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arXiv:2301.01927

Towards simultaneous coherent radiation in the visible and microwave bands with doped molecular crystals

Hao Wu, Tong Li, Zhang‐qi Yin, Jiyang Ma, Xu‐Ri Yao, Bo Zhang, Mark Oxborrow, Qing Zhao

Published Jan 5, 2023• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2301.01927

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Room-temperature MASERs (Microwave Amplification by Stimulated Emission of Radiation) are coherent sources that exploit stimulated emission to amplify electromagnetic waves at microwave frequencies. Here we report the first demonstration of an LED-pumped maser based on photo-excited triplet states of pentacene in p-terphenyl. The LED light is brightness enhanced and guided using a Cerium-doped Yttrium Aluminium Garnet luminescent crystal that uses light recycling to reach record luminance and power levels. We observe stable maser emission at 1.45 GHz using LED pumping at a much lower pump threshold power. This new maser is cost-effective, safe, and environmentally friendly, and hence ensures a wide variety of potential uses, including more sensitive magnetic resonance body scanners, quantum optical coherence tomography, advanced quantum computer components, portable atomic clocks, and better radio astronomy devices for deep space exploration.
Molecular room temperature masers have emerged as promising sources of coherent microwaves, but systematic comparisons of organic gain media under uniform conditions remain limited. This paper presents a characterization of two systems, pentacene doped para terphenyl (Pc:PTP, 1.45 GHz) and 6,13 diazapentacene doped para terphenyl (DAP:PTP, 1.478 GHz), examined at four concentrations, including a new 0.05 percent DAP:PTP sample. By evaluating L band masing media under identical conditions, optimal doping levels and gain materials for high power operation are identified. The optimized system produced room temperature continuous wave masing with a peak output of 2.34 mW (+3.69 dBm), marking the first milliwatt level emission from an organic maser. Spectral coherence times of 465 ns and coherence lengths up to 150 m were obtained. Coupling to a high Q cavity mode enables collective spin photon interactions, with Rabi oscillations revealing coherent ensemble dynamics. Frequency domain analysis shows normal mode splitting of 1.37 MHz for Pc:PTP and 2.14 MHz for DAP:PTP, confirming strong coupling. Cavity QED analysis yields cooperativities C* = 304-803 for Pc:PTP and 405-1071 for DAP:PTP, among the highest for organic systems. Quantitative metrics of signal to noise ratio, spectral coherence distance, and throughput demonstrate the potential of these masers for radar, secure communication, and quantum interface technologies.
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.
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 narrowband cryogenic load, removing photons from the otherwise room-temperature mode via stimulated absorption. The noise temperature of the microwave mode dropped to 50_{-32}^{+18} 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 ∼10 K (corresponding to ∼140 microwave photons). These observations, when combined with engineering improvements to deepen the cooling, identify the system as a narrowband 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.
Abstract Crystal defects in solid‐state spintronic materials play a crucial role in altering the optical properties of their hosts, enabling widespread applications in the field of quantum information processing. While the majority of the leading platforms are inorganic, they come with limitations such as the challenging material preparations and insufficient amount of active spins. Here, pentacene‐doped p‐terphenyl (Pc:Ptp), an organic spintronic material with easy preparations and tailorable functionalities 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 anisotropy, attributed to the unique packing of the doped molecules (i.e., active spins) 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 the organic spintronic material.
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 delicate quantum characteristics. Here, a solid-state hybrid system, constituted by a photo-excited pentacene triplet spin ensemble coupled to a dielectric resonator, is reported 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, efficient tuning of the maser emission characteristics at ≈9.4 GHz is achieved, which is key to optimizing the performance of the maser device. The work not only pushes the boundaries of the operating frequency and functionality of the existing pentacene masers but also demonstrates 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.