and sensitive implementation of differential luminescence thermometry using balanced photo-detectors.
We demonstrate cooling of a 2 micron thick GaAs/InGaP double-heterostructure to 165 K from ambient using an all-solid-state optical refrigerator. Cooler is comprised of Yb(3+)-doped YLF crystal, utilizing 3.5 Watts of absorbed power near the E4-E5 Stark manifold transition.
Lasers, Solid-State , Optical Fibers , Refrigeration/instrumentation , Semiconductors/instrumentation , Models, Theoretical , Pancreatitis-Associated Proteins , Thermodynamics
