We consider the stimulated Raman transition between two long-lived states via multiple intermediate states, such as between hyperfine ground states in the alkali-metal atoms. We present a concise treatment of the general, multilevel, off-resonant case, and we show how the lightshift emerges naturally in this approach. We illustrate our results by application to alkali-metal atoms and we make specific reference to cesium. We comment on some artifacts, due solely to the geometrical overlap of states, which are relevant to existing experiments.
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…
We present an analytic description of the effects of dephasing processes on stimulated Raman adiabatic passage in a tripod quantum system. To this end, we develop an effective two-level model. Our analysis makes use of the adiabatic approximation in the weak dephasing regime. An effective master equation for a two-level system formed by two dark states is derived, where analytic solutions are obtained by utilizing the Demkov-Kunike model. From these, it is found that the fidelity for the final coherent superposition state decreases exponentially for increasing dephasing rates. Depending on the…
We implement high-efficiency coherent excitation to a Rydberg state using stimulated Raman adiabatic passage in a cold atom electron and ion source. We achieve an efficiency of 60% averaged over the laser excitation volume with a peak efficiency of 82%, a 1.6 times improvement relative to incoherent pulsed-laser excitation. Using pulsed electric field ionization of the Rydberg atoms we create electron bunches with durations of 250 ps. High-efficiency excitation will increase source brightness, crucial for ultrafast electron diffraction experiments, and coherent excitation to high-lying Rydberg…
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.
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.
Stimulated Raman spectroscopy has become a powerful tool to study the spatiodynamics of molecular bonds with high sensitivity, resolution and speed. However, sensitivity and speed of state-of-the-art stimulated Raman spectroscopy are currently limited by the shot-noise of the light beam probing the Raman process. Here, we demonstrate an enhancement of the sensitivity of continuous-wave stimulated Raman spectroscopy by reducing the quantum noise of the probing light below the shot-noise limit by means of amplitude squeezed states of light. Probing polymer samples with Raman shifts around 2950 $…
We consider stimulated Raman adiabatic passage (STIRAP) processes in tripod systems and show how to generate purely geometric phase changes of the quantum states involved. The geometric phases are controlled by three laser fields where pulse shapes, relative field strength and phases can be controlled. We present a robust set of universal gates for quantum computing based on these geometric phases: a one-qubit phase gate, a Hadamard gate and a two-qubit phase gate.
We report on the experimental demonstration of stimulated Raman adiabatic passage (STIRAP) in a Tm$^{3+}$:YAG crystal. Tm$^{3+}$:YAG is a promising material for use in quantum information processing applications, but as yet there are few experimental investigations of coherent Raman processes in this material. We investigate the effect of inhomogeneous broadening and Rabi frequency on the transfer efficiency and the width of the two-photon spectrum. Simulations of the complete Tm$^{3+}$:YAG system are presented along with the corresponding experimental results.
The space-time method is applied to a model system-the Simple Harmonic Oscillator in a laser field to simulate the Stimulated Raman Adiabatic Passage (STIRAP) process. The Space-Time method is a computational theory first introduced by Weatherford et. al. to solve Time-Dependent Systems with one boundary value and applied to electron spin system with invariant Hamiltonian [Journal of Molecular Structure {\bf 592} 47]. The implementation in the present work provides an efficient and general way to solve the Time-Dependent Schr{ö}dinger Equation and can be applied to multi-state systems. The alg…
We propose a scheme which can produce desired nonadiabatic passages for the stimulated Raman transition in three-level systems. The state transfer in the protocol is realized by following the evolution of the dynamical basis itself and no additional coupling field is required. We also investigate the interplay between the present nonadiabatic protocol and the shortcut to adiabaticity. By incorporating the latter technology, we show that alternative passages with less occupancy of the intermediate level could be designed.
Stimulated Raman adiabatic passage (STIRAP) is a widely used protocol to realize high-fidelity and robust quantum control in various quantum systems. However, further application of this protocol in superconducting qubits is limited by population leakage caused by the only weak anharmonicity. Here we introduce an optimally controlled shortcut-to-adiabatic (STA) technique to speed up the STIRAP protocol in a superconducting qudit. By modifying the shapes of the STIRAP pulses, we experimentally realize a fast (32 ns) and high-fidelity quantum state transfer. In addition, we demonstrate that our …
We study the scattering problem of photon and polariton in a one-dimensional coupled-cavity system. Analytical approximate analysis and numerical simulation show that a photon can stimulate the photon emission from a polariton through polariton-photon collisions. This observation opens the possibility of photon-stimulated transition from insulating to radiative phase in a coupled-cavity QED system. Inversely, we also find that a polariton can be generated by a two-photon Raman scattering process. This paves the way towards single photon storage by the aid of atom-cavity interaction.
We generate half-excited symmetric Dicke states of two and four ions. We use multi-level stimulated Raman adiabatic passage (STIRAP) whose intermediate states are phonon Fock states. This process corresponds to the spin squeezing operation and half-excited Dicke states are generated during multi-level STIRAP. This method does not require local access for each ion or the preparation of phonon Fock states. Furthermore, it is robust since it is an adiabatic process. We evaluate the Dicke state using a witness operator and determine the upper and lower bounds of the fidelity without using full qua…
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…
Quantum control methods for three-level systems have become recently an important direction of research in quantum information science and technology. Here we present numerical simulations using realistic experimental parameters for quantum process tomography in STIRAP (stimulated Raman adiabatic passage) and saSTIRAP (superadiabatic STIRAP). Specifically, we identify a suitable basis in the operator space as the identity operator together with the 8 Gell-Mann operators, and we calculate the corresponding process matrices, which have $9\times 9=81$ elements. We discuss these results for the id…
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 demonstrate experimentally how the process of Stimulated Raman Adiabatic Passage (STIRAP) can be utilized for efficient coherent internal state transfer in single trapped and laser-cooled $^{40}$Ca$^+$ ions. The transfer from the D$_{3/2}$ to the D$_{5/2}$ state, is detected by a fluorescence measurement revealing the population not transfered to the D$_{5/2}$ state. A coherent population transfer efficiency at the level of 95 % in a setup allowing for the internal state detection of individual ions in a string has been obtained.
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…
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. …
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 propose a non-Hermitian generalization of stimulated Raman adiabatic passage (STIRAP), which allows one to increase speed and fidelity of the adiabatic passage. This is done by adding balanced imaginary (gain/loss) terms in the diagonal (bare energy) terms of the Hamiltonian and choosing them such that they cancel exactly the nonadiabatic couplings, providing in this way an effective shortcut to adiabaticity. Remarkably, for a STIRAP using delayed Gaussian-shaped pulses in the counter-intuitive scheme the imaginary terms of the Hamiltonian turn out to be time independent. A possible physica…
We report on the first observation of stimulated Raman scattering from a Lambda-type three-level atom, where the stimulation is realized by the vacuum field of a high-finesse optical cavity. The scheme produces one intracavity photon by means of an adiabatic passage technique based on a counter-intuitive interaction sequence between pump laser and cavity field. This photon leaves the cavity through the less-reflecting mirror. The emission rate shows a characteristic dependence on the cavity and pump detuning, and the observed spectra have a sub-natural linewidth. The results are in excellent a…
We analyze coherent two-color photoassociation of a Bose-Einstein condensate, focusing on stimulated Raman adiabatic passage (STIRAP) in free-bound-bound transitions from atoms to molecules. This problem is of particular interest since STIRAP is predicted to be necessarily absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. However, Bose-stimulation enhances the free-bound dipole matrix element for an atomic condensate, and photoassociative STIRAP turns out to be a viable mechanism for converting an atomic condensate to a molecular condensate with near-unit …
It is proved that a qubit encoded in excited states of a V-type quantum system cannot be perfectly transferred to the state of the cavity field mode using a single rectangular laser pulse. This obstacle can be overcome by using a two-stage protocol, in which the fidelity of a state-mapping operation can be increased to nearly one.
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…
We present a general formalism for describing stimulated Raman adiabatic passage in a multi-level atom. The atom is assumed to have two ground state manifolds a and b and an excited state manifold e, and the adiabatic passage is carried out by resonantly driving the a-e and b-e transitions with time-dependent fields. Our formalism gives a complete description of the adiabatic passage process, and can be applied to systems with arbitrary numbers of degenerate states in each manifold and arbitrary couplings of the a-e and b-e transitions. We illustrate the formalism by applying it to both a simp…
Accurate control of a quantum system is a fundamental requirement in many areas of modern science ranging from quantum information processing to high-precision measurements. A significantly important goal in quantum control is to prepare a desired state as fast as possible with sufficiently high fidelity allowed by available resources and experimental constraints. Stimulated Raman adiabatic passage (STIRAP) is a robust way to realize high-fidelity state transfer but it requires a sufficiently long operation time to satisfy the adiabatic criteria. We here theoretically propose and then experime…
Vacuum-stimulated Raman scattering in strongly coupled atom-cavity systems allows one to generate free-running single photon pulses on demand. Most properties of the emitted photons are well defined, provided spontaneous emission processes do not contribute. Therefore, electronic excitation of the atom must not occur, which is assured for a system adiabatically following a dark state during the photon-generation process. We experimentally investigate the conditions that must be met for adiabatic following in a time-of-flight driven system, with atoms passing through a cavity and a pump beam or…
We present the derivation of the frequency dependent scalar, vector, and tensor dynamical polarizabilities for the two hyperfine levels of the 87Rb atom 5s ground state. Based on the characterization of the dynamical polarizabilities, we analyze and measure the differential vector and tensor light shift between the 5s ground state sub-levels with near-resonant, stimulated Raman transitions. These results clarify that the tensor polarizabilities for the ground states of alkali atoms are absent when the light field is far-detuned from the atomic resonance and the total electronic angular momentu…
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 observe velocity-selective two-photon resonances in a cold atom cloud in the presence of a magnetic field. We use these resonances to demonstrate a simple magnetometer with sub-mG resolution. The technique is particularly useful for zeroing the magnetic field and does not require any additional laser frequencies than are already used for standard magneto-optical traps. We verify the effects using Faraday rotation spectroscopy.
Efficient initialization and manipulation of quantum states is important for numerous applications and it usually requires the ability to perform high fidelity and robust swapping of the populations of quantum states. Stimulated Raman adiabatic passage (STIRAP) has been known to perform efficient and robust inversion of the ground states populations of a three-level system. However, its performance is sensitive to the initial state of the system. In this contribution we demonstrate that a slight modification of STIRAP, where we introduce a non-zero single-photon detuning, allows for efficient …
We consider a quantum memory scheme based on the conversion of a signal pulse into a long-lived spin coherence via stimulated off-resonant Raman process. For a storing medium consisting of alkali atoms, we have calculated the Autler-Townes resonance structure created by a strong control field. By taking into account the upper hyperfine states of the D1 optical transition, we show important deviations from the predictions of the usual three-level Lambda-scheme approximation and we demonstrate an enhancement of the process for particular detunings of the control. We estimate the memory efficienc…
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 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…
We propose a simple technique for the generation of arbitrary-sized Dicke states in a chain of trapped ions. The method uses global addressing of the entire chain by two pairs of delayed but partially overlapping laser pulses to engineer a collective adiabatic passage along a multi-ion dark state. Our technique, which is a many-particle generalization of stimulated Raman adiabatic passage (STIRAP), is decoherence-free with respect to spontaneous emission and robust against moderate fluctuations in the experimental parameters. Furthermore, because the process is very rapid, the effects of heati…
The rapid experimental progress in the field of superconducting nanocircuits gives rise to an increasing quest for advanced quantum-control techniques for these macroscopically coherent systems. Here we demonstrate theoretically that stimulated Raman adiabatic passage (STIRAP) should be possible with the quantronium setup of a Cooper-pair box. The scheme appears to be robust against decoherence and should be realizable even with the existing technology. As an application we present a method to generate single-phonon states of a nanomechnical resonator by vacuum-stimulated adiabatic passage wit…
We experimentally demonstrate composite stimulated Raman adiabatic passage (CSTIRAP), which combines the concepts of composite pulse sequences and adiabatic passage. The technique is applied for population transfer in a rare-earth doped solid. We compare the performance of CSTIRAP with conventional single and repeated STIRAP, either in the resonant or the highly detuned regime. In the latter case, CSTIRAP improves the peak transfer efficiency and robustness, boosting the transfer efficiency substantially compared to repeated STIRAP. We also propose and demonstrate a universal version of CSTIRA…
We present a three-dimensional theory of stimulated Raman scattering (SRS) or superradiance. In particular we address how the spatial and temporal properties of the generated SRS beam, or Stokes beam, of radiation depends on the spatial properties of the gain medium. Maxwell equations for the Stokes field operators and of the atomic operators are solved analytically and a correlation function for the Stokes field is derived. In the analysis we identify a superradiating part of the Stokes radiation that exhibit beam characteristics. We show how the intensity in this beam builds up in time and a…
We describe how stimulated Raman adiabatic passage (STIRAP) can be applied to create spectral holes in an inhomogeneously broadened system. Due to the robustness of STIRAP, our proposal guarantees high flexibility and accuracy and, at variance with traditional spectral hole burning techniques, it may require substantially less time resources since it does not rely upon the spontaneous decay of an intermediate excited state. We investigate the effects on the scheme of dephasing and dissipation as well as of unintentional driving of undesired transitions due to a finite splitting of the initial …
Stimulated Raman adiabatic passage is a quantum protocol that can be used for robust state preparation in a three-level system. It has been commonly employed in quantum optics, but recently this technique has drawn attention also in circuit quantum electrodynamics. The protocol relies on two slowly varying drive pulses that couple the initial and the target state via an intermediate state, which remains unpopulated. Here we study the detrimental effect of the parasitic couplings of the drives into transitions other than those required by the protocol. The effect is most prominent in systems wi…
We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals…
We consider the population transfer process in a Lambda-type atomic medium of unequal oscillator strengths by stimulated Raman adiabatic passage via bright-state (b-STIRAP) taking into account propagation effects. Using both analytic and numerical methods we show that the population transfer efficiency is sensitive to the ratio q_p/q_s of the transition oscillator strengths. We find that the case q_p>q_s is more detrimental for population transfer process as compared to the case where $q_p \leq q_s$. For this case it is possible to increase medium dimensions while permitting efficient populati…
Collective two-color photoassociation of a freely-interacting 87Rb Bose-Einstein condensate is theoretically examined, focusing on stimulated Raman adiabatic passage (STIRAP) from an atomic to a stable molecular condensate. In particular, Drummond et al. [Phys. Rev. A 65, 063619 (2002); cond-mat/0110578] have predicted that particle-particle interactions can limit the efficiency of collective atom-molecule STIRAP, and that optimizing the laser parameters can partially overcome this limitation. We suggest that the molecular conversion efficiency can be further improved by treating the initial c…
We exploit a microscopically derived master equation for the study of STIRAP in the presence of decay from the auxiliary level toward the initial and final state, and compare our results with the predictions obtained from a phenomenological model previously used [P. A. Ivanov, N. V. Vitanov, and K. Bergmann, Phys. Rev. A 72, 053412 (2005)]. It is shown that our approach predicts a much higher efficiency. The effects of temperature are also taken into account, proving that in b-STIRAP thermal pumping can increase the efficiency of the population transfer.
We use optimal control theory to obtain shortcuts to adiabaticity which maximize population transfer in a three-level STIRAP system, for a given finite duration of the process and specified dissipation rate at the intermediate state. We fix the sum of the intensities of the pump and Stokes pulses and use the mixing angle as the sole control variable. We determine the optimal variation of this angle and reveal the role of singular arc in the optimal trajectory, in order to minimize the effect of dissipation.
Squeezed spin states have important applications in quantum metrology and sensing. It has been shown by Sørensen and Mølmer [Phys. Rev. A 66, 022314(2002)] that an effective one-axis-twisting interaction can be realized in a cavity setup via a double off-resonance stimulated Raman scattering, resulting in a noise reduction scaling $\propto 1/N^{2/3}$ with $N$ being the atom number. Here, we show that, by making an appropriate change of the initial input spin state, it is possible to produce a one-axis-twisting spin squeezing via a \emph{single} off-resonance stimulated Raman scattering, which …
We propose the use of stimulated Raman adiabatic passage (STIRAP) to offer a fast high fidelity method of performing SU(2) rotations on spinor Bose Einstein condensates (BEC). Past demonstrations of BEC optical control suffer from difficulties arising from collective enhancement of spontaneous emission and inefficient two-photon transitions originating from selection rules. We present here a novel scheme which allows for arbitrary coherent rotations of two-component BECs while overcoming these issues. Numerical tests of the method show that for BECs of \ce{^{87}Rb} with up to $ 10^4 $ atoms an…
We study dynamics of a two-color photoassociation of atoms into diatomic molecules via nonlinear Stimulated Raman adiabatic passage (STIRAP) process. This system has a famous counterpart in (linear) quantum mechanics, and been discussed recently in the context of generalizing quantum adiabatic theorem to nonlinear systems. Here we use another approach to study adiabaticity and stability in the system: we apply methods of classical Hamiltonian dynamics. We found nonlinear dynamical instabilities, cases of complete integrability, and improved conditions of adiabaticity.
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…
Stimulated Raman adiabatic passage (STIRAP) is a widely-used technique of coherent state-to-state manipulation for many applications in physics, chemistry, and beyond. The adiabatic evolution of the state involved in STIRAP, called adiabatic passage, guarantees its robustness against control errors, but also leads to problems of low efficiency and decoherence. Here we propose and experimentally demonstrate an alternative approach, termed stimulated Raman "user-defined" passage (STIRUP), where a parameterized state is employed for constructing desired evolutions to replace the adiabatic passage…
Solid state quantum emitters have shown strong potential for applications in quantum information, but spectral inhomogeneity of these emitters poses a significant challenge. We address this issue in a cavity-quantum dot system by demonstrating cavity-stimulated Raman spin flip emission. This process avoids populating the excited state of the emitter and generates a photon that is Raman shifted from the laser and enhanced by the cavity. The emission is spectrally narrow and tunable over a range of at least 125 GHz, which is two orders of magnitude greater than the natural linewidth. We obtain t…
