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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Non-equilibrium rate theory for polariton relaxation dynamics

We derive an analytic expression of the non-equilibrium Fermi’s golden rule (NE-FGR) expression for a Holstein–Tavis–Cumming Hamiltonian, a universal model for many molecules collectively coupled to the optical cavity. These NE-FGR expressions capture the full-time-dependent behavior of the rate constant for transitions from polariton states to dark states. The rate is shown to be reduced to the well-known frequency domain-based equilibrium Fermi’s golden rule (E-FGR) expression in the equilibrium and collective limit and is shown to retain the same scaling with the number of sites in non-equilibrium and non-collective cases. We use these NE-FGR to perform population dynamics with a time-non-local and time-local quantum master equation and obtain accurate population dynamics from the initially occupied upper or lower polariton states. Furthermore, NE-FGR significantly improves the accuracy of the population dynamics when starting from the lower polariton compared to the E-FGR theory, highlighting the importance of the non-Markovian behavior and the short-time transient behavior in the transition rate constant.

Chemical dynamics↗
DOE OSTI2026

Quantum nanophotonic interface for tin-vacancy centers in thin-film diamond

The negatively charged tin-vacancy center in diamond (SnV − ) is an excellent solid state qubit with optically-addressable transitions and a long electron spin coherence time at elevated (∼1.7 K). However, implementing scalable quantum nodes with high-fidelity optical readout of the electron spin state requires efficient photon emission and collection from the system. Here, in this manuscript, we report a quantum photonic interface for SnV−centers based on one-dimensional photonic crystal cavities fabricated in diamond thin films. Furthermore, we provide a rigorous description of the spontaneous emission dynamics of our system, taking into account individual contributions from both the C and D transitions of the emitter. This allows for determination of Purcell factors per transition and, by extension, the C/D branching ratio SnV− zero phonon line. We observe quality factors up to ~6000 across this sample, and measure up to a 12-fold lifetime reduction, which translates into a Purcell factor of 𝐹 𝐶 =26.2±1.5 for a targeted C transition. By considering the cavity mode polarization alignment with the C and D transition dipole moments, we validate the C/D branching ratio to be 𝜂 BR =0.75±0.01, in line with previous theoretical and experimental findings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Overcoming the fundamental limit of quantum transduction via intraband entanglement

A quantum transducer converts an input signal to an output probe at a distant frequency band while maintaining the quantum information with high fidelity, which is crucial for quantum networking and distributed quantum sensing and computing. In terms of microwave–optical quantum transduction, the state-of-the-art quantum transducers suffer low transduction efficiency from weak nonlinear coupling, wherein increasing pump power to enhance efficiency inevitably leads to thermal noise from heating. Moreover, we reveal that the efficiency-bandwidth product of a cavity electro-optical or electro-optomechanical transducer is fundamentally limited by pump power and nonlinear coupling coefficient, irrespective of cavity engineering efforts. To overcome this fundamental limit, we propose to noiselessly boost the transduction efficiency by consuming intraband entanglement (e.g., microwave–microwave or optical–optical entanglement in the case of microwave–optical transduction). Via a squeezer–coupler–antisqueezer sandwich structure, the protocol enhances the transduction efficiency to unity in the ideal lossless case, given an arbitrarily weak pump and nonlinear coupling. In practical cavity systems, our entanglement-assisted protocol surpasses the non-assisted fundamental limit of the efficiency-bandwidth product and reduces the threshold cooperativity for positive quantum capacity by a factor proportional to two-mode squeezing gain. Given a fixed cooperativity, our approach increases the broadband quantum capacity by orders of magnitude. The entanglement-assisted advantage is robust to ancilla loss and cavity detuning.

Shi, Haowei [Southern California U.] (ORCID:000000↗
DOE OSTI2023

SERAPH: Wavelike Dark Matter Searches with SRF Cavities

Haloscopes consisting of a microwave cavity with a high quality factor (Q) connected to low-noise electronics have been deployed to detect wavelike axions and dark photons. But the dark matter mass is unknown, so haloscopes must be tunable to search through the photon coupling vs. mass parameter space. Therefore, the scan rate for haloscope experiments is a crucial figure of merit and is proportional to the cavity’s quality factor. State-of-the-art experiments like ADMX currently use copper cavities with 𝑄∼80000. However, implementing superconducting cavities with 𝑄∼1010 can increase the instantaneous scan rate by possibly a factor of 105.This presentation will report progress on the SERAPH experiment, a family of superconducting haloscopes being developed by the Superconducting Quantum Materials and Systems (SQMS) Center. In this presentation, I will first discuss the principles behind operating a haloscope whose bandwidth is much narrower than the dark matter halo energy distribution. I will then describe the first SERAPH experiments implementing a 1.3 GHz Niobium cavity with an ultra-high quality factor (Q~1010) that has achieved the best sensitivity and deepest exclusion to wavelike dark photon dark matter by almost an order of magnitude. Next, I will discuss progress on the next phase of SERAPH, which will search dark photon dark matter using a widely-tunable SRF cavity (4-7 GHz). I will finally describe plans for subsequent SERAPH experiments to search for dark photons and axions with tunable SRF cavities tolerant to multi-Tesla magnetic fields and quantum sensors that subvert the Standard Quantum Limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Room-temperature valley-selective emission in Si-MoSe 2 heterostructures enabled by high-quality-factor chiroptical cavities

Transition metal dichalcogenides possess valley pseudospin, enabling coupling between photon spin and electron spin for classical and quantum information processing. However, rapid valley-dephasing processes have impeded the development of scalable, high-performance valleytronic devices operating at room temperature. Here we demonstrate that a chiral resonant metasurface can enable room-temperature valley-selective emission in MoSe 2 monolayers independent of excitation polarization. This platform provides circular eigen-polarization states with a high quality factor (Q-factor) and strong chiral near-field enhancement. The fabricated Si chiral metasurfaces exhibit chiroptical resonances with Q-factors up to 450 at visible wavelengths. We reveal degrees of circular polarization (DOP) reaching a record high of 0.5 at room temperature. Our measurements show that the high DOP can be attributed to the significantly increased chiroptical local density of states, which enhances valley-specific radiative transition rates by a factor of ~13. Our work could facilitate the development of ultracompact chiral classical and quantum light sources.

42 ENGINEERING↗
DOE OSTI2023

All-epitaxial resonant cavity enhanced long-wave infrared detectors for focal plane arrays

Here, we demonstrate a monolithic all-epitaxial resonant-cavity architecture for long-wave infrared photodetectors with substrate-side illumination. An nBn detector with an ultra-thin (t ≈ 350 nm) absorber layer is integrated into a leaky resonant cavity, formed using semitransparent highly doped (n⁺⁺) epitaxial layers, and aligned to the anti-node of the cavity’s standing wave. The devices are characterized electrically and optically and demonstrate an external quantum efficiency of 25% at T ¼ 180 K in an architecture compatible with focal plane array configurations.

42 ENGINEERING↗
DOE OSTI2025

When do molecular polaritons behave like optical filters?

This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light–matter coupling regime. Under weak laser irradiation and when the single-molecule light–matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or “filtered”) laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light–matter states) and those that can occur in the weak coupling regime. Here, we further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.

Schwennicke, Kai [University of California, San Di↗
DOE OSTI2023

SERAPH: Wavelike Dark Matter Searches with SRF Cavities

Haloscopes consisting of a microwave cavity with a high quality factor (Q) connected to low-noise electronics have been deployed to detect wavelike axions and dark photons. But the dark matter mass is unknown, so haloscopes must be tunable to search through the photon coupling vs. mass parameter space. Therefore, the scan rate for haloscope experiments is a crucial figure of merit and is proportional to the cavity’s quality factor. State-of-the-art experiments like ADMX currently use copper cavities with 𝑄∼80000. However, implementing superconducting cavities with 𝑄∼1010 can increase the instantaneous scan rate by possibly a factor of 105. This presentation will report progress on the SERAPH experiment, a family of superconducting haloscopes being developed by the Superconducting Quantum Materials and Systems (SQMS) Center. In this presentation, I will first discuss the principles behind operating a haloscope whose bandwidth is much narrower than the dark matter halo energy distribution. I will then describe the first SERAPH experiments implementing a 1.3 GHz Niobium cavity with an ultra-high quality factor (Q~1010) that has achieved the best sensitivity and deepest exclusion to wavelike dark photon dark matter by almost an order of magnitude. Next, I will discuss progress on the next phase of SERAPH, which will search dark photon dark matter using a widely-tunable SRF cavity (4-7 GHz). I will finally describe plans for subsequent SERAPH experiments to search for dark photons and axions with tunable SRF cavities tolerant to multi-Tesla magnetic fields and quantum sensors that subvert the Standard Quantum Limit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Studying phonon coherence with a quantum sensor

Nanomechanical oscillators offer numerous advantages for quantum technologies. Their integration with superconducting qubits shows promise for hardware-efficient quantum error-correction protocols involving superpositions of mechanical coherent states. Limitations of this approach include mechanical decoherence processes, particularly two-level system (TLS) defects, which have been widely studied using classical fields and detectors. In this manuscript, we use a superconducting qubit as a quantum sensor to perform phonon number-resolved measurements on a piezoelectrically coupled phononic crystal cavity. This enables a high-resolution study of mechanical dissipation and dephasing in coherent states of variable size ($\overline{n}$ ≃ 1 – 10 phonons). We observe nonexponential relaxation and state size-dependent reduction of the dephasing rate, which we attribute to TLS. Using a numerical model, we reproduce the dissipation signatures (and to a lesser extent, the dephasing signatures) via emission into a small ensemble (N = 5) of rapidly dephasing TLS. Our findings comprise a detailed examination of TLS-induced phonon decoherence in the quantum regime.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

3D superconducting radio-frequency resonators for quantum computing

Superconducting radiofrequency (SRF) technology is being used not only in discovery science programs and basic research but also for several applications that benefit society more directly. The advantage of superconducting resonators over those made of normal-conducting metal is their ability to store electromagnetic energy with much lower dissipation. The high quality factor and longer dissipation time provided by these superconducting resonators can deliver superior performance. Currently, the quantum processing architecture uses resonators and interconnecting circuits operating in the microwave regime with superconducting strip-line technology and low noise electronic devices for switching and communication. The performance of these devices can be enhanced by embedding them in 3D SRF cavity resonators to prolong the coherence time, which improves the utility of the device by reducing error rates and allowing more manipulations (calculations) before the quantum state decays. In this presentation, I will review the current technology and progress towards the three dimensional SRF cavities to enhance the coherence time.

Dhakal, Pashupati↗
DOE OSTI2021

THz time-domain characterization of amplifying quantum-cascade metasurface

An amplifying quantum-cascade (QC) metasurface, the key component of the QC vertical-external-cavity surface-emitting-laser (VECSEL), is studied as a function of injected current density using reflection-mode terahertz time domain spectroscopy. Nearly perfect absorption is measured at zero bias, which is associated with the transition from the weak to strong coupling condition between the metasurface resonance and an intersubband transition within the QC material. An increase in reflectance is observed as the device is biased, both due to reduction in intersubband loss and the presence of intersubband gain. Significant phase modulation associated with the metasurface resonance is observed via electrical control, which may be useful for electrical tuning of QC-VECSEL. These results provide insight into the interaction between the intersubband QC-gain material and the metasurface and modify the design rules for QC-VECSELs for both biased and unbiased regions.

42 ENGINEERING↗
DOE OSTI2020

Cavity electro-optics in thin-film lithium niobate for efficient microwave-to-optical transduction

Linking superconducting quantum devices to optical fibers via microwave-optical quantum transducers may enable large-scale quantum networks. For this application, transducers based on the Pockels electro-optic (EO) effect are promising for their direct conversion mechanism, high bandwidth, and potential for low-noise operation. However, previously demonstrated EO transducers require large optical pump power to overcome weak EO coupling and reach high efficiency. Here, we create an EO transducer in thin-film lithium niobate, a platform that provides low optical loss and strong EO coupling. We demonstrate on-chip transduction efficiencies of up to and of optical pump power. The transduction efficiency can be improved by further reducing the microwave resonator’s piezoelectric coupling to acoustic modes, increasing the optical resonator quality factor to previously demonstrated levels, and changing the electrode geometry for enhanced EO coupling. We expect that with further development, EO transducers in thin-film lithium niobate can achieve near-unity efficiency with low optical pump power.

Holzgrafe, Jeffrey (ORCID:0000000160121451)↗
DOE OSTI2025

Low-dimensional solid-state single-photon emitters

Solid-state single-photon emitters (SPEs) are attracting significant attention as fundamental components in quantum computing, communication, and sensing. Low-dimensional materials-based SPEs (LD-SPEs) have drawn particular interest due to their high photon extraction efficiency, ease of integration with photonic circuits, and strong coupling with external fields. The accessible surfaces of LD materials allow for deterministic control over quantum light emission, while enhanced quantum confinement and light–matter interactions improve photon emissive properties. This perspective examines recent progress in LD-SPEs across four key materials: zero-dimensional (0D) semiconductor quantum dots, one-dimensional (1D) nanotubes, two-dimensional (2D) materials, including hexagonal boron nitride (hBN) and transition metal dichalcogenides (TMDCs). We explore their structural and photophysical properties, along with techniques such as spectral tuning and cavity coupling, which enhance SPE performance. Finally, we address future challenges and suggest strategies for optimizing LD-SPEs for practical quantum applications.

42 ENGINEERING↗
DOE OSTI2024

The role of excitation vector fields and all-polarisation state control in cavity magnonics

Recently the field of cavity magnonics, a field focused on controlling the interaction between magnons and photons confined within microwave resonators, has drawn significant attention as it offers a platform for enabling advancements in quantum- and spin-based technologies. Here, we introduce excitation vector fields, whose polarisation and profile can be easily tuned in a two-port cavity setup, thus acting as an effective experimental dial to explore the coupled dynamics of cavity magnon-polaritons. Moreover, we develop theoretical models that accurately predict and reproduce the experimental results for any polarisation state and field profile within the cavity resonator. This versatile experimental platform offers a new avenue for controlling spin-photon interactions by manipulating the polarisation of excitation fields. By introducing real-time tunable parameters that control the polarisation state, our experiment delivers a mechanism to readily control the exchange of information between hybrid systems.

condensed-matter physics↗
DOE OSTI2026

How Do You Hear a Quantum Computer Whisper?

Quantum transduction is the process of upconverting microwave quantum signals into optical signals to develop quantum networks through optical fibers outside the dilution refrigerator, enabling connections between quantum technologies on the quantum internet. In this project, upconversion is achieved by directing an optical laser and the microwave quantum signal into an electro-optic bulk crystal. The crystal is housed within a Superconducting Radio Frequency (SRF) cavity designed to maximize the overlap between the microwave field and the crystal volume. In the presence of microwaves, the refractive index of the crystal changes through the Pockels effect. This change in refractive index modifies the propagation of the optical field within the crystal, allowing the quantum information carried by the microwave field to be transferred to the optical field. This study focuses on coupling laser light from suspended waveguide chips into the whispering-gallery modes (WGMs) of the crystal to enable transduction. The coupling efficiency between the optical field in the suspended waveguide and the WGM depends on the position of the laser spot on the crystal. To address this challenge, a feedback-based algorithm is being developed to fine-tune the waveguide position so that the optical signal is coupled efficiently into the crystal. After passing through the crystal, the optical signal is detected by a photodiode connected to an oscilloscope. The algorithm evaluates the coupling quality and iteratively adjusts the waveguide position to maximize coupling efficiency. The expected outcome is an automated waveguide alignment method that improves optical coupling and enables more efficient microwave-to-optical quantum transduction.

Karanastasis, Mihael [Fermilab]↗
DOE OSTI2023

Encapsulating Semiconductor Quantum Dots in Supramolecular Cages Enables Ultrafast Guest–Host Electron and Vibrational Energy Transfer

In the field of supramolecular chemistry, host- guest systems have been extensively explored to encapsulate a wide range of substrates, owing to emerging functionalities in nano-confined space that cannot be achieved in dilute solutions. However, host-guest chemistry is still limited to encapsulation of small guests. Herein, we construct a water-soluble metallo-supramolecular hexagonal prism with a large hydrophobic cavity by anchoring multiple polyethylene glycol chains onto the building blocks. Then, assembled prisms are able to encapsulate quantum dots (QDs) with diameters of less than 5.0 nm. Furthermore, we find that the supramolecular cage around each QD strongly modifies the photophysics of the QD by universally increasing the rates of QD relaxation processes via ultrafast electron and vibrational energy transfer. In conclusion, taken together, these efforts expand the scope of substrates in host-guest systems and provide a new approach to tune the optical properties of QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Shining light on the microscopic resonant mechanism responsible for cavity-mediated chemical reactivity

Strong light–matter interaction in cavity environments is emerging as a promising approach to control chemical reactions in a non-intrusive and efficient manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating a chemical reaction has, however, remained unclear, hampering progress in this frontier area of research. We leverage quantum-electrodynamical density-functional theory to unveil the microscopic mechanism behind the experimentally observed reduced reaction rate under cavity induced resonant vibrational strong light-matter coupling. We observe multiple resonances and obtain the thus far theoretically elusive but experimentally critical resonant feature for a single strongly coupled molecule undergoing the reaction. While we describe only a single mode and do not explicitly account for collective coupling or intermolecular interactions, the qualitative agreement with experimental measurements suggests that our conclusions can be largely abstracted towards the experimental realization. Specifically, we find that the cavity mode acts as mediator between different vibrational modes. In effect, vibrational energy localized in single bonds that are critical for the reaction is redistributed differently which ultimately inhibits the reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

SRF Levitation and Trapping of Nanoparticles Experiment

The levitation and trapping of micro particles using lasers is not a new accomplishment and has been applied in containerless processing and spectroscopy of microparticles. Recent developments in the field of optomechanics have achieved levitating nanoparticles such that quantum phenomena was observed which would have relevance in quantum science and technology. This two-year project sought to levitate and trap mesoscopic particles using radio frequency (RF) fields in a resonating superconducting RF (SRF) cavity. By exploiting the intrinsic characteristics of an SRF resonating cavity, the project was to explore overcoming a major limit faced by current laser trapping techniques. The goal was to establish a foundation to enable the observation of quantum phenomena of an isolated mechanical oscillator interacting with microwave fields. If successful the experiment could establish its ground-breaking relevance to quantum information science and technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗