arXiv subjects

Max Attwood

Publications and source records attributed to Max Attwood.

12 recordsLinked to original sources

arXiv2026

Host-guest Crystal Engineering Tailors the Room Temperature Spin Dynamics in Molecular Quantum Devices

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.

quant-ph↗

arXiv2026

Heterogeneous Optically-Detected Spin-Acoustic Resonance in Solid-State Molecular Thin-film

We report an implementation of spin-acoustic resonance in pentacene thin films integrated on a high-quality-factor (high-Q) surface acoustic wave (SAW) resonator on a lithium niobate substrate. Heterogeneous optically detected spin-acoustic resonance (HODSAR) is an optically detected spin-resonance measurement in which the resonant drive is delivered mechanically by a surface acoustic wave (SAW). By leveraging the photo-excited triplet state of pentacene at room temperature, we demonstrate coherent spin manipulation via acoustic driving under zero externally applied magnetic field. The heterogeneously integrated device, referred to as HODSAR, utilizes spin-phonon coupling to achieve mechanically driven, zero-field spin resonance, opening avenues for room-temperature mechanically addressable spin control and device integration. We show that the high-Q multimode response of the SAW resonator enables spectrally selective acoustic addressing of triplet transitions near 105 MHz. Coherent control is evidenced by Rabi oscillations, with a Rabi frequency that increases linearly with the square root of the applied RF input power over the measured drive range, consistent with driven two-level dynamics under acoustic excitation. These results establish spin-acoustic resonance in a heterogeneously integrated molecular thin-film platform and provide a quantitative basis for benchmarking mechanically mediated spin control.

quant-ph↗

arXiv2025

Single-LED-pumped, room-temperature, solid-state maser

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.

quant-ph↗

arXiv2025

L-Band Milliwatt Room-Temperature Solid-State Maser

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.

physics.app-ph↗

arXiv2025

Feasibility of Free-Space Transmission using L-Band Maser Signals in Organic Gain Media

Atmospheric conditions such as fog, humidity, and scattering by foliage routinely degrade optical free-space (FS) links, motivating alternatives that are robust in adverse conditions. Coherent microwave sources offer a compelling alternative for quantum-secure communication, yet their propagation outside enclosed resonators has remained untested. Here, we demonstrate room-temperature FS transmission of maser signals generated using organic L-band (1-2 GHz) gain media, pentacene doped p-terphenyl (Pc: PTP), and Diazapentacene-doped p-terphenyl (DAP:PTP). Spectral and temporal coherence is preserved over distances up to 25 cm, approximately one wavelength at the masing frequency. Tests included polarisation misalignment, high-humidity conditions, and partial occlusion by foliage to emulate realistic FS reception scenarios. Strong spin-photon coupling was maintained, as confirmed by persistent rabi oscillations and normal-mode splitting. An instantaneous peak output of 4.29 mW (+6.32 dBm) from a 0.01% DAP:PTP gain medium. with a pulse duration of ~4 {\mu}s, marks a performance benchmark for directly coupled masers. These findings demonstrate a proof-of-concept for masers as viable platforms for short-range, interference-resilient coherent microwave links, with future relevance to quantum sensing and secure communication technologies.

physics.app-ph↗

arXiv2025

Chemically Tuning Room Temperature Pulsed Optically Detected Magnetic Resonance

Optical detection of magnetic resonance enables spin-based quantum sensing with high spatial resolution and sensitivity-even at room temperature-as exemplified by solid-state defects. Molecular systems provide a complementary, chemically tunable, platform for room-temperature optically detected magnetic resonance (ODMR)-based quantum sensing. A critical parameter governing sensing sensitivity is the optical contrast-i.e., the difference in emission between two spin states. In state-of-the-art solid-state defects such as the nitrogen-vacancy center in diamond, this contrast is approximately 30%. Here, capitalizing on chemical tunability, we show that room-temperature ODMR contrasts of 40% can be achieved in molecules. Using a nitrogen-substituted analogue of pentacene (6,13-diazapentacene), we enhance contrast compared to pentacene and, by determining the triplet kinetics through time-dependent pulsed ODMR, show how this arises from accelerated anisotropic intersystem crossing. Furthermore, we translate high-contrast room-temperature pulsed ODMR to self-assembled nanocrystals. Overall, our findings highlight the synthetic handles available to optically readable molecular spins and the opportunities to capitalize on chemical tunability for room-temperature quantum sensing.

quant-ph↗

arXiv2024

Surveying optically addressable spin qubits for quantum information and sensing technology

Quantum technologies offer ways to solve certain tasks more quickly, efficiently, and with greater precision than their classical counterparts. Yet substantial challenges remain in the construction of sufficiently error-free and scalable quantum platforms needed to unlock any real benefits to society. Acknowledging that this hardware can take vastly different forms, our review here focuses on so-called spintronic (\textit{i.e.}~spin-electronic) materials that use electronic or nuclear spins to embody qubits. Towards helping the reader to spot trends and pick winners, we have surveyed the various families of optically addressable spin qubits and attempted to benchmark and identify the most promising ones in each. We go on to reveal further trends that demonstrate how qubit lifetimes depend on the material's synthesis, the concentration/distribution of its embedded qubits, and the experimental conditions.

quant-ph↗

arXiv2024

Unlocking the Potential of Photoexcited Molecular Electron Spins for Room Temperature Quantum Information Processing

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, $α$,$γ$-bisdiphenylene-$β$-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.

cond-mat.mtrl-sci↗

arXiv2024

Room-temperature optically detected coherent control of molecular spins

Benefiting from both molecular tunability and versatile methods for deployment, optically interfaced molecular spins are a promising platform for quantum technologies such as sensing and imaging. Room-temperature optically detected coherent spin control is a key enabler for many applications, combining sensitive readout, versatile spin manipulation, and ambient operation. Here we demonstrate such functionality in a molecular spin system. Using the photoexcited triplet state of organic chromophores (pentacene doped in a para-terphenyl host), we optically detect coherent spin manipulation with photoluminescence contrasts exceeding 10% and microsecond coherence times at room temperature. We further demonstrate how coherent control of multiple triplet sublevels can significantly enhance optical spin contrast, and extend optically detected coherent control to a thermally evaporated thin film, retaining high photoluminescence contrast and coherence times of order one microsecond. These results open opportunities for room-temperature quantum technologies that can be systematically tailored through synthetic chemistry.

quant-ph↗

arXiv2023

`Maser-in-a-Shoebox': a portable plug-and-play maser device at room-temperature and zero magnetic-field

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.

quant-ph↗

arXiv2022

Move aside pentacene: Diazapentacene doped para-terphenyl as a zero-field room-temperature maser with strong coupling for cavity quantum electrodynamics

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.

quant-ph↗

arXiv2020

Room-temperature quasi-continuous-wave pentacene maser pumped by an invasive Ce:YAG luminescent concentrator

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$4 ms and an output power of up to -25 dBm. The maser is optically pumped by a cerium-doped YAG (Ce:YAG) luminescent concentrator (LC) whose wedge-shaped output is embedded inside a 0.1% pentacene-doped para-terphenyl (Pc:Ptp) crystal. The pumped crystal is located inside a ring of strontium titanate (STO) that supports a TE$_{01δ}$ 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.

physics.app-ph↗