We demonstrate the generation of coherent Stokes pulses with randomized linear-polarization in diamond, when the pump wave-vector and linear polarization were oriented along the $[110]$ and $[1\bar{1}0]$ axes respectively. In this configuration the excitation of multiple Raman modes produces isotropic gain, preventing the Stokes pulse from acquiring a deterministic orientation and is instead randomized by the zero-point motion of the crystal. Experimental polarization measurements were consistent with an independent, identical distribution with an estimated entropy rate of 6.67 bits per pulse.
Multi-frequency Raman generation is a promising method of producing ultrashort laser pulses with high intensities and visible wavelength frequencies. In experimental realizations of multi-frequency Raman generation the Raman order peaks display several behaviours that are not explained by the current theory. We derive an analytic and perturbative expression for the spectrum radiated by a Raman medium excited by multiple Gaussian laser pulses and show that it qualitatively agrees with experimental observations.
We propose a new technique for comparing two Raman active samples. The method employs optical interference of the signals generated via coherent anti-Stokes Raman scattering (CARS) of broadband laser pulses with noisy spectra. It does not require spectrally resolved detection, and no prior knowledge about either the Raman spectrum of the samples, or the spectrum of the incident light is needed. We study the proposed method theoretically, and demonstrate it in a proof-of-principle experiment on Toluene and ortho-Xylene samples.
We present two methods for efficient detection of chiral molecules based on sequences of single pulses and Raman pulse pairs. The chiral molecules are modelled by a closed-loop three-state system with different signs in one of the couplings for the two enantiomers. One method uses a sequence of three interaction steps: a single pulse, a Raman pulse, and another single pulse. The other method uses a sequence of only two interaction steps: a Raman pulse, and a single pulse. The second method is simpler and faster but requires a more sophisticated Raman pulse than the first one. Both techniques a…
Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth (FWHM ~14.2eV, 181 as) pulses tuned to the oxygen and nitrogen K-edges. Crosspeaks in 2D signals reveal electronic Franck-Condon overlaps between valence orbitals and relaxed orbitals in the presence of the core hole.
We describe a fiber Raman amplifier for nanosecond and sub-nanosecond pulses centered around 1260 nm. The amplification takes place inside a 4.5-m-long polarization-maintaining phosphorus-doped fiber, pumped at 1080 nm by 3-ns-long pulses with a repetition rate of 200 kHz and up to 1.75 kW peak power. The input seed pulses are of sub-mW peak-power and minimal duration of 0.25 ns, carved off a continuous-wave laser with sub-MHz linewidth. We obtain linearly-polarized output pulses with peak-powers of up to 1.4 kW, corresponding to peak-power conversion efficiency of over 80%. An ultrahigh small…
We have found a new hidden symmetry of time reversal light-atom interaction in the photon echo quantum memory with Raman atomic transition. The time-reversed quantum memory creates generalized conditions for ideal compression/decompression of time duration of the input light pulses and its wavelength. Based on a general analytical approach to this scheme, we have studied the optimal conditions for the light field compression/decompression in resonant atomic systems characterized by realistic spectral properties. The demonstrated necessary conditions for the effective quantum conversion of the …
The theory of stimulated Raman adiabatic passage in a three-level Lambda-scheme of the interaction of an atom or molecule with light, which takes the nonadiabatic processes at the beginning and the end of light pulses into account, is developed.
Stimulated Raman adiabatic passage (STIRAP), driven with pulses of optimum shape and delay has the potential of reaching fidelities high enough to make it suitable for fault-tolerant quantum information processing. The optimum pulse shapes are obtained upon reduction of STIRAP to effective two-state systems. We use the Dykhne-Davis-Pechukas (DDP) method to minimize nonadiabatic transitions and to maximize the fidelity of STIRAP. This results in a particular relation between the pulse shapes of the two fields driving the Raman process. The DDP-optimized version of STIRAP maintains its robustnes…
We propose and experimentally demonstrate a scheme to generate optically-controlled delays based on off-resonant Raman absorption. Dispersion in a transparency window between two neighboring, optically-activated Raman absorption lines is used to reduce the group velocity of broadband 765 nm pulses. We implement this approach in a potassium titanyl phosphate (KTP) waveguide at room temperature, and demonstrate Raman-induced delays of up to 140 fs for a 650-fs duration, 1.8-THz bandwidth, signal pulse; the available delay-bandwidth product is $\approx1$. Our approach is applicable to single phot…
We present a general and versatile technique of population transfer based on {\it parallel adiabatic passage} by femtosecond shaped pulses. Their amplitude and phase are specifically designed to optimize the adiabatic passage corresponding to parallel eigenvalues at all times. We show that this technique allows the robust adiabatic population transfer in a Raman system with the total pulse area as low as 3 $π$, corresponding to a fluence of one order of magnitude below the conventional stimulated Raman adiabatic passage process. This process of short duration, typically pico- and subpicosecond…
Using a single channel active Raman gain medium we show a $(220\pm 20)$ns advance time for an optical pulse of $τ_{FWHM}=15.4 μ$s propagating through a 10 cm medium, a lead time that is comparable to what was reported previously. In addition, we have verified experimentally all the features associated with this single channel Raman gain system. Our results show that the reported gain-assisted superluminal propagation should not be attributed to the interference between the two frequencies of the pump field.
We investigate the role of non-uniform spatial density profiles of trapped atomic Bose-Einstein condensates in the propagation of Raman-matched laser pulses under conditions for electromagnetically induced transparency (EIT). We find that the sharp edged axial density profile of an interacting condensate (due to a balance between external trap and repulsive atomic interaction) is advantageous for obtaining ultra slow averaged group velocities. Our results are in good quantitative agreement with a recent experiment report [Nature {\bf 397}, 594 (1999)].
Semiconductor quantum dots embedded in optical cavities are promising on-demand sources of single photons. Here, we theoretically study single photon emission from an optically driven two-photon Raman transition between the biexciton and the ground state of a quantum dot. The advantage of this process is that it allows all-optical control of the properties of the emitted single photon with a laser pulse. However, with the presence of other decay channels and excitation-induced quantum interference, on-demand emission of the single Raman photon is generally difficult to achieve. Here we show th…
We introduce a high-fidelity technique for coherent control of three-state quantum systems, which combines two popular control tools --- stimulated Raman adiabatic passage (STIRAP) and composite pulses. By using composite sequences of pairs of partly delayed pulses with appropriate phases the nonadiabatic transitions, which prevent STIRAP from reaching unit fidelity, can be canceled to an arbitrary order by destructive interference, and therefore the technique can be made arbitrarily accurate. The composite phases are given by simple analytic formulas, and they are universal for they do not de…
We present a general analysis for the interaction of a probe laser radiation with a coherently prepared molecular Raman medium. We describe a general formalism which includes dispersive effects, such as group velocity and group velocity dispersion (GVD). When dispersion is negligible, the analysis is especially simple and insightful. We show that molecular oscillations result in a modulated instantaneous susceptibility of the medium. The effect of the time-varying susceptibility on a probe laser pulse is two-fold: the output frequency becomes modulated because of the time-varying phase velocit…
The dynamics of a soliton propagating in a single-mode optical fiber with gain, loss, and Raman coupling to thermal phonons is analyzed. Using both soliton perturbation theory and exact numerical techniques, we predict that intrinsic thermal quantum noise from the phonon reservoirs is a larger source of jitter and other perturbations than the gain-related Gordon-Haus noise, for short pulses, assuming typical fiber parameters. The size of the Raman timing jitter is evaluated for both bright and dark (topological) solitons, and is larger for bright solitons. Because Raman thermal quantum noise i…
We combine multi-channel electronic structure theory with quantum optimal control to derive Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and phase control facilitated by the pump pulse carrier envelope phase. Our results open a route to creating core-hole excitations in molecules and aggregates that locally address specific atoms and represent the first step t…
We investigate the prospects of creating broad rotational wave packets by means of molecular interaction with long sequences of intense femtosecond pulses. Using state-resolved rotational Raman spectroscopy of oxygen, subject to a sequence of more than 20 laser pulses with peak intensities exceeding $10^{13}$ W/cm$^{2}$ per pulse, we show that the centrifugal distortion is the main obstacle on the way to reaching high rotational states. We demonstrate that the timing of the pulses can be optimized to partially mitigate the centrifugal limit. The cumulative effect of a long pulse sequence resul…
We describe analytically and numerically the process of population transfer by stimulated Raman adiabatic passage through a bright state when the pulses propagate in a medium. Limitations of the adiabaticity are analyzed and interpreted in terms of reshaping of the pulses. We find parameters for the pulses for which the population transfer is nearly complete over long distances.
We developed single-shot shaped pulses for ultra high fidelity (UH-fidelity) population transfer on a 3-level quantum system in lambda configuration. To ensure high fidelity, we use the Lewis-Riesenfeld (L-R) method to derive a family of solutions leading to an exact transfer, where the solutions follow a single dynamical mode of the L-R invariant. Among this family, we identify a tracking solution with a single parameter to control simultaneously the fidelity of the transfer, the population of the excited state, and robustness. We define a measure of the robustness of an UH-fidelity transfer …
We present a general systematic approach to design robust and high-fidelity quantum logic gates with Raman qubits using the technique of composite pulses. We use two mathematical tools -- the Morris-Shore and Majorana decompositions -- to reduce the three-state Raman system to an equivalent two-state system. They allow us to exploit the numerous composite pulses designed for two-state systems by extending them to Raman qubits. We construct the NOT, Hadamard, and rotation gates by means of the Morris-Shore transformation with the same uniform approach: sequences of pulses with the same phases f…
We examine the dynamics associated with the creation of a vortex in a Bose-Einstein condensate (BEC), from another nonrotating BEC using two-photon Raman transition with Gaussian (G) and Laguerre-Gaussian (LG) laser pulses. In particular, we consider BEC of Rb atoms at their hyperfine ground states confined in a quasi two dimensional harmonic trap. Optical dipole potentials created by G and LG laser pulses modify the harmonic trap in such a way that density profiles of the condensates during the Raman transition process depend on the sign of the generated vortex. We investigate the role played…
We apply the inverse geometric optimization technique to generate an optimal and robust stimulated Raman exact passage (STIREP) considering the loss of the upper state as a characterization parameter. Control fields temporal shapes that are optimal with respect to pulse area, energy, and duration, are found to form a simple sequence with a combination of intuitively (near the beginning and the end) and counter-intuitively ordered pulse pairs. The resulting dynamics produces a loss which is about a third of that of the non-robust optimal STIREP. Alternative optimal solutions featuring lower los…
We present mirror and beamsplitter pulse designs that improve the fidelity of atom interferometry and increase its tolerance of systematic inhomogeneities. These designs are demonstrated experimentally with a cold thermal sample of $^{85}$Rb atoms. We first show a stimulated Raman inversion pulse design that achieves a ground hyperfine state transfer efficiency of 99.8(3)%, compared with a conventional $π$ pulse efficiency of 75(3)%. This inversion pulse is robust to variations in laser intensity and detuning, maintaining a transfer efficiency of 90% at detunings for which the $π$ pulse fideli…
We introduce an atomic gravimetric sequence using Raman-type composite light pulses that excites a superposition of two momentum states with the same internal level. The scheme allows the suppression of common noise, making it less sensitive to external fluctuations of electromagnetic fields. The Raman beams are generated with a fiber modulator and are capable of momentum transfer in opposite directions. We obtain analytical expressions for the interference fringes in terms of three perturbative parameters that characterize the imperfections due to undesired frequencies introduced by the modul…
Counterdiabatic Raman Atom Optics for Compact High-Sensitivity Gravimetry
Hamad Bin Khalifa University（哈马德·本·哈利法大学）；P. J. Šafárik University（帕尔科维奇·沙法里克大学）；New York University Shanghai（纽约大学上海分校）；NYU-ECNU Institute of Physics at NYU Shanghai（纽约大学上海华东师范大学物理研究所）；Center for Quantum and Topological Systems (CQTS), NYUAD Research Institute, New York University Abu Dhabi（纽约大学阿布扎比分校量子与拓扑系统中心（CQTS）研究学院）；Department of Physics, New York University（纽约大学物理系）；The University of Adelaide（阿德莱德大学）；Institute for Research in Fundamental Sciences (IPM)（基础科学研究所）
We study beating of a probe field with a time-varying susceptibility in a coherently prepared Raman medium. We consider the general case of an arbitrary variation of susceptibility, which corresponds to a superposition of an arbitrary number of excited Raman transitions. We derive a general analytical solution and conservation relations for this process. We show that the interference between Raman polarizations may substantially affect frequency modulation and pulse compression for the probe field.
Quantum memories are vital to the scalability of photonic quantum information processing (PQIP), since the storage of photons enables repeat-until-success strategies. On the other hand the key element of all PQIP architectures is the beam splitter, which allows to coherently couple optical modes. Here we show how to combine these crucial functionalities by addressing a Raman quantum memory with multiple control pulses. The result is a coherent optical storage device with an extremely large time-bandwidth product, that functions as an array of dynamically configurable beam splitters, and that c…
We treat theoretically the two-pulse plane-wave propagation problem associated with the stimulated Raman process. A strong pump pulse and a weak probe pulse interact self-consistently during mutual propagation through a medium in the three-level lambda configuration. We treat the pulse interaction fully coherently, but take initially incoherent mixed ground states to describe the medium. We present analytic pulse envelope solutions to the nonlinear evolution equations, and then test them numerically. We show that the entire process can be interpreted consistently as a three-regime evolution, i…
In this paper we evaluate the performance of two superadiabatic stimulated Raman adiabatic passage (STIRAP) protocols derived from Gaussian and sin-cos pulses, under dissipation and Ornstein-Uhlenbeck noise in the energy levels. We find that for small amplitudes of Stokes and pump pulses, the population transfer is mainly achieved directly through the counterdiabatic pulse, while for large amplitudes the conventional STIRAP path dominates. This kind of "hedging" leads to a remarkable robustness against dissipation in the lossy intermediate state. For small pulse amplitudes and increasing noise…
We report new experiments on polarization squeezing using ultrashort photonic pulses in a single pass of a birefringent fiber. We measure what is to our knowledge a record squeezing of -6.8 +/- 0.3 dB in optical fibers which when corrected for linear losses is -10.4 +/- 0.8 dB. The measured polarization squeezing as a function of optical pulse energy, which spans a wide range from 3.5-178.8 pJ, shows a very good agreement with the quantum simulations and for the first time we see the experimental proof that Raman effects limit and reduce squeezing at high pulse energy.
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
Microwave pulse sequences are the basis of coherent manipulation of the electronic spin ground state in nitrogen-vacancy (NV) centers. In this work we demonstrate stimulated Raman transitions (SRT) and stimulated Raman adiabatic passage (STIRAP), two ways to drive the dipole-forbidden transition between two spin sublevels in the electronic triplet ground state of the NV center. This is achieved by a multitone Raman microwave pulse which simultaneously drives two detuned transitions via a virtual level for SRT or via two adiabatic and partially overlapping resonant microwave pulses for STIRAP. …
The adiabatic manipulation of quantum states is a powerful technique that has opened up new directions in quantum engineering, enabling tests of fundamental concepts such as the Berry phase and its nonabelian generalization, the observation of topological transitions, and holds the promise of alternative models of quantum computation. Here we benchmark the stimulated Raman adiabatic passage process for circuit quantum electrodynamics, by using the first three levels of a transmon qubit. We demonstrate a population transfer efficiency above 80% between the ground state and the second excited st…
This work investigates the utility of femtosecond pulse shaping in increasing the efficiency of Raman excitation of molecules in the strong-field interaction regime. We study experimentally and theoretically the effect of pulse shaping on the strength of non-resonant coherent anti-Stokes Raman scattering in iodine vapor at laser intensities exceeding $10^{13}$ W/cm$^2$. We show that unlike the perturbative case, shaping strong non-resonant laser pulses can increase the signal strength beyond that observed with the transform-limited excitation. Both adiabatic and non-adiabatic schemes of excita…
We have verified a mechanism for Raman excitation of atoms through continuum levels previously obtained by quantum optimal control using the multi-configurational time-dependent Hartree-Fock (MCTDHF) method. For the optimal control, which requires running multiple propagations to determine the optimal pulse sequence, we used the computationally inexpensive time-dependent configuration interaction singles (TDCIS) method. TDCIS captures all of the necessary correlation of the desired processes but assumes that ionization pathways reached via double excitations are not present. MCTDHF includes th…
A chirped-pulse quantum control scheme applicable to Coherent Anti-Stokes Raman Scattering spectroscopy, named as C-CARS, is presented aimed at maximizing the vibrational coherence in molecules. It implies chirping of three incoming pulses in the four-wave mixing process of CARS, the pump, the Stokes and the probe, to fulfil the conditions of adiabatic passage. The scheme is derived in the framework of rotating wave approximation and adiabatic elimination of excited state manifold simplifying the four-level model system into a ``super-effective'' two level system. The robustness, spectral sele…
A Raman compression scheme suitable for x-rays, where the Langmuir wave is created by an intense beam rather than the pondermotive potential between the seed and pump pulses, is proposed. The required intensity of the seed and pump pulses enabling the compression could be mitigated by more than a factor of 100, compared to conventionally available other Raman compression schemes. The relevant wavelength of x-rays ranges from 1 to 10 nm.
Electron and vibrational dynamics of molecules are commonly studied by subjecting them to two interactions with a fast actinic pulse that prepares them in a nonstationary state and after a variable delay period $T$, probing them with a Raman process induced by a combination of a broadband and a narrowband pulse. This technique known as femtosecond stimulated Raman spectroscopy (FSRS) can effectively probe time resolved vibrational resonances. We show how FSRS signals can be modeled and interpreted using the stochastic Liouville equations (SLE) originally developed for NMR lineshapes. The SLE p…
A scheme for fine tuning of quantum operations to improve their performance is proposed. A quantum system in $Λ$ configuration with two-photon Raman transitions is considered without adiabatic elimination of the excited (intermediate) state. Conditional dynamics of the system is studied with focus on improving fidelity of quantum operations. In particular, the $π$ pulse and $π/2$ pulse quantum operations are considered. The dressed states for the atom-field system, with an atom driven on one transition by a classical field and on the other by a quantum cavity field, are found. A discrete set o…
We explore coherent control of stimulated Raman scattering in the nonimpulsive regime. Optical pulse shaping of the coherent pump field leads to control over the stimulated Raman output. A model of the control mechanism is investigated.
We propose a technique which produces nearly complete ionization of the population of a discrete state coupled to a continuum by a two-photon transition via a lossy intermediate state whose lifetime is much shorter than the interaction duration. We show that using counterintuitively ordered pulses, as in stimulated Raman adiabatic passage (STIRAP), wherein the pulse coupling the intermediate state to the continuum precedes and partly overlaps the pulse coupling the initial and intermediate states, greatly increases the ionization signal and strongly reduces the population loss due to spontaneo…
The interaction between ultrashort light pulses and non-absorbing materials is dominated by Impulsive Stimulated Raman Scattering (ISRS). The description of ISRS in the context of pump\&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by me…
The probability of emission of a single photon via Raman scattering of laser pulse on the three-level $Λ$ - type atom in microcavity is studied. The duration of the pulse is considered to be short enough, so that the hyperfine structure of the upper level remains totally unresolved, while that of the lower level is totally resolved. The coherent laser pulse is assumed to be in resonance with the transition between one hyperfine structure component of the lower atomic level and all hyperfine structure components of the upper level, while the quantized cavity field is assumed to be in resonance …
We propose a class of schemes for robust population transfer between quantum states that utilize trains of coherent pulses and represent a generalized adiabatic passage via a wave packet. We study piecewise Stimulated Raman Adiabatic Passage with pulse-to-pulse amplitude variation, and piecewise chirped Raman passage with pulse-to-pulse phase variation, implemented with an optical frequency comb. In the context of production of ultracold ground-state molecules, we show that with almost no knowledge of the excited potential, robust high-efficiency transfer is possible
Phase-Randomized Laser Pulse Generation at 10 GHz for Quantum Photonic Applications
Toshiba Europe Ltd（东芝欧洲有限公司）；Cambridge University Engineering Department（剑桥大学工程系）；Escuela de Ingeniería de Telecomunicación, University of Vigo（维戈大学电信工程学院）
The Gradient Echo Memory (GEM) scheme has potential to be a suitable protocol for storage and retrieval of optical quantum information. In this paper, we review the properties of the $Λ$-GEM method that stores information in the ground states of three-level atomic ensembles via Raman coupling. The scheme is versatile in that it can store and re-sequence multiple pulses of light. To date, this scheme has been implemented using warm rubidium gas cells. There are different phenomena that can influence the performance of these atomic systems. We investigate the impact of atomic motion and four-wav…
The Stimulated Raman Adiabatic Passage (STIRAP) procedure is a robust and complete population transfer method which have various application in chemistry and atomic physics. Here, we study the effects of one-photon detuning, transition time, pulse width, and pulse delay parameters on the population transfer via STIRAP and b-STIRAP techniques. Moreover, the impact of the field amplitude which decreases the population transfer has been analyzed and it is shown that in b-STIRAP, the robustness of the complete transition can be improved by decreasing the field amplitude in the single-photon resona…
The coherent superposition of two-atomic levels induced by coherent population trapping is employed in a standard $Λ$ type scheme to form a tripod-like system. A weak probe pulse scanning across the system is shown to experience a crossover from absorption to transparent and then to amplification. Consequently the group velocity of the probe pulse can be controlled to propagate either as a subluminal, a standard, a superluminal or even a negative speed. It is shown that the propagation behavior of the light field is entirely determined and controlled by the initial states of the coherent super…
Broadband quantum memories hold great promise as multiplexing elements in future photonic quantum information protocols. Alkali vapour Raman memories combine high-bandwidth storage, on-demand read-out, and operation at room temperature without collisional fluorescence noise. However, previous implementations have required large control pulse energies and suffered from four-wave mixing noise. Here we present a Raman memory where the storage interaction is enhanced by a low-finesse birefringent cavity tuned into simultaneous resonance with the signal and control fields, dramatically reducing the…
We present recent results on the coherent control of an optical transition in a single rubidium atom, trapped in an optical tweezer. We excite the atom using resonant light pulses that are short (4 ns) compared with the lifetime of the excited state (26 ns). By varying the intensity of the laser pulses, we can observe an adjustable number of Rabi oscillations, followed by free decay once the light is switched off. To generate the pulses we have developed a novel laser system based on frequency doubling a telecoms laser diode at 1560 nm. By setting the laser intensity to make a pi-pulse, we use…
Using double optical Raman rephasing, an inversion-free resonant Raman echo is studied in an inhomogeneously broadened spin ensemble of a solid medium, where the Raman optical field-excited spin coherence has a frozen propagation vector. Unlike photon echoes whose quantum memory application is strictly limited due to πrephasing pulse-induced population inversion causing quantum noises, the optical Raman field-excited spin echo is inherently silent owing to the frozen propagation vector. Thus, the doubly rephased Raman echo can be directly applied for quantum interface in a population inversion…
We consider the coherent stimulated Raman process developing in an optically dense disordered atomic medium, which can also incoherently scatter the light over all outward directions. The Raman process is discussed in the context of a quantum memory scheme and we point out the difference in its physical nature from a similar but not identical protocol based on the effect of electromagnetically induced transparency (EIT). We show that the Raman and EIT memory schemes do not compete but complement one another and each of them has certain advantages in the area of its applicability. We include in…
