Search

Color centers, which are point defects in crystals, play a crucial role in altering the optical properties of their host materials, enabling widespread applications in the field of quantum information processing. While the majority of the state-of-the-art color centers are inorganic, they come with limitations such as the challenging material preparations and insufficient amount of available centers. In contrast, organic color centers have recently gained attention due to their ease of preparations and tailorable functionalities. Here, pentacene-doped p-terphenyl (Pc:Ptp), an organic color-center system normally used for microwave quantum electronics, is demonstrated for the first time its ability of self-cavity laser emission at room temperature. The laser emission is characterized by strong polarization and high anisotropy, attributed to the unique packing of the color-center molecules within the crystal. The optical coherence is found to be a figure of merit to distinguish the processes of the amplified spontaneous emission (ASE) and lasing in Pc:Ptp. This work highlights the potential of Pc:Ptp as a compact and efficient platform for light-matter interactions , offering significant promise for enhancing the performance of solid-state quantum devices based on this organic color-center system., Comment: 21 pages,9 figures(including supplementary information)

Future information processing technologies like quantum memory devices have the potential to store and transfer quantum states to enable quantum computing and networking. A central consideration in practical applications for such devices is the nature of the light-matter interface which determines the storage state density and efficiency. Here, we employ an organic radical, $\alpha$,$\gamma$-bisdiphenylene-$\beta$-phenylallyl (BDPA) doped into an o-terphenyl host to explore the potential for using tuneable and high-performance molecular media in microwave-based quantum applications. We demonstrate that this radical system exhibits millisecond-long spin-lattice relaxation and microsecond-long phase memory times at room temperature, while also having the capability to generate an oscillating spin-polarized state using a co-dissolved photo-activated tetraphenylporphyrin moiety, all enabled by using a viscous liquid host. This latest system builds upon collective wisdom from previous molecules-for-quantum literature by combining careful host matrix selection, with dynamical decoupling, and photoexcited triplet-radical spin polarisation to realise a versatile and robust quantum spin medium.

We introduce a method, which we here name ``active pre-cooling'' (APC), for removing, just prior to performing a measurement, a large fraction of the deleterious thermal photons that would otherwise occupy the electromagnetic modes of a microwave cavity or some alternative form of radio-frequency resonator. The removal is achieved by temporarily over-coupling the cavity's modes to an active cold load (ACL). We report a room-temperature bench-top demonstration of the method, where this load takes the form of the input of a commercial low-noise amplifier (LNA). No isolator is inserted between the LNA's input and the cavity's coupling port. The noise temperature of a monitored microwave mode drops to 123 K. Upon incorporating our pre-coolable cavity into a time-resolved (tr-) EPR spectrometer, a commensurate improvement in the signal-to-noise ratio is observed, corresponding to a factor-of-5 speed up over a conventional tr-EPR measurement at room temperature for the same precision and/or sensitivity. Modeling indicates the feasibility, for realistic mode quality factors and couplings, of cooling the room-temperature cavity's modes down to a few tens of K, and for this coldness to last several tens of s, whilst the cavity and its contents are optimally interrogated by a microwave tone or pulse sequence. The method thus provides a simple and generally applicable approach to improving the sensitivity and/or read-out speed in pulsed and time-resolved EPR spectroscopy, quantum detection and other radiometric measurements. It provides a first-stage cold reservoir (of microwave photons) for other, deeper cooling methods to work from and, through the use of cryogenic ACLs (realized, in the first instance, as the inputs of existing cryogenic low-noise amplifiers), the method could itself be directly extended to lower temperature regimes., Comment: 22 pages, 18 figures, 2 tables (including Supplemental Information)

High-accuracy microwave sensing is widely demanded in various fields, ranging from cosmology to microwave quantum technology. Quantum receivers based on inorganic solid-state spin systems are promising candidates for such purpose because of the stability and compatibility, but their best sensitivity is currently limited to a few pT/$\sqrt{\rm{Hz}}$. Here, by utilising an enhanced readout scheme with the state-of-the-art solid-state maser technology, we develop a robust microwave quantum receiver functioned by organic molecular spins at ambient conditions. Owing to the maser amplification, the sensitivity of the receiver achieves 6.14 $\pm$ 0.17 fT/$\sqrt{\rm{Hz}}$ which exceeds three orders of magnitude than that of the inorganic solid-state quantum receivers. The heterodyne detection without additional local oscillators improves bandwidth of the receiver and allows frequency detection. The scheme can be extended to other solid-state spin systems without complicated control pulses and thus enables practical applications such as electron spin resonance spectroscopy, dark matter searches, and astronomical observations., Comment: 10 pages, 4 figures

Quantum electronics operating in the microwave domain are burgeoning and becoming essential building blocks of quantum computers, sensors and communication devices. However, the field of microwave quantum electronics has long been dominated by the need for cryogenic conditions to maintain the delicate quantum characteristics. Here we report on a solid-state hybrid system, constituted by a photo-excited pentacene triplet spin ensemble coupled to a dielectric resonator, that is for the first time capable of both coherent microwave quantum amplification and oscillation at X band via the masing process at room temperature. By incorporating external driving and active dissipation control into the hybrid system, we achieve efficient tuning of the maser emission characteristics at around 9.4 GHz, which is key to optimizing the performance of the maser device. Our work not only pushes the boundaries of the operating frequency and functionality of the existing pentacene masers, but also demonstrate a universal route for controlling the masing process at room temperature, highlighting opportunities for optimizing emerging solid-state masers for quantum information processing and communication., Comment: 25+7 pages, 5+3 figures

Masers, the microwave analogues of lasers, have seen a renaissance owing to the discovery of gain media that mase at room-temperature and zero-applied magnetic field. However, despite the ease with which the devices can be demonstrated under ambient conditions, achieving the ubiquity and portability which lasers enjoy has to date remained challenging. We present a maser device with a miniaturized maser cavity, gain material and laser pump source that fits within the size of a shoebox. The gain medium used is pentacene-doped in para-terphenyl and it is shown to give a strong masing signal with a peak power of -5 dBm even within a smaller form factor. The device is also shown to mase at different frequencies within a small range of 1.5 MHz away from the resonant frequency. The portability and simplicity of the device, which weighs under 5 kg, paves the way for demonstrators particularly in the areas of low-noise amplifiers, quantum sensors, cavity quantum electrodynamics and long-range communications.

Coherent sources exploiting the stimulated emission of non-equilibrium quantum systems, i.e. gain media, have proven indispensable for advancing fundamental research and engineering. The operating electromagnetic bands of such coherent sources have been continuously enriched for increasing demands.Nevertheless, for a single bench top coherent source, simultaneous generation of radiation in multiple bands, especially when the bands are widely separated, present formidable challenges with a single gain medium. Here, we propose a mechanism of simultaneously realizing the stimulated emission of radiation in the visible and microwave bands, i.e. lasing and masing actions, at ambient conditions by utilizing photoexcited singlet and triplet states of the pentacene molecules that are doped in p-terphenyl. The possibility is validated by the observed amplified spontaneous emission (ASE) at 645 nm with a narrow linewidth around 1 nm from the pentacene-doped p-terphenyl crystal used for masing at 1.45 GHz and consolidated by a 20 fold lower threshold of ASE compared to the reported masing threshold. The overall threshold of the pentacene-based multiband coherent source can be optimized by appropriate alignment of the pump-light polarization with the pentacene's transition dipole moment. Our work not only shows a great promise on immediate realization of multiband coherent sources but also establishes an intriguing solid-state platform for fundamental research of quantum optics in multiple frequency domains., Comment: 30 pages, 4 figures

Steady-state superradiance and superradiant lasing attract significant attentions in the field of optical lattice clocks, but have not been achieved so far due to the technical challenges and atom loss problem. In this article, we propose that their counter-part may be observed in the microwave domain with solid-state spins-microwave resonator systems at room temperature with realistic technical restrictions. To validate our proposal, we investigate systematically the system dynamics and steady-state by solving quantum master equations for the multi-level and multi-process dynamic of trillions of spins. To this end, we employ a mean-field approach, and convert the mean-field dynamics of the spin ensemble into the one in a more intuitive Dicke state picture. Our calculations show that for systems with nitrogen vacancy center spins and pentacene molecular spins the superradiant Rabi oscillations occur firstly due to transitions among different Dicke states, and the subsequent continuous-wave superradiant masing can achieve a linewidth well below millihertz. Our work may guide further exploration of transient and steady-state superradiant masing with the mentioned and other solid-state spins systems, such as silicon vacancy centers in silicon carbide and boron vacancy centers in hexagonal boron nitride, where the coherent radiation with ultra-narrow linewidth may find applications in deep-space communications, radio astronomy and high-precision metrology., Comment: 16 pages, 8 figures, 1 table

Masers, the microwave analogue of lasers, promise to deliver ultra-low noise amplification of microwave signals for use in medical MRI imaging and deep-space communication. Research on masers in modern times was rekindled thanks to the discovery of gain media that were operable at room-temperature, eschewing bulky cryogenics that hindered their use. However, besides the two known materials of pentacene doped in para-terphenyl and negatively-charged nitrogen-vacancy defects in diamond, there has been scarce progress in the search for completely new room-temperature gain media. Here we show the discovery of 6,13-diazapentacene doped in para-terphenyl as a maser gain medium that can operate at room-temperature and without an external magnetic field. A measured maser pulse power of -10 dBm shows it is on par with pentacene-doped para-terphenyl in absolute power, while possessing compelling advantages against its pentacene predecessor in that it has a faster amplification startup time, can be excited with longer wavelength light at 620 nm and enjoys greater chemical stability from added nitrogen groups. Furthermore, we show that the maser bursts allow 6,13-diazapentacene-doped para-terphenyl to reach the strong coupling regime for cavity quantum electrodynamics, where it has a high cooperativity of 182. We study the optical and microwave spin dynamics of 6,13-diazapentacene-doped para-terphenyl in order to evaluate its behavior as a maser gain medium, where it features fast intersystem crossing and an advantageously higher triplet quantum yield. Our results pave the way for the future discovery of other similar maser materials and help point to such materials as promising candidates for the study of cavity quantum electrodynamic effects at room-temperature., Comment: Main text 16 page, 11 figures. Supplementary has 7 pages, 4 figures

Quantum sensing with solid-state systems finds broad applications in diverse areas ranging from material and biomedical sciences to fundamental physics. Several solid-state spin sensors have been developed, facilitating the ultra-sensitive detection of physical quantities such as magnetic and electric fields and temperature. Exploiting collective behaviour of non-interacting spins holds the promise of pushing the detection limit to even lower levels, while to date, those levels are scarcely reached due to the broadened linewidth and inefficient readout of solid-state spin ensembles. Here, we experimentally demonstrate that such drawbacks can be overcome by newly reborn maser technology at room temperature in the solid state. Owing to maser action, we observe a 4-fold reduction in the inhomogeneously broadened linewidth of a molecular spin ensemble, which is narrower than the same measured from single spins at cryogenic temperatures. The maser-based readout applied to magnetometry showcases a signal-to-noise ratio (SNR) of 30 dB for single shots. This technique would be a significant addition to the toolbox for boosting the sensitivity of solid-state ensemble spin sensors., Comment: 9 pages, 4 figures

We demonstrate the cooling of a microwave mode at 2872 MHz through its interaction with optically spin-polarized NV$^-$ centers in diamond at zero applied magnetic field, removing thermal photons from the mode. By photo-exciting (pumping) a brilliant-cut red diamond jewel with a continuous-wave 532-nm laser, outputting 2 W, the microwave mode is cooled down to a noise temperature of 188 K. This noise temperature can be preserved continuously for as long as the diamond is optically excited and kept cool. The latter requirement restricted operation out to 10 ms in our preliminary setup. The mode-cooling performance of NV$^-$ diamond is directly compared against that of pentacene-doped para-terphenyl, where we find that the former affords the advantages of cooling immediately upon light excitation without needing to mase beforehand (or at all) and being able to cool continuously at substantially lower optical pump power.

We experimentally demonstrate the temporary removal of thermal photons from a microwave mode at 1.45 GHz through its interaction with the spin-polarized triplet states of photo-excited pentacene molecules doped within a p-terphenyl crystal at room temperature. The crystal functions electromagnetically as a narrow-band cryogenic load, removing photons from the otherwise room-temperature mode via stimulated absorption. The noise temperature of the microwave mode dropped to $50^{+18}_{-32}$ K (as directly inferred by noise-power measurements) while the metal walls of the cavity enclosing the mode remained at room temperature. Simulations based on the same system's behavior as a maser (which could be characterized more accurately) indicate the possibility of the mode's temperature sinking to $\sim$10 K (corresponding to $\sim$140 microwave photons). These observations, when combined with engineering improvements to deepen the cooling, identify the system as a narrow-band yet extremely convenient platform -- free of cryogenics, vacuum chambers and strong magnets -- for realizing low-noise detectors, quantum memory and quantum-enhanced machines (such as heat engines) based on strong spin-photon coupling and entanglement at microwave frequencies., Comment: 6 pages, 4 figures

We establish a testbed system for the development of high-sensitivity Electron Spin Resonance (ESR) techniques for small samples at cryogenic temperatures. Our system consists of a Niobium Nitride thin-film planar superconducting microresonator designed to have a concentrated mode volume to couple to a small amount of paramagnetic material, and to be resilient to magnetic fields of up to 400 mT. At 65 mK we measure high-cooperativity coupling ($C \approx 19$) to an organic radical microcrystal containing $10^{12}$ spins in a pico-litre volume. We detect the spin-lattice decoherence rate via the dispersive frequency shift of the resonator. Techniques such as these could be suitable for applications in quantum information as well as for pulsed ESR interrogation of very few spins and could provide insights into the surface chemistry of, for example, the material defects in superconducting quantum processors., Comment: 8 pages 5 figures

We present in this work a quasi-continuous-wave (CW) pentacene maser operating at 1.45 GHz in the Earth's magnetic field at room temperature with a duration of $\sim$4 ms and an output power of up to -25 dBm. The maser is optically pumped by a cerium-doped YAG (Ce:YAG) luminescent concentrator (LC) whose wedge-shaped output is embedded inside a 0.1% pentacene-doped para-terphenyl (Pc:Ptp) crystal. The pumped crystal is located inside a ring of strontium titanate (STO) that supports a TE$_{01\delta}$ mode of high magnetic Purcell factor. Combined with simulations, our results indicate that CW operation of pentacene masers at room-temperature is perfectly feasible so long as excessive heating of the crystal is avoided., Comment: 10 pages, 8 figures

Slow noise processes, with characteristic timescales ~1s, have been studied in planar superconducting resonators. A frequency locked loop is employed to track deviations of the resonator centre frequency with high precision and bandwidth. Comparative measurements are made in varying microwave drive, temperature and between bare resonators and those with an additional dielectric layer. All resonators are found to exhibit flicker frequency noise which increases with decreasing microwave drive. We also show that an increase in temperature results in a saturation of flicker noise in resonators with an additional dielectric layer, while bare resonators stop exhibiting flicker noise instead showing a random frequency walk process., Comment: 4 pages, 2 figures, version 4 http://prb.aps.org/abstract/PRB/v87/i14/e140501

We present a new application and implementation of the so-called Pound locking technique for the interrogation of superconducting microresonators. We discuss how by comparing against stable frequency sources this technique can be used to characterize properties of resonators that can not be accessed using traditional methods. Specifically, by analyzing the noise spectra and the Allan deviation we obtain valuable information about the nature of the noise in superconducting planar resonators. This technique also greatly improves the read-out accuracy and measurement throughput compared to conventional methods., Comment: 5 pages

This article reports on the long-term frequency stabilty characterisation of a new type of cryogenic sapphire oscillator using an autonomous pulse-tube cryocooler as its cold source. This new design enables a relative frequency stability of better than 4.5e-15 over one day of integration. This represents to our knowledge the best long-term frequency stability ever obtained with a signal source based on a macroscopic resonator., Comment: 9 pages, 5 figures

The zero-field Fe3+:sapphire whispering-gallery-mode maser oscillator exhibits several alluring features: Its output is many orders of magnitude brighter than that of an active hydrogen maser and thus far less degraded by spontaneous-emission (Schawlow-Townes) and/or receiving-amplifier noise. Its oscillator loop is confined to a piece of mono-crystalline rock bolted into a metal can. Its quiet amplification combined with high resonator Q provide the ingredients for exceptionally low phase noise. We here concentrate on novelties addressing the fundamental conundrums and technical challenges that impede progress. (1) Roasting: The "mase-ability" of sapphire depends significantly on the chemical conditions under which it is grown and heat-treated. We provide some fresh details and nuances here. (2) Simplification: This paper obviates the need for a Ka-band synthesizer: it describes how a 31.3 GHz loop oscillator, operating on the preferred WG pump mode, incorporating Pound locking, was built from low-cost components. (3) "Dark Matter": A Siegman-level analysis of the experimental data determines the substitutional concentration of Fe3+ in HEMEX to be less than a part per billion prior to roasting and up to a few hundred ppb afterwards. Chemical assays, using different techniques (incl. glow discharge mass spectra spectroscopy and neutron activation analysis) consistently indicate, however, that HEMEX contains iron at concentrations of a few parts per million. Drawing from several forgotten-about/under-appreciated papers, this substantial discrepancy is addressed. (4) Excitons: Towards providing a new means of controlling the Fe3+:sapph. system, a cryogenic sapphire ring was illuminated, whilst masing, with UV light at wavelengths corresponding to known electronic and charge-transfer (thus valence-altering) transitions. Preliminary experiments are reported., Comment: pdf only; submitted to the proceedings of the 24th European Frequency and Time Forum, 13-15th April, 2010

This paper explains how a popular, commercially-available software package for solving partial-differential-equations (PDEs), as based on the finite-element method (FEM), can be configured to calculate, efficiently, the frequencies and fields of the whispering-gallery (WG) modes of axisymmetric dielectric resonators. The approach is traceable; it exploits the PDE-solver's ability to accept the definition of solutions to Maxwell's equations in so-called `weak form'. Associated expressions and methods for estimating a WG mode's volume, filling factor(s) and, in the case of closed(open) resonators, its wall(radiation) loss, are provided. As no transverse approximation is imposed, the approach remains accurate even for quasi-transverse magnetic/electric modes of low, finite azimuthal mode order. The approach's generality and utility are demonstrated by modeling several non-trivial structures: (i) two different optical microcavities [one toroidal made of silica, the other an AlGaAs microdisk]; (ii) a 3rd-order sapphire:air Bragg cavity; (iii) two different cryogenic sapphire WG-mode resonators; both (ii) and (iii) operate in the microwave X-band. By fitting one of (iii) to a set of measured resonance frequencies, the dielectric constants of sapphire at liquid-helium temperature have been estimated., Comment: 10 pages, 8 figures, submitted to IEEE Microwave Theory and Techniques. Last revision March 19 2007. This paper is a significantly abridged/revised version of quant-ph/0607156

It is described, explicitly, how a popular, commercially-available software package for solving partial-differential-equations (PDEs), as based on the finite-element method (FEM), can be configured to calculate the frequencies and fields of the whispering-gallery (WG) modes of axisymmetric dielectric resonators. The approach is traceable; it exploits the PDE-solver's ability to accept the definition of solutions to Maxwell's equations in so-called `weak form'. Associated expressions and methods for estimating a WG mode's volume, filling factor(s) and, in the case of closed(open) resonators, its wall (radiation) loss, are provided. As no transverse approxi-mation is imposed, the approach remains accurate even for so-called quasi-TM and -TE modes of low, finite azimuthal mode order. The approach's generality and utility are demonstrated by modeling several non-trivial structures: (i)two different optical microcavities [one toroidal made of silica, the other an AlGaAs microdisk]; (ii) a 3rd-order microwave Bragg cavity containing alumina layers (iii) two different cryogenic sapphire X-band microwave resonators. By fitting one of the latter to a set of measured resonance frequencies, the dielectric constants of sapphire at liquid-helium temperature have been estimated., Comment: 21 pages, 8 figures, 4 tables; submitted to IEEE Transactions on Microwave Theory and Techniques. Corrected 20th March 2007