Two classes of analytic solutions for three-state systems involving two overlapping laser pulses of different shapes, or of similar shapes but with their centers displaced, are presented. We find a remarkable connection between the order of arrival of the two overlapping pulses and the effectiveness of transfer from the ground state to the third state, and we find remarkable results for the maximum occupation probability of the intermediate state. The approach of these analytic solutions to the adiabatic-following process is also demonstrated.
Two classes of analytic solutions for three-state systems involving two overlapping laser pulses of different shapes, or of similar shapes but with their centers displaced, are presented. We find a remarkable connection between the order of arrival of the two overlapping pulses and the effectiveness of transfer from the ground state to the third state, and we find remarkable results for the maximum occupation probability of the intermediate state. The approach of these analytic solutions to the adiabatic-following process is also demonstrated.
This paper presents an analytic study of the properties of a three-state system coupled to two external laser fields on two-photon resonance. The intermediate state is generally off single-photon resonance and can decay irreversibly out of the system. The two fields are assumed to have the same pulse-shaped time dependence but may have different strengths. Various general properties for arbitrary pulse shapes, detunings and decay rates are derived and illustrated with an exactly solvable analytic model. They include the conditions for complete population transfer and depletion, complete population loss or no loss, various limitations on the values of the populations, the effect of overdamping at large decay rates and others.
A simple model with only three quantum states is used for an atom or molecule in which two transitions are driven by two overlapping laser pulses. The amplitudes of the two pulses are not proportional to the same function of time. The authors impose the 'two-photon resonance' condition, but the two pulses separately are not applied at the resonant frequencies. For pulse pairs having certain shapes, the wavefunctions are written in terms of generalised hypergeometric functions. Simple formulae for transition probabilities are then obtained, are are used to discuss transfer of the three-state system from its ground state to its highest state.
This paper analyzes the extension of the three-state process of stimulated Raman adiabatic passage to chainwise-connected multistate systems. A necessary condition for such a process is the existence of an adiabatic-transfer state, which connects adiabatically the initial state of the chain to its final state. Various counterintuitive pulse sequences are examined, in all of which the pulse that drives the last transition of the chain precedes the pulse driving the first transition, while the pulses driving the intermediate transitions may have different timings. The paper demonstrates some important qualitative differences and similarities between the systems with odd and even number of states. In the on-resonance case, an adiabatic-transfer state always exists for an odd number of states while it never exists for an even number of states. In the off-resonance case, however, the two types of systems behave in a very similar manner and the condition for existence of an adiabatic-transfer state is essentially the same. This condition, which imposes certain limitations on the laser parameters, is derived in a simple and compact form. It is also shown analytically that, besides by large detunings, the populations of the intermediate states (which are generally nonzero during the transfer) can be damped by large intermediate couplings. It is concluded that for an odd number of states, the optimal case is the on-resonance one, with equal and large intermediate couplings. For an even number of states, the optimal (off-resonance) case is when the intermediate couplings and the detunings have similar values. Various numerical examples of success and failure of multistate population transfer confirm the analytic conclusions.
Quantum changes of three-state systems have some similarities with those of two-state systems. When subject to steady illumination the populations may undergo oscillations similar to the Rabi cycling of two-state systems, and various forms of adiabatic following are possible. Analytic solutions to the relevant TDSE exist [Sho90, Chap. 23]. The additional degree of freedom, typically allowing controllable parameters of a second laser pulse, allows a wider variety of controlled excitation. The resulting differences and similarities to two-state systems have been discussed at length [Whi76; Sho77; Rad82b; Yoo85; Car87]. Three-state linkages Two-field linkages . The simplest extension of two-state excitation allows two laser fields, here identified by letters P (for pump) and S (for Stokes), as befits the stimulated Raman process discussed in Chap. 14. The carrier frequencies of the two fields, ω P and ω S , are each assumed to be close to resonance with one, and only one, Bohr frequency, so that each field can be uniquely identified with a particular transition (failure of this restriction, and the resulting linkage ambiguity, is discussed in [Una00]). I will assume that the P field is (near) resonance only with the 1–2 transition, while the S field is (near) resonant only with the 2–3 transition; these interactions thereby form a two-step linkage chain. This system has three possible linkage patterns, shown in Fig. 13.1. The linkage patterns (sometimes called configurations) differ by the ordering of the energies of the linked states.With the assumption that population initially occupies state 1, as in Fig. 13.1, the definitions are: Ladder : The ladder system has the energy ordering E 1 < E 2 < E 3 .
We demonstrate that various properties of population transfer by delayed pulses in three-level systems on two-photon resonance can be deduced analytically and for general pulse shapes. We use the fact that the three-level system reduces to effective two-level problems at large intermediate-level detuning \ensuremath{\Delta}, on resonance (\ensuremath{\Delta}=0) and for completely overlapping pulses. Special attention is paid to the effect of the pulse order on the population transfer efficiency. We show that on resonance the transfer efficiency depends substantially on the pulse order, while at large \ensuremath{\Delta} it does not. We also find that under some natural restrictions on the symmetry of the problem, the population of the initial level does not depend on the pulse order at any \ensuremath{\Delta}. Furthermore, we demonstrate that the population transfer in the three-level system can be viewed as a level-crossing problem in an equivalent two-level system not only at large \ensuremath{\Delta} (which is known) but also on resonance, \ensuremath{\Delta}=0. The effective on-resonance two-level problem is interesting by itself as it shows that a level crossing and adiabatic evolution do not necessarily lead to complete population inversion. As examples throughout the paper, we present several analytically solvable models.
Ongoing work aimed at developing highly efficient methods of populating a chosen sublevel of an energy level highlights the need to understand off-resonant effects in coherent excitation. This motivated us to re-examine some aspects of the theory of coherent excitation in a three-state system with a view to obtaining algebraic expressions for off-resonant eigenvalues and eigenvectors. Earlier work gives simple closed-form expressions for the eigenvalues this system, expressions applying even when the system is not on two-photon resonance. We present here expressions of similar simplicity for the components of the normalised eigenvectors. The analytic properties of these components explain the observed sensitivity of the stimulated-Raman-adiabatic-passage process (STIRAP) to the condition of two-photon resonance. None of the eigenstates is ‘trapped’ or ‘dark’ unless the system is on two-photon resonance; off resonance, all states have nonzero projections on the unperturbed intermediate state. A simple argument shows that no dressed state can be adiabatically connected to both the unperturbed initial and final states when the system is off two-photon resonance. That is, adiabatic transfer from initial to final state requires that these be degenerate before and after the STIRAP pulse sequence, and this implies zero two-photon detuning. However, substantial transfer probabilities are observed experimentally for very small two-photon detunings. We show that such systems are characterised by very sharp avoided crossings of two eigenvalues, and that the observed population transfer can be understood as an effect of non adiabatic transitions occurring at the avoided crossings.