Coherent Manipulation Research Articles

Coherent control of an optical tweezer phonon laser

The creation and manipulation of coherence continues to capture the attention of scientists and engineers. The optical laser is a canonical example of a system that, in principle, exhibits complete coherence. Recent research has focused on the creation of coherent, laser-like states in other physical systems. The phonon laser is one example where it is possible to amplify self-sustained mechanical oscillations. A single mode phonon laser in a levitated optical tweezer has been demonstrated through appropriate balance of active feedback gain and damping. In this work, coherent control of the dynamics of an optical tweezer phonon laser is used to share coherence between its different modes of oscillation, creating a multimode phonon laser. The coupling of the modes is achieved by periodically rotating the asymmetric optical potential in the transverse focal plane of the trapping beam via trap laser polarization rotation. The presented theory and experiment demonstrate that coherence can be transferred across different modes of an optical tweezer phonon laser, and are a step toward using these systems for precision measurement and quantum information processing.

Transient stimulated Raman scattering spectroscopy and imaging

Stimulated Raman scattering (SRS) has been developed as an essential quantitative contrast for chemical imaging in recent years. However, while spectral lines near the natural linewidth limit can be routinely achieved by state-of-the-art spontaneous Raman microscopes, spectral broadening is inevitable for current mainstream SRS imaging methods. This is because those SRS signals are all measured in the frequency domain. There is a compromise between sensitivity and spectral resolution: as the nonlinear process benefits from pulsed excitations, the fundamental time-energy uncertainty limits the spectral resolution. Besides, the spectral range and acquisition speed are mutually restricted. Here we report transient stimulated Raman scattering (T-SRS), an alternative time-domain strategy that bypasses all these fundamental conjugations. T-SRS is achieved by quantum coherence manipulation: we encode the vibrational oscillations in the stimulated Raman loss (SRL) signal by femtosecond pulse-pair sequence excited vibrational wave packet interference. The Raman spectrum was then achieved by Fourier transform of the time-domain SRL signal. Since all Raman modes are impulsively and simultaneously excited, T-SRS features the natural-linewidth-limit spectral line shapes, laser-bandwidth-determined spectral range, and improved sensitivity. With ~150-fs laser pulses, we boost the sensitivity of typical Raman modes to the sub-mM level. With all-plane-mirror high-speed time-delay scanning, we further demonstrated hyperspectral SRS imaging of live-cell metabolism and high-density multiplexed imaging with the natural-linewidth-limit spectral resolution. T-SRS shall find valuable applications for advanced Raman imaging.

The concentration estimation for ensemble of NV– color centers with spin coherent manipulation

The concentration and distribution of negatively charged nitrogen-vacancy color centers (NV−) directly affect the sensitivity and resolution of quantum sensing. In this paper, a simple method is proposed to estimate the concentration of the ensemble of NV− centers with spin coherent manipulation. The stray fluorescence is eliminated by separating the fluorescence near the NV− zero-phonon line. By introducing a single NV− fluorescence quantitative model, the number of NV− centers in the diamond under test can be obtained. The average concentration of the ensemble of NV− centers in the sample can be obtained by combining the detection volume. Compared with the results measured by electron spin resonance, the concentration of NV− centers measured by our method can be verified, and the maximum error between the two methods is less than 4.3%. The results show that the method provides an effective reference for accurately characterizing the concentration distribution characteristics of the NV− ensemble.

Microwave coupled Zeeman splitting spectroscopy of a cesium nPJ Rydberg atom.

We perform measurements of microwave spectra of cesium Rydberg 51S1/2 → 51PJ transitions with the linewidth approaching the Fourier limit. A two-photon scheme excites the ground-state atoms to the Rydberg 51S1/2 state, and a weak microwave photon couples the Rydberg transition of 51S1/2 → 51PJ. The hyperfine structure of 51P1/2 can be clearly resolved with a narrow linewidth microwave spectra by using the method of ion detection. Furthermore, we investigate the Zeeman effect of the 51P1/2,3/2 state. The theoretical calculations reproduce the measurement well. Our experimental measurements provide a reliable technical solution for the investigation of high angular momentum Rydberg states, which is conducive to further realizing the coherent manipulation of Rydberg energy levels and improving the sensitivity of electromagnetic field measurement.

Fast generation of spin squeezing via resonant spin-boson coupling

We propose protocols for the creation of useful entangled states in a system of spins collectively coupled to a bosonic mode, directly applicable to trapped-ion and cavity QED setups. The protocols use coherent manipulations of the resonant spin-boson interactions naturally arising in these systems to prepare spin squeezed states exponentially fast in time. The resonance condition harnesses the full spin-boson coupling and thus avoids the slower timescales when operating in the off-resonance regime. We demonstrate the robustness of the protocols by analyzing the effects of natural sources of decoherence in these systems and show their advantage compared to more standard slower approaches where entanglement is generated with off-resonant spin-boson interactions.

Switchable multi-wavelength coherent polarization manipulation component based on single-layered hollowed S-shaped metasurface

High-performance metasurface polarization manipulation components have important applications in the fields of polarization imaging, polarization detection, and communication. Single-layered metasurface components have attracted a great deal of interest, but it is still a challenge to realize high-efficiency and dynamic polarization manipulation. Combined with coherent control techniques, we propose a single-layered hollowed S-shaped metasurface design that may accomplish multi-wavelength polarization switching in the optical to near-infrared band. The single-layered metasurface enables a real-time switchable effect between dual-wavelength and single-wavelength polarization properties by controlling the phase difference between two coherent counter-propagating lights. The physical mechanism of switchable multi-wavelength coherent polarization manipulation is elucidated based on the electric field distribution of the hollowed S-shaped structure. The effect of metal layer thickness on the switchable coherent polarization properties is investigated in detail. The proposed hollowed S-shaped metasurface significantly improves the polarization performance of the single-layered structure, which is expected to facilitate the development of switchable and compact polarization components.

High-Sensitivity ac-Charge Detection with a MHz-Frequency Fluxonium Qubit

Owing to their strong dipole moment and long coherence times, superconducting qubits have demonstrated remarkable success in hybrid quantum circuits. However, most qubit architectures are limited to the GHz frequency range, severely constraining the class of systems they can interact with. The fluxonium qubit, on the other hand, can be biased to very low frequency while being manipulated and read out with standard microwave techniques. Here, we design and operate a heavy fluxonium with an unprecedentedly low transition frequency of 1.8 MHz. We demonstrate resolved sideband cooling of the “hot” qubit transition with a final ground state population of 97.7%, corresponding to an effective temperature of 23 μK. We further demonstrate coherent manipulation with coherence times T1=34 μs, T2*=39 μs, and single-shot readout of the qubit state. Importantly, by directly addressing the qubit transition with a capacitively coupled waveguide, we showcase its high sensitivity to a radio-frequency field. Through cyclic qubit preparation and interrogation, we transform this low-frequency fluxonium qubit into a frequency-resolved charge sensor. This method results in a charge sensitivity of 33 μe/Hz, or an energy sensitivity (in joules per hertz) of 2.8ℏ. This method rivals state-of-the-art transport-based devices, while maintaining inherent insensitivity to dc-charge noise. The high charge sensitivity combined with large capacitive shunt unlocks new avenues for exploring quantum phenomena in the 1–10 MHz range, such as the strong-coupling regime with a resonant macroscopic mechanical resonator. Published by the American Physical Society 2024

Long-lived valley states in bilayer graphene quantum dots

Bilayer graphene is a promising platform for electrically controllable qubits in a two-dimensional material. Of particular interest is the ability to encode quantum information in the valley degree of freedom, a two-fold orbital degeneracy that arises from the symmetry of the hexagonal crystal structure. The use of valleys could be advantageous, as known spin- and orbital-mixing mechanisms are unlikely to be at work for valleys, promising more robust qubits. The Berry curvature associated with valley states allows for electrical control of their energies, suggesting routes for coherent qubit manipulation. However, the relaxation time of valley states—which ultimately limits these qubits’ coherence properties and therefore their suitability as practical qubits—is not yet known. Here we measure the characteristic relaxation times of these spin and valley states in gate-defined bilayer graphene quantum dot devices. Different valley states can be distinguished from each other with a fidelity of over 99%. The relaxation time between valley triplets and singlets exceeds 500 ms and is more than one order of magnitude longer than for spin states. This work facilitates future measurements on valley-qubit coherence, demonstrating bilayer graphene as a practical platform hosting electrically controlled, long-lived valley qubits.

Dielectric and Wavefunction Engineering of Electron Spin Lifetime in Colloidal Nanoplatelet Heterostructures.

Colloidal semiconductor nanoplatelets (NPLs) have emerged as low-cost and free-standing alternates of traditional quantum wells. The giant heavy- and light-hole splitting in NPLs allows for efficient optical spin injection. However, the electron spin lifetimes for prototypical CdSe NPLs are within a few picoseconds, likely limited by strong electron-hole exchange in these quantum- and dielectric-confined materials. Here how this hurdle can be overcome with engineered NPL-heterostructures is demonstrated. By constructing type-I CdSe/ZnS core/shell NPLs, dielectric screening inside the core is strongly enhanced, prolonging the electron spin polarization time (τesp) to over 30ps (or 60ps electron spin-flip time). Alternatively, by growing type-II CdSe/CdTe core/crown NPLs to spatially separate electron and hole wavefunctions, the electron-hole exchange is strongly suppressed, resulting in τesp as long as 300ps at room temperature. This study not only exemplifies how the well-established synthetic chemistry of colloidal heterostructures can aid in spin dynamics control but also establishes the feasibility of room-temperature coherent spin manipulation in colloidal NPLs.

Quantum spin coherence and electron spin distribution channels in vanadyl-containing lantern complexes.

We herein investigate the heterobimetallic lantern complexes [PtVO(SOCR)4] as charge neutral electronic qubits based on vanadyl complexes (S = 1/2) with nuclear spin-free donor atoms. The derivatives with R = Me (1) and Ph (2) give highly resolved X-band EPR spectra in frozen CH2Cl2/toluene solution, which evidence the usual hyperfine coupling with the 51V nucleus (I = 7/2) and an additional superhyperfine interaction with the I = 1/2 nucleus of the 195Pt isotope (natural abundance ca. 34%). DFT calculations ascribe the spin density delocalization on the Pt2+ ion to a combination of π and δ pathways, with the former representing the predominant channel. Spin relaxation measurements in frozen CD2Cl2/toluene-d8 solution between 90 and 10 K yield Tm values (1-6 μs in 1 and 2-11 μs in 2) which compare favorably with those of known vanadyl-based qubits in similar matrices. Coherent spin manipulations indeed prove possible at 70 K, as shown by the observation of Rabi oscillations in nutation experiments. The results indicate that the heavy Group 10 metal ion is not detrimental to the coherence properties of the vanadyl moiety and that Pt-VO lanterns can be used as robust spin-coherent building blocks in materials science and quantum technologies.

Non-uniform magnetic fields for single-electron control.

Controlling single-electron states becomes increasingly important due to the wide-ranging advances in electron quantum optics. Single-electron control enables coherent manipulation of individual electrons and the ability to exploit the wave nature of electrons, which offers various opportunities for quantum information processing, sensing, and metrology. Here we explore non-uniform magnetic fields, which offer unique mechanisms for single-electron control. Considering the modeling perspective, conventional electron quantum transport theories are commonly based on gauge-dependent electromagnetic potentials. A direct formulation in terms of intuitive electromagnetic fields is thus not possible. In an effort to rectify this, a gauge-invariant formulation of the Wigner equation for general electromagnetic fields has been proposed [M. Nedjalkov et al., Phys. Rev. B, 2019, 99, 014423]. However, the complexity of this equation requires the derivation of a more convenient formulation for linear electromagnetic fields [M. Nedjalkov et al., Phys. Rev. A, 2022, 106, 052213]. This formulation directly includes the classical formulation of the Lorentz force and higher-order terms, depending on the magnetic field gradient, that are negligible for small variations of the magnetic field. In this work, we generalize this equation in order to include a general, non-uniform electric field and a linear, non-uniform magnetic field. The thus obtained formulation has been applied to investigate the capabilities of a linear, non-uniform magnetic field to control single-electron states in terms of trajectory, interference patterns, and dispersion. This has led to the exploration of a new type of transport inside electronic waveguides based on snake trajectories and the possibility of splitting wavepackets to realize edge states.

Oriented Triplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular Donor-Acceptor Single Cocrystal.

The photogeneration of multiple unpaired electron spins within molecules is a promising route to applications in quantum information science because they can be initialized into well-defined, multilevel quantum states (S > 1/2) and reproducibly fabricated by chemical synthesis. However, coherent manipulation of these spin states is difficult to realize in typical molecular systems due to the lack of selective addressability and short coherence times of the spin transitions. Here, these challenges are addressed by using donor-acceptor single cocrystals composed of pyrene and naphthalene dianhydride to host spatially oriented triplet excitons, which exhibit promising photogenerated qutrit properties. Time-resolved electron paramagnetic resonance (TREPR) spectroscopy demonstrates that spatially orienting triplet excitons in a single crystal platform imparts narrow, well-resolved, tunable resonances in the triplet EPR spectrum, allowing selective addressability of the spin sublevel transitions. Pulse-EPR spectroscopy reveals that at temperatures above 30 K, spin decoherence of these triplet excitons is driven by exciton diffusion. However, coherence is limited by electronic spin dipolar coupling below 30 K, where T2 varies nonlinearly with the optical excitation density due to exciton annihilation. Overall, an optimized coherence time of T2 = 7.1 μs at 20 K is achieved. These results provide important insights into designing solid-state molecular excitonic materials with improved spin qutrit properties.

Emission and coherent control of Levitons in graphene

Flying qubits encode quantum information in propagating modes instead of stationary discrete states. Although photonic flying qubits are available, the weak interaction between photons limits the efficiency of conditional quantum gates. Conversely, electronic flying qubits can use Coulomb interactions, but the weaker quantum coherence in conventional semiconductors has hindered their realization. In this work, we engineered on-demand injection of a single electronic flying qubit state and its manipulation over the Bloch sphere. The flying qubit is a Leviton propagating in quantum Hall edge channels of a high-mobility graphene monolayer. Although single-shot qubit readout and two-qubit operations are still needed for a viable manipulation of flying qubits, the coherent manipulation of an itinerant electronic state at the single-electron level presents a highly promising alternative to conventional qubits.

Sub-nanosecond coherent optical manipulation of a single aromatic molecule at cryogenic temperature

Single molecules trapped in the solid state at liquid helium temperatures are promising quantum emitters for the development of quantum technologies owing to their remarkable photostability and their lifetime-limited optical coherence time of the order of 10 ns. The coherent preparation of their electronic state requires resonant excitation with a Rabi period much shorter than their optical coherence time. Sculpting the optical excitation with sharp edges and a high on–off intensity ratio (∼3 × 105) from a single-frequency laser beam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrene molecule embedded in a naphthalene matrix at 3.2 K, over more than 17 Rabi periods. With pulses tailored for a half-Rabi period, the electronic excited state is prepared with fidelity as high as 0.97. Using single-molecule Ramsey spectroscopy, we prove up to 5 K that the optical coherence lifetime remains at its fundamental upper limit set by twice the excited-state lifetime, making single molecules suitable for quantum bit manipulations under standard cryogen-free cooling technologies.

Nonlinear parametric generation in a four-level inverted-type quantum well nanostructure

In this study, we introduce an innovative semiconductor quantum well (SQW) nanostructure, which exhibits a unique four-level configuration arranged in an inverted Y-shape. This configuration enables interaction with three laser fields and demonstrates the intriguing nonlinear phenomenon of parametric generation. Our investigation delves into a wide range of parametric conditions, aiming to understand the profound impact of various system parameters on the generation and propagation of new light fields within this groundbreaking nanostructure. By employing a combination of analytical and numerical methods, we not only reveal the potential for precise manipulation of coherence among energy levels but also showcase its practical implications — high-efficiency and tunability in the parametric generation process. This pioneering scheme represents a significant advancement in the field of SQW structures, bridging the gap between theoretical exploration and practical application. Our findings promise exciting prospects for the development of novel light sources and optical devices based on SQW structures, thereby pushing the boundaries of what is achievable in various applications and setting new standards for the state-of-the-art in this domain.

Twin-Capture Rydberg State Excitation Enhanced with Few-Cycle Laser Pulses

Quantum excitation is usually regarded as a transient process occurring instantaneously, leaving the underlying physics shrouded in mystery. Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses. We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities. We also uncover new facets of the excitation dynamics, including the launching of an electron wave packet through strong-field ionization, the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn, resulting in twin captures into Rydberg orbitals. By tuning the laser intensity, we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale. Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states, thus benefiting Rydberg-state-based quantum technology.

Enhancement of microwave fields in pulse EPR of quantum paraelectrics

The pulse electron paramagnetic resonance (EPR) is widely used in different branches of material and life sciences, including promising applications in quantum information processing and quantum sensing. Here, we study the effect of the high polarizability of KTaO3 and SrTiO3 quantum paraelectrics on local electric and magnetic field components of microwaves (MW) at Fe3+ and Mn2+ paramagnetic ions. The measurements are performed with a commercial EPR spectrometer using dielectric and split-ring resonators. It is found that the power of MW pulses used in coherent spin manipulation at nanoseconds timescale decreases to milliwatts as compared to the tens–hundreds of watts usually used for spins in conventional materials. The amplification of MW fields is related to the very high dielectric permittivity (up to 25 000 in SrTiO3) of quantum paraelectrics at GHz frequencies and temperatures below 20 K. This creates the large induced polarization and, thus, huge displacement current and in turn the secondary MW magnetic field. Numerical simulations support the observation of the enhanced magnetic MW field in the high-permittivity sample. The low MW power for excitation of spin transitions in quantum paraelectrics eliminates the requirement of expensive high-power MW equipment. This approach also allows to globally control spin qubits in tandem with integrated devices based on conventional semiconductor MW circuits working at mW powers. It is suggested that quantum paraelectrics can also be used as substrates for deposition of nanoparticles or films of other materials, which would be manipulated by the low-power MW pulses.

Sensitivity of atom based on slow light propagation and rotary photon drag: an efficient and secure model for quantum-based sensors in Internet of Things

Quantum technology has the potential to revolutionize sensors and the Internet of Things (IoT). Efficient and secure data transfer among sensors and IoT devices is a major challenge. To address this, the manuscript presents coherent manipulation of the scattering cross section and its sensitivity based on subluminal propagation and rotary photon drag, using an atomic medium with two levels coupled with a cavity. The group index of the proposed atomic medium is measured in the range of -0.1le n_gle 150 and group velocity in the range of 2times 10^6m/sle v_gle pm 2times 10^9m/s. The maximum delay time is reported to t_g=0.3mu s and rotary photon drag to theta _d=pm 5 micro radian. This effect of photon drag is used in sensing, energy harvesting, and optical switching in IoT. The scattering cross-section of 0.1times 10^{21}m^2 is reported. The scattering cross-section impacts the efficiency and reliability of quantum-based communication for IoT. The maximum cross-sectional sensitivity is measured to S_sigma =0.4times 10^{-19}m^2/n_r. The cross-sectional sensitivity potentially impacts secure communication and highly precise detection in sensors and IoT.

Coherent manipulation of nuclear spins in the strong driving regime

Spin-based quantum information processing makes extensive use of spin-state manipulation. This ranges from dynamical decoupling of nuclear spins in quantum sensing experiments to applying logical gates on qubits in a quantum processor. Fast manipulation of spin states is highly desirable for accelerating experiments, enhancing sensitivity, and applying elaborate pulse sequences. Strong driving using intense radio-frequency (RF) fields can, therefore, facilitate fast manipulation and enable broadband excitation of spin species. In this work, we present an antenna for strong driving in quantum sensing experiments and theoretically address challenges of the strong driving regime. First, we designed and implemented a micron-scale planar spiral RF antenna capable of delivering intense fields to a sample. The planar antenna is tailored for quantum sensing experiments using the diamond’s nitrogen-vacancy (NV) center and should be applicable to other solid-state defects. The antenna has a broad bandwidth of 22 MHz, is compatible with scanning probes, and is suitable for cryogenic and ultrahigh vacuum conditions. We measure the magnetic field induced by the antenna and estimate a field-to-current ratio of G/A, representing a six-fold increase in efficiency compared to the state-of-the-art, crucial for cryogenic experiments. We demonstrate the antenna by driving Rabi oscillations in 1H spins of an organic sample on the diamond surface and measure 1H Rabi frequencies of over 500 kHz, i.e. -pulses shorter than 1 —an order of magnitude faster than previously reported in NV-based nuclear magnetic resonance (NMR). Finally, we discuss the implications of driving spins with a field tilted from the transverse plane in a regime where the driving amplitude is comparable to the spin-state splitting, such that the rotating wave approximation does not describe the dynamics well. We present a simple recipe to optimize pulse fidelity in this regime based on a phase and offset-shifted sine drive, which may be optimized in situ without numerical optimization procedures or precise modeling of the experiment. We consider this approach in a range of driving amplitudes and show that it is particularly efficient in the case of a tilted driving field. The results presented here constitute a foundation for implementing fast nuclear spin control in various systems.

Characterization of Quantum Frequency Processors

Frequency-bin qubits possess unique synergies with wavelength-multiplexed lightwave communications, suggesting valuable opportunities for quantum networking with the existing fiber-optic infrastructure. Although the coherent manipulation of frequency-bin states requires highly controllable multi-spectral-mode interference, the quantum frequency processor (QFP) provides a scalable path for gate synthesis leveraging standard telecom components. Here we summarize the state of the art in experimental QFP characterization. Distinguishing between physically motivated “open box” approaches that treat the QFP as a multiport interferometer, and “black box” approaches that view the QFP as a general quantum operation, we highlight the assumptions and results of multiple techniques, including quantum process tomography of a tunable beamsplitter—to our knowledge the first full process tomography of any frequency-bin operation. Our findings should inform future characterization efforts as the QFP increasingly moves beyond proof-of-principle tabletop demonstrations toward integrated devices and deployed quantum networking experiments.