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Ziqiu Huang

Publications and source records attributed to Ziqiu Huang.

4 recordsLinked to original sources

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

Scaleable LED-pumped Room-temperature Maser using a Multi-blade Optical Injector

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.

physics.optics

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

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