Multiphoton Transitions Research Articles

Band structure effects in above threshold photoemission

We have performed an angle-resolved two-photon and three-photon photoemission study of the Ag(111) surface employing ultrashort laser pulses as the excitation source. We show the presence of multi-photon resonances between electronic states at selected points of the Brillouin zone which appear in the high-order photoemission spectral region. We observe clear signatures of electronic band structure effects of the Ag crystal in above-threshold photoemission (ATP) processes, identifying two types of transitions, which either proceed via non-resonant multi-photon excitation from an occupied initial state, or involve a real intermediate state located above the vacuum level of the solid directly influencing the ATP process. For this latter class of phenomena, we suggest that electron populations created by incoherent processes give a contribution to the multi-photon transition, possibly allowing us to trace the transmission of photoexcited electrons through the crystal.

Electromagnetically induced absorption via incoherent collisions

We conduct theoretical studies on electromagnetically induced absorption via incoherent collisions in an inhomogeneously broadened ladder-type three-level system with the density-matrix approach. The effects of the collision-induced coherence decay rates as well as the probe laser field intensity on the probe field absorption are examined. It is shown that with the increase of the collisional decay rates in a moderate range, a narrow dip due to electromagnetically induced transparency superimposed on the Doppler-broadened absorption background can be turned into a narrow peak under the conditions that the probe field intensity is not very weak as compared to the pump field, which results from the enhancement of constructive interference and suppression of destructive interference between one-photon and multiphoton transition pathways. The physical origin of the collision-assisted electromagnetically induced absorption is analyzed with a power-series solution of the density-matrix equations.

Rotational temperature analysis of N2 by resonant enhanced multi-photon ionization with fluorescence detection

A non-invasive, optical technique to determine the rotational temperature of molecular nitrogen at atmospheric pressure by direct probing of the N2(X1Σg+,v=0) ground state with subsequent analysis of the rotational state distribution is presented. A tunable probe laser was scanned over resonant-enhanced, multi-photon ionization transitions initiating from various N2(X1Σg+,v=0,J″) states. At atmospheric pressure, the laser photo-ionization also induced N2+ fluorescence bands. Analysis of the relative fluorescence as a function of laser wavelength produced a calculated N2(X1Σg+,v=0,J″) rotational state distribution and determined the rotational temperature. The analysis also resulted in the assignment and tabulation of 11 previously unreported term energies for N2(b1Πu+,v=6) and N2(b1Πu-,v=6) for J′ > 22, based on the experimental data. The method resulted in temperature determinations for two experimental trials in atmospheric N2 gas flows at room temperature and 600 K that were in good agreement with thermocouple measurements in the vicinity of the laser probe region.

Calculation of Multiphoton Transition in Li Atoms via Chirped Microwave Pulse

The position and width of avoided crossings of Li atom energy levels in a static electric field is presented by using the B-spline basis set method combined with the model potential. Using the time-dependent multilevel approach, the population of Li atoms is transferred to the target state completely by one-photon, two-photon or a single multiphoton adiabatic rapid passage, which requires only a small frequency sweep. The calculation results agree well with the experiment and novel explanations are given to understand the experimental results.

Single-Photon Optomechanics

Optomechanics experiments are rapidly approaching the regime where the radiation pressure of a single photon displaces the mechanical oscillator by more than its zero-point uncertainty. We show that in this limit the power spectrum has multiple sidebands and that the cavity response has several resonances in the resolved-sideband limit. Using master-equation simulations, we also study the crossover from the weak-coupling many-photon to the single-photon strong-coupling regime. Finally, we find non-Gaussian steady states of the mechanical oscillator when multiphoton transitions are resonant. Our study provides the tools to detect and take advantage of this novel regime of optomechanics.

Multiphoton association reaction He + H+ → HeH+ steered by ultra-short laser pulse

The multiphoton association reaction He + H+ → HeH+ in the electronic ground state is investigated using the time-dependent quantum wave packet method. It is shown that the collision pairs He + H+ in continuum state transfer into ν = 0 state and then produce stable molecules HeH+ through emission of two or three photons. The multiphoton transition takes place via intermediate states, and the transfer probability is determined by the collision energy and the intermediate states. The populations of the intermediate states and ν = 0 state can be controlled by the laser duration. The three-photon transition is more efficient than the two-photon transition for producing the molecule HeH+ in ν = 0 state. © 2010 Wiley Periodicals, Inc. Int J Quantum Chem, 2011

Weak-field multiphoton femtosecond coherent control in the single-cycle regime

Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.

Experimental observation of carrier-envelope-phase effects by multicycle pulses

We present an experimental and theoretical study of carrier-envelope phase (CEP) effects on the population transfer between two bound atomic states interacting with pulses consisting of many cycles. Using intense radio-frequency pulse with Rabi frequency of the order of the atomic transition frequency, we investigated the influence of CEP on the control of phase dependent multi-photon transitions between the Zeeman sub-levels of the ground state of $^{87}$Rb. Our scheme has no limitation on the duration of the pulses. Extending the CEP control to longer pulses creates interesting possibilities to generate pulses with accuracy that is better then the period of optical oscillations.

Nonlinear interband and intersubband transitions in quantum dots for multiphoton photodetectors

Accurate nonperturbative Floquet theory is used to study nonlinear multiphoton transitions in quantum dot involving interband and intersubband states. The interband transitions generate electron-hole pairs, which in turn give rise to photocurrent useful for making multiphoton photodetector. We find the direct role of multiphoton absorption processes over the single photon absorption in enhancing the sensitivity of the photodetector for photon energy equal to or less than the half of the bandgap energy.

A Treatment of the Absorption Spectrum for a Multiphoton V‐TypeThree‐Level Atom Interacting with a Squeezed Coherent Field in thePresence of Nonlinearities

We study the interaction of a three‐level atom with a single mode field through multiphoton transition in a cavity, taking explicitly into account the existence of forms of nonlinearities of both the field and the intensity‐dependent atom‐field coupling. The analytical forms of the absorption spectrum is calculated using the dressed states of the system. The effects of photon multiplicities, mean photon number, detuning, Kerr‐like medium, and the intensity‐dependent coupling functional on the absorption spectrum are analyzed.

多光子跃迁过程中的量子衍射与量子相干控制

多光子跃迁过程中的量子衍射与量子相干控制

Microscopic theory of the extremely nonlinear terahertz response of semiconductors

AbstractThe extreme nonlinear terahertz response of initially unexcited intrinsic semiconductor nanostructures is studied theoretically by solving extended semiconductor Bloch equations numerically. The coupled dynamics of intraband acceleration and multiphoton interband transitions leads to high‐harmonic generation up to several tens of the exciting terahertz frequency. It is shown that the actual cut‐off frequency is determined by the band structure and not by the excitation strength.

Extension of the sum rule for the transition rates between multiplets to the multiphoton case

The sum rule for the transition rates between the components of two multiplets, known for the one-photon transitions, is extended to the multiphoton transitions in hydrogen and hydrogen-like ions. As an example the transitions 3p-2p, 4p-3p and 4d-3d are considered. The numerical results are compared with previous calculations.

Sensitive frequency dependence of the carrier-envelope phase effect on bound-bound transitions: An interference perspective

We investigate numerically with Hylleraas coordinates the frequency dependence of the carrier-envelope phase (CEP) effect on bound-bound transitions of helium induced by an ultrashort laser pulse of a few cycles. We find that the CEP effect is very sensitive to the carrier frequency of the laser pulse, occurring regularly even at far-off-resonance frequencies. By analyzing a two-level model, we find that the CEP effect can be attributed to the quantum interference between neighboring multiphoton transition pathways, which is made possible by the broadened spectrum of the ultrashort laser pulse. A general picture is developed along this line to understand the sensitivity of the CEP effect to the laser's carrier frequency. Multilevel influence on the CEP effect is also discussed.

Precise control of state-selective excitation in stimulated Raman scattering

Multiphoton transitions can be manipulated by tailoring the ultrashort laser pulse. In this paper, we propose two schemes for achieving precise control of the selective excitation between two excited states in stimulated Raman-scattering process. We theoretically demonstrate that by properly designing the spectral phase distribution, the stimulated Raman transition probability for one excited state is kept at zero or a maximal value, while that for the other excited state can be continuously tuned over a wide range. Furthermore, the influence of the spectral bandwidth on the tunable range by the two schemes is discussed. We conclude that these schemes have significant application to the selective excitation of femtosecond coherent anti-Stokes Raman scattering.

Quasienergy description of the driven Jaynes-Cummings model

We analyze the driven resonantly coupled Jaynes-Cummings model in terms of a quasienergy approach by switching to a frame rotating with the external modulation frequency and by using the dressed atom picture. A quasienergy surface in phase space emerges whose level spacing is governed by a rescaled effective Planck constant. Moreover, the well-known multiphoton transitions can be reinterpreted as resonant tunneling transitions from the local maximum of the quasienergy surface. Most importantly, the driving defines a quasienergy well which is nonperturbative in nature. The quantum-mechanical quasienergy state localized at its bottom is squeezed. In the Purcell-limited regime, the potential well is metastable and the effective local temperature close to its minimum is uniquely determined by the squeezing factor. The activation occurs in this case via dressed spin-flip transitions rather than via quantum activation as in other driven nonlinear quantum systems such as the quantum Duffing oscillator. The local maximum is, in general, stable. However, in presence of resonant coherent or dissipative tunneling transitions the system can escape from it and a stationary state arises as a statistical mixture of quasienergy states being localized in the two basins of attraction. This gives rise to a resonant or an antiresonant nonlinear response of the cavity at multiphoton transitions. The model finds direct application in recent experiments with a driven superconducting circuit quantum electrodynamics setup.

TWO MOVING ATOMS INTERACTING WITH TWO-MODE THERMAL FIELD

In this paper, we have presented some results of entanglement between two moving atoms, when the multi-photon transition occurs. We obtain the general solution of the system using the unitary operator approach. It is shown that the center-of-mass motion plays an important role on the entanglement dynamics. It is also shown that the initial state settings have an impact on the evaluation.

Multifrequency spin resonance in diamond

Magnetic resonance techniques provide a powerful tool for controlling spin systems, with applications ranging from quantum information processing to medical imaging. Nevertheless, the behavior of a spin system under strong excitation remains a rich dynamical problem. In this paper, we examine spin resonance of the nitrogen-vacancy center in diamond under conditions outside the regime where the usual rotating wave approximation applies, focusing on effects of multifrequency excitation and excitation with orientation parallel to the spin quantization axis. Strong-field phenomena such as multiphoton transitions and coherent destruction of tunneling are observed in the spectra and analyzed via numerical and analytic theory. In addition to illustrating the response of a spin system to strong multifrequency excitation, these observations may inform techniques for manipulating electron-nuclear spin quantum registers.

“Doubly Magic” Conditions in Magic-Wavelength Trapping of Ultracold Alkali-Metal Atoms

In experiments with trapped atoms, atomic energy levels are shifted by the trapping optical and magnetic fields. Regardless of this strong perturbation, precision spectroscopy may be still carried out using specially crafted, "magic" trapping fields. Finding these conditions for particularly valuable microwave transitions in alkali-metal atoms has so far remained an open challenge. Here I demonstrate that the microwave transitions in alkali-metal atoms may be indeed made impervious to both trapping laser intensity and fluctuations of magnetic fields. I consider driving multiphoton transitions between the clock levels and show that these "doubly magic" conditions are realized at special values of trapping laser wavelengths and fixed values of relatively weak magnetic fields. This finding has implications for precision measurements and quantum information processing with qubits stored in hyperfine manifolds.

Multiplication of qubits in a doubly resonant bichromatic field

Multiplication of spin qubits arises at double resonance in a bichromatic field when the frequency of the radio-frequency (rf) field is close to that of the Rabi oscillation in the microwave field, provided its frequency equals the Larmor frequency of the initial qubit. We show that the operational multiphoton transitions of dressed qubits can be selected by the choice of both the rotating frame and the rf phase. In order to enhance the precision of dressed qubit operations in the strong-field regime, the counter-rotating component of the rf field is taken into account.