The rich internal structure and long-range dipole-dipole interactions establish polar molecules as unique instruments for quantumcontrolled applications and fundamental investigations. Their potential fully unfolds at ultracold temperatures, where a plethora of effects is predicted in many-body physics [1,2], quantum information science [3,4], ultracold chemistry [5,6], and physics beyond the standard model [7,8]. These objectives have inspired the development of a wide range of methods to produce cold molecular ensembles [9][10][11][12][13][14]. However, cooling polyatomic molecules to ultracold temperatures has until now seemed intractable. Here we report on the experimental realization of opto-electrical cooling [15], a paradigm-changing cooling and accumulation method for polar molecules. Its key attribute is the removal of a large fraction of a molecule's kinetic energy in each step of the cooling cycle via a Sisyphus effect, allowing cooling with only few dissipative decay processes. We demonstrate its potential by reducing the temperature of about 10 6 trapped CH 3 F molecules by a factor of 13.5, with the phase-space density increased by a factor of 29 or a factor of 70 discounting trap losses. In contrast to other cooling mechanisms, our scheme proceeds in a trap, cools in all three dimensions, and works for a large variety of polar molecules. With no fundamental temperature limit anticipated down to the photon-recoil temperature in the nanokelvin range, our method eliminates the primary hurdle in producing ultracold polyatomic molecules. The low temperatures, large molecule numbers and long trapping times up to 27 s will allow an interaction-dominated regime to be attained, enabling collision studies and investigation of evaporative cooling toward a BEC of polyatomic molecules.The ability to prepare ultracold molecular ensembles has an application potential akin to that of ultracold atoms some decades ago. In fact, the association of KRb dimers [16] as well as the laser cooling of SrF [17] has brought fascinating physics within reach. However, both approaches are restricted to a highly specialized set of purely diatomic molecule species. In order to investigate fundamental physics based on relativistic effects near heavy nuclei or parity violation effects in chiral molecules, or to study molecules of astrophysical, biological, or chemical interest, a more general approach to preparing ultracold molecular ensemble is imperative. This holds in particular for the rich chemical variety of carbon-, nitrogen-, or oxygen-based molecules for which the constituent atoms have not even been laser cooled. Devising a dissipative process to cool such molecules into the ultracold regime has been an exceedingly challenging problem. The standard approach for atoms, laser cooling, is in general impossible for molecules due to the lack of suitable cycling transitions. Creating an artificial cycling transition via cavity cooling [18] has not been demonstrated despite substantial experimental [19] and theoretical [20][21][...
We present a method which delivers a continuous, high-density beam of slow and internally cold polar molecules. In our source, warm molecules are first cooled by collisions with a cryogenic helium buffer gas. Cold molecules are then extracted by means of an electrostatic quadrupole guide. For ND3 the source produces fluxes up to (7± 7 4 ) × 10 10 molecules/s with peak densities up to (1.0± 1.0 0.6 ) × 10 9 molecules/cm 3 . For H2CO the population of rovibrational states is monitored by depletion spectroscopy, resulting in single-state populations up to (82 ± 10)%.
The performance of organic thin-film transistors (OTFT) for flexible, low cost and disposable "plastic" electronic products advances rapidly: various organic semiconductors display hole or electron carrier mobilities [1] that compare favorably with those of hydrogenated amorphous silicon, [2] the inorganic counterpart for such applications as flexible displays, [3,4] smart cards and radio frequency identification tags, [5,6] nonvolatile memories [7] and sensors. [8,9] The possibility for tailoring functional organic materials, bears potential towards novel electronic products such as smart skins, [10] smart textiles [11] and "invisible electronics", [12] where multiple functionalities, portability and ubiquitous integration is requested. In this context diverse properties of organic thin-film devices are inevitable such as lightweight, low power consumption, low operationvoltage and compatibility with diverse substrates.[12]Reducing the threshold voltage and the subthreshold swing is essential for operating OTFTs at low-voltage levels. When combined with very low gate leakage currents, OTFTs may also become a key element in high-end sensor applications, such as flexible touch pads and screens or thermal imaging tools for night vision, surveillance or for the detection of undesired heat loss paths in buildings.The aforementioned transistor parameters not only critically depend on the thickness and the dielectric properties of the gate insulator, [12][13][14] but also on the trapped charge densities at the interface between these materials. The selection of semiconductors and gate insulators with excellent interface properties is currently the challenge in the quest for improving the performance of OTFTs.Here we show that bottom-gate OTFTs based on the organic semiconductor pentacene and high-k nanocomposite gate dielectrics, exhibit transistor performances with very low gate leakage currents, subthreshold swings close to the theoretical limit, and low-voltage battery operation. The subthreshold swings of OTFTs with different organic and hybrid gate dielectrics follow an inverse dependence on the gate capacitance as is expected by standard MOS theory. The trapped charge carrier density at the interface between the semiconductor and the dielectric surpasses that of the SiO 2 -pentacene interface, being close to the average trap densities in the SiO 2 -Si interface in metal oxide semiconductor transistors. [15] We also report the first application of these OTFTs in an optothermal light sensor. We describe the transistor, the temperature sensitive fluorinated polymer, their combination in an integrated circuit, and the application of this circuit as a thermal infrared sensor and as a switch that can be operated by a laser pointer. Figure 1 shows the structure of low-voltage organic transistors with high dielectric constant (high-k) oxide-polymer nanocomposites. Al 2 O 3 or ZrO 2 were chosen as high-k dielectric materials, combined with poly(a-methyl styrene) (PaMS) or poly(vinyl cinnamate) (PVCi) to form a smooth and ...
We investigate the interaction between light and molecular systems modelled as quantum emitters coupled to a multitude of vibrational modes via a Holstein-type interaction. We follow a quantum Langevin equations approach that allows for analytical derivations of absorption and fluorescence profiles of molecules driven by classical fields or coupled to quantized optical modes. We retrieve analytical expressions for the modification of the radiative emission branching ratio in the Purcell regime and for the asymmetric cavity transmission associated with dissipative cross-talk between upper and lower polaritons in the strong coupling regime. We also characterize the Förster resonance energy transfer process between donor-acceptor molecules mediated by the vacuum or by a cavity mode.PACS numbers: 05.60.Gg, 37.30.+i, 81.05.Fb Recent experimental progress [1] has shown that the Purcell enhancement of the zero-phonon line of a single molecule can strongly alter the branching ratio of spontaneous emission between the line of interest and additional Stokes lines thus turning the molecule into an ideal quantum emitter. At the mesoscopic level, experiments in the collective strong coupling regime of organic molecules with cavities or delocalized plasmonic modes have shown important light-induced modifications of material properties. Experimental and theoretical endeavors go into the direction of charge and energy transport enhancement [2-6], Förster resonance energy transfer (FRET) enhancement [7][8][9][10][11], modified chemical reactivity [12][13][14][15][16], polariton dynamics [17,18] etc. Oftentimes however, experiments rely on theoretical models developed for standard cavity quantum electrodynamics (cavity QED) [19][20][21] with two-level systems where one distinguishes between i) the Purcell regime, characterized by modifications of the spontaneous emission rates and ii) the strong coupling regime leading to the occurrence of hybrid light-matter states referred to as polaritons. Recent theoretical efforts aim at covering this gap by solving a generalized light-electronic-vibrations problem modeled as a Holstein-Tavis-Cummings Hamiltonian. Investigations aim at providing an understanding of the vibrationally induced cavity polariton asymmetry [18,22], vibrationally dressed polaritons [23], dark vibronic polaritons [24,25], developing a cavity Born-Oppenheimer theory [26,27] or deriving relevant simplified models for large scale numerics in the mesoscopic limit [28].We provide here an alternative path based on solving the Holstein-Tavis-Cummings dynamics at the level of operators rather than states. The basic model considers a molecular box (see Fig. 1(b)) comprised of an internal electronic transition coupled to any number of vibrational modes. Radiative decay and vibrational relaxation are included as stochastic source terms in a set of coupled standard quantum Langevin equations [29][30][31][32][33] for vibrational and polaron operators (similarly applied in optomechanical systems [34][35][36]). The method is nu...
Many-body correlations govern a variety of important quantum phenomena such as the emergence of superconductivity and magnetism. Understanding quantum many-body systems is thus one of the central goals of modern sciences. Here we demonstrate an experimental approach towards this goal by utilizing an ultracold Rydberg gas generated with a broadband picosecond laser pulse. We follow the ultrafast evolution of its electronic coherence by time-domain Ramsey interferometry with attosecond precision. The observed electronic coherence shows an ultrafast oscillation with a period of 1 femtosecond, whose phase shift on the attosecond timescale is consistent with many-body correlations among Rydberg atoms beyond mean-field approximations. This coherent and ultrafast many-body dynamics is actively controlled by tuning the orbital size and population of the Rydberg state, as well as the mean atomic distance. Our approach will offer a versatile platform to observe and manipulate non-equilibrium dynamics of quantum many-body systems on the ultrafast timescale.
We present a versatile electric trap for the exploration of a wide range of quantum phenomena in the interaction between polar molecules. The trap combines tunable fields, homogeneous over most of the trap volume, with steep gradient fields at the trap boundary. An initial sample of up to 10(8), CH(3)F molecules is trapped for as long as 60 s, with a 1/e storage time of 12 s. Adiabatic cooling down to 120 mK is achieved by slowly expanding the trap volume. The trap combines all ingredients for opto-electrical cooling, which, together with the extraordinarily long storage times, brings field-controlled quantum-mechanical collision and reaction experiments within reach.
We provide a fully analytical treatment for the partial refrigeration of the thermal motion of a quantum mechanical resonator under the action of feedback. As opposed to standard cavity optomechanics where the aim is to isolate and cool a single mechanical mode while the object's overall temperature is largely unaltered, the aim here is to simultaneously extract the thermal energy from many of its vibrational modes. We consider a standard cold-damping technique where homodyne read-out of the cavity output field is fed into a feedback loop that provides a cooling action directly applied on the mechanical resonator. Analytical and numerical results predict that low final occupancies are achievable independently on the number of modes addressed by the feedback as long as the cooling rate is smaller than the intermode frequency separation. For resonators exhibiting nearly degenerate pairs of modes cooling is less efficient and a weak dependence on the number of modes is obtained. These scalings hint towards the design of frequency resolved mechanical resonators where efficient refrigeration is possible via simultaneous cold-damping feedback. arXiv:1908.07348v1 [quant-ph]
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