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Optics Express

Invasive optical pumping for room-temperature masers, time-resolved EPR, triplet-DNP, and quantum engines exploiting strong coupling

Hao Wu, Shamil Mirkhanov, Wern Ng, Kuan‐Cheng Chen, Yuling Xiong, Mark Oxborrow

Published Sep 2, 2020• 6 citations
Publisher

Abstract

We explore an approach for optically pumping a body of optically dense magnetic material. This challenge arises in time-resolved electron paramagnetic resonance (TREPR), triplet-based dynamic nuclear polarisation (DNP), and cavity QED. Crystals of pentacene-doped p-terphenyl were grown around variously shaped ends of optical waveguides, through which pump light could be injected deeply into the crystal. When incorporated into a maser as the gain medium, we found that, compared to conventional side-pumping, 11 times less pump beam intensity was needed to reach the masing threshold and 54 times more pulse energy could be absorbed by the gain medium without damage, resulting in a record peak output power of -5 dBm.

DOI
10.1364/oe.401294

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We explore an approach for optically pumping a body of optically dense magnetic material. This challenge arises in time-resolved electron paramagnetic resonance (TREPR), triplet-based dynamic nuclear polarisation (DNP), and cavity QED. Crystals of pentacene-doped p-terphenyl were grown around variously shaped ends of optical waveguides, through which pump light could be injected deeply into the crystal. When incorporated into a maser as the gain medium, we found that, compared to conventional side-pumping, 11 times less pump beam intensity was needed to reach the masing threshold and 54 times more pulse energy could be absorbed by the gain medium without damage, resulting in a record peak output power of -5 dBm.
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.
Masers can deliver ultralow-noise amplification of microwave signals in medical imaging and deep-space communication, with recent research being rekindled through the discovery of gain media operating at room-temperature, eschewing bulky cryogenics that hindered their use. This work shows the discovery of 6,13-diazapentacene doped in para-terphenyl (DAP:PTP) as a maser gain medium that can operate at room-temperature, without an external magnetic field. With a maser output power of -10 dBm, it is on par with pentacene-doped para-terphenyl in masing power, while possessing compelling advantages such as faster amplification startup times, being pumped by longer wavelength light at 620 nm and greater chemical stability from nitrogen groups. Furthermore, the maser bursts from DAP:PTP allow one to reach the strong coupling regime for cavity quantum electrodynamics, with a high cooperativity of 182. The optical and microwave spin dynamics of DAP:PTP are studied in order to evaluate its capabilities as a maser gain medium, where it features fast intersystem crossing and an advantageously higher triplet quantum yield. The results pave the way for the future discovery of similar maser materials and help designate them as promising candidates for quantum sensors, optoelectronic devices and the study of cavity quantum electrodynamic effects at room-temperature.
Though the performance of room-temperature masers has improved over the last decade, relatively little attention has been paid to the optics used to pump the maser's gain medium. In this work, we investigate a novel multi-blade optical ``injector'' that permits more effective and more scaleable pumping. The reported work encompasses an interdisciplinary mix of conceptualization, simulation, crystal growth, fabrication, and microwave engineering. Our gain medium is pentacene dissolved as a solid solution with para-terphenyl (Pc:PTP) molecular crystal. We accurately determine this pentacene's molecular absorption cross-section as a function of wavelength. Ray-tracing is then used to assess how different designs of waveguide inject light into the Pc:PTP crystal. A multi-blade injector made of high-refractive-index glass (namely Ohara S-TIH6) is predicted to pump it more completely and uniformly than previous designs. Upon hand-fabricating such an injector and Bridgman-growing a crystal of 0.1% Pc:PTP over it, an experimental maser oscillator using this combined injector-crystal assembly is demonstrated. The performance and scaleability of multiblade injection vis-a-vis alternative strategies is analyzed.
Through their ability to achieve cryogenic levels of noise performance while operating at room temperature, optically-pumped, solid-state (OPSS) masers show great promise as quantum sensors, oscillators, and amplifiers. We here demonstrate maser oscillation in a microwave cavity containing a crystal of pentacene-doped para-terphenyl (ptc:ptp) pumped by a single, chip-scale LED. Here, unlike previous work, the size of the pump source does not dominate the size of the maser system as a whole. This miniaturization is achieved through invasive optical pumping in the form of a waveguide, the tip of which is embedded into the maser crystal. Using experimental measurements combined with microwave and optical simulations, we find that our approach offers at least a factor-of-2 enhancement in cooperativity over end-on optical excitation. We use our simulations to define a figure of merit for maser pumping efficiency, and conclude that there remains significant headroom to improve the performance of ptc:ptp masers through improved optical design.
Masers, the microwave analogs 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 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.
Molecular materials that enable coherent control over an electron's spin state at room temperature are promising candidates for quantum technologies, including quantum sensors and ultra-low noise microwave amplifiers, known as masers. Host-guest molecular crystals enable independent control of spin-active guests and their local environments to enhance molecular spin properties and so improve device performance. Using electron paramagnetic resonance and optically-detected magnetic resonance, we demonstrate the ability to tune triplet population, depopulation, and spin-lattice relaxation by modulating host-dependent lattice rigidity and vibrational coupling to significantly reduce the operating requirements for building useful masers. Importantly, the most rigid host, picene, reveals the ability to slow spin-lattice relaxation without lengthening triplet lifetime, though at the cost of strain-induced line width broadening and reduced triplet spin polarisation. We also find that deuteration reduces the triplet resonance line width and vibrationally-mediated triplet depopulation. Consequently, we find that perdeuterated pentacene in perdeuterated p-terphenyl is the most viable candidate for building a continuous wave maser. This work demonstrates host-guest engineering as an important and practical method for tuning the spin-dependent performance of room-temperature molecular quantum technologies.