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# TEN BILLION YEARS OF GALAXY EVOLUTION

## 1 INTRODUCTION

As paleontologists dig down to deeper layers in the Earth they encounter ever older fossils. By the same token astronomers can look back in time by observing galaxies at ever larger redshifts. The high resolution provided by the Hubble Space Telescope (HST) makes it possible to study the evolution of the structure within galaxies over time-scales approaching the age of the Universe. Astronomers can now explore the evolution of morphological classes of galaxies in ways that are similar to those in which paleontologists study the evolution of fossil species and genera over time. Perhaps the most unexpected result of such work is that the Hubble tuning fork diagram only provides a satisfactory framework for the classification of galaxies with $`z0.5`$, i.e. for galaxies with ages 111All ages used in the present paper are for a Universe in which h = 0.7, $`\mathrm{\Omega }_m`$ = 0.3 and $`\mathrm{\Omega }{}_{\mathrm{\Lambda }}{}^{}=0.7`$ less than half the age of the Universe. Furthermore, with increasing look-back time, it becomes ever more difficult to shoehorn galaxies into the morphological sequence Sa - Sb - Sc.

It is the purpose of the present paper to examine the details of how the Hubble classification scheme breaks down with increasing redshift. Part of the evolution of galaxies over the last 10 Gyr is, no doubt, due to internal factors, whereas the rapidly growing frequency of mergers with increasing redshift is beautifully visible on HST images. Such growth in the merger frequency with increasing redshift, which is expected from hierarchical merger models (Carlberg 2000), provides an external contribution to the secular changes of galaxy morphology. Strong observational support for a rapid increase in the merger and accretion rate of galaxies towards larger redshifts is provided by the present data, and by observations of Patton et al. (2002).

## 2 CHANGES OF GALAXY MORPHOLOGY WITH TIME

The Ohio State Bright Spiral Galaxy Survey of Eskridge et al. (2002) provides a more or less unbiased (van den Bergh et al. 2002) sample of nearby spiral galaxies. After degrading 101 of these images to the resolution and signal-to-noise ratio of galaxies at z = 0.7 in the Hubble Deep Field (HDF) van den Bergh et al. (2002) find that only 12% of these objects at $`z0.0`$ are classified as being peculiar. Such peculiar galaxies are, by definition, galaxies that do not fit comfortably into the Hubble classification scheme. This observed fraction of peculiar objects among nearby spirals is significantly lower than that encountered in the HDF and its Flanking Fields (FF), in which van den Bergh et al. (2000) found that 17 out of 37 (46%) of spirals with $`0.60<z<0.89`$ are peculiar. In other words almost half of all spiral galaxies appear to be peculiar at look-back times of $``$ 8 Gyr. This comparison is almost independent of bandshift effects because the ground-based z = 0 images were classified in B light, whereas the classifications of galaxies at $`z0.7`$ were made in the infrared F814W band. In other words the galaxies at z = 0.0 and z = 0.7 were classified at almost the same rest wavelength.

Van den Bergh et al. (2000) show that distant early-type galaxies are less likely to be peculiar than is the case for galaxies of later morphological types. Only 1/22 (5%) of E - Sa - Sab galaxies were observed to be peculiar at $`z0.7`$, compared to 11/16 (69%) of Sb-Sbc galaxies. These figures probably under-state the difference in the fraction of peculiar early-type and late-type galaxies. This is so because a significant fraction of “Sc” galaxies are so peculiar at $`z0.7`$ that many of them have been classified as “proto-Sc”, “Pec”, or “?”. These results suggest that compact early-type galaxies started to approach their “normal” present-day morphology faster than did more extended late-type spirals. However, a caveat is that it might be more difficult to see peculiarities in distant compact early -type galaxies than in equally distant (but more open) late-type spirals.

## 3 BARRED SPIRALS

Hubble (1936) noted that nearby spiral galaxies fall naturally into two sequences, which he dubbed “normal spirals” \[Sa - Sb - Sc\] and “barred spirals” \[SBa - SBb - SBc\]. One of the first surprises (van den Bergh et al. 1996) provided by inspection of the Hubble Space Telescope images of the Hubble Deep Field North (HDFN) (Williams et al. 1996) was that the frequency of barred spirals appeared to decrease with increasing redshift. This conclusion was subsequently confirmed in the HDFN and HDFS by Abraham et al. (1999). However, before accepting this conclusion, one has to test whether the apparent decrease in the frequency of bars with increasing redshift might be due to (1) diminishing resolution with increasing redshift and/or (2) to a decrease in the signal-to- noise ratio with increasing z. Furthermore such investigations have to be carried out at constant rest wavelength to guard against a possible wavelength dependence of the frequency of bars (Eskridge et al. 2000). Such an investigation has recently been undertaken by van den Bergh et al. (2002) who compared the fraction of barred objects among a representative sample of nearby spirals observed in blue light, with the fraction of galaxies classified as SB in the same sample of galaxies, but with resolution and signal-to-noise ratio degraded to that for HST images at $`z0.7`$. To compensate for band shift effects these degraded images were classified in the HST F814W band. The data showed that $``$2/3 of the strongly barred \[DDO types SB0-SBa-SBb-SBc\] galaxies could still be recognized as barred spirals at $`z0.7`$. In other words most of the observed decrease in the frequency of SB galaxies between z = 0.0 and z = 0.7 is intrinsic, and not due to the effects of a decrease in resolution and noise with increasing redshift. However, it should be emphasized that such resolution and noise problems might render some bars (if they exist) unobservable at $`z0.7`$.

Table 1 lists the fraction of all spirals (including objects of type S0) with known redshifts that are barred in the HDF (North) from van den Bergh et al. (2000), and in the HDF (South) from van den Bergh & Abraham (2002). These data show that the fraction of barred \[S(B) + S(B?) + SB\] spirals decreases from $``$23% for galaxies with $`z<0.5`$ to $``$4% for galaxies with $`z>0.7`$. As has already been noted above all of these classifications were made at, or close to, the ground-based B band. Taken at face value these results suggest that the frequency of barred spirals at $`z>0.5`$ might be lower than it is in nearby regions of the Universe. If confirmed by future observations, this result could be explained by assuming that the disks of spirals at large look-back times are still too chaotic (dynamically hot) to be susceptible to global bar-like instabilities. Such global dynamical instability of disks is currently (Sellwood & Willkinson 1993) the favored formation mode for bars in spiral galaxies. The notion that galaxies at large redshifts are more chaotic than nearby ones is also supported by the work of Reshetnikov et al. (2002), who find that disks at large redshifts are (on average) more often warped than are the disks of nearby galaxies.

It is noted in passing that only $``$ 40% of strongly barred galaxies with I(814W) $`<22`$ mag, degraded to the resolution and signal-to-noise ratio of the HDF FF (corresponding to an integration time of two orbits), were recognizable as barred spirals. This clearly shows that the low signal-to-noise ratio in the Flanking Fields makes it more difficult to recognize bar-like features in distant galaxies.

In the original version of this paper it was noted that the HDF(South) galaxy J223302.81-603325.2, at a photometric redshift z = 1.578, is the only presently known barred spiral at a large redshift. However, a more recent photometric redshift of this object that is posted on the Stony Brook web site (see http:// www.ess.sunysb.edu/astro.hdfs) appears to show that the photometric redshift of this object is actually only z = 0.76. At this much lower redshift it is less surprising to find a barred spiral.

## 4 GRAND-DESIGN SPIRALS

Luminous “grand-design” spiral galaxies of DDO luminosity classes I, I-II, and II have large dimensions and are therefore relatively easy to recognize at great distances. The combined data for the HDF(North) by van den Bergh et al. (2000) and for the HDF(South) by van den Bergh & Abraham (2002) contain classifications for 110 spirals of known redshift, of which only seven are grand-design objects. None of these grand-design spirals have $`z>0.7`$. Possibly this lack of very distant grand- design spirals is linked to the observation that the spiral structure of late-type galaxies appears to become increasingly chaotic as one moves to larger redshifts. However, it is not yet safe to conclude that grand-design spirals only exist at low redshifts. This is so because a Kolmogorov-Smirnov test on small samples described above shows no statistically significant difference between the redshift distributions of ordinary spirals and of grand-design spirals. So it is not yet possible to say at which epoch luminous disk galaxies started to form their grand- design spiral features. It would clearly be of great interest to look into this question in more detail by obtaining redshifts (and accurate morphological classifications) for much larger samples of distant grand-design spirals. A possible complication is provided by the fact that some interacting objects at $`z>0.7`$ exhibit tidal features that might be confused with the chaotic spiral arms that are diagnostic of the most distant known spiral galaxies.

## 5 FREQUENCY OF CLASSIFICATION TYPES

A number of authors (Brinchmann et al. 1998, Lilly et al. 1995,1998, van den Bergh 2001) have considered the possible evolution of the frequency distributions of galaxy types over time. In particular Lilly et al. (1995) and van den Bergh (2001) concluded, from observations of galaxies in the Canada-France Redshift Survey, that there is very little change in either the density (or in the luminosity) of the reddest (early-type) galaxies over the entire range $`0<z<1`$. However, this conclusion should be treated with caution because changes in the space density \[and hence galaxy morphology along any particular line of sight\] may be affected by the well known correlation (Dressler 1980) between the frequency of classification types and space density. To avoid such problems in the future it will be necessary to undertake deep homogeneous redshift and classification surveys of numerous galaxies at many positions on the sky. Only in this way will it eventually be possible to gain better insight into systematic changes in the relative frequency distributions of different galaxy types with look-back time.

## 6 MERGERS

Both the HDF(North) and the HDF(South) are crowded fields. It is therefore expected (and spectroscopy confirms) that a significant fraction of all close binary galaxies are optical, rather than physical, pairs. Galaxies were therefore only classified as a “Merger” if (1) their main bodies overlapped or (2) if their outer structures appeared to show evidence for physical overlap or tidal distortion. Since faint outer tidal features are probably “lost in the noise” in the short exposure Flanking Fields. Only classifications in the Hubble Deep Fields themselves (van den Bergh, Cohen & Crabbe 2001, van den Bergh & Abraham 2002) were used to estimate the fractions of merging galaxies that are listed in Table 2. These data show that about 5% of galaxies with $`z<1.2`$ in the Hubble Deep Fields appear to be mergers. For comparison (see Table 2) van den Bergh & Abraham (2002) find that 62 out of 109 (57%) of their sample of HST galaxies with (mostly photometric) redshifts of $`z>2.0`$ appear to be mergers. In other words the typical galaxy at $`z<1`$ (age $`<8`$ Gyr) is single, whereas the average object at $`z>2`$ (age $`>10`$ Gyr) appears to be merging.

## 7 GALAXY MORPHOLOGY AT $`z>2`$

The majority of galaxies with $`z<1`$ are observed to be disk galaxies. On the other hand a large fraction of the galaxies with $`z>2`$ are best described as resembling centrally concentrated “blobs”, many of which appear to be interacting (or merging) with other blobs. Probably these blobs are the progenitors of our present day galactic bulges and elliptical galaxies. This speculation is supported by the observation that the objects seen at $`z>2`$ typically have quite small linear dimensions (Ferguson, Dickinson & Williams 2000). Furthemore fitting of multi-color observations to evolutionary models (Popovich, Dickinson Ferguson 2001) suggests masses of $`10^9`$-$`10^{11}`$ $`\mathrm{\Omega }_{}`$ for the luminous inner regions of Lyman break galaxies (LBGs). Such values are diagnostic for the cores of galaxies rather than rather than of giant young star clusters. Clustering properties of LBGs have so far placed placed only weak constraints (Primack, Wechsler & Somerville 2002) on the masses of the halos of Lyman break galaxies.

### 7.1 Morphology at $`z<1`$

As has been noted above galaxy morphology starts to deviate noticeably from that of the templates of the Hubble classification system at redshifts $`z>0.5`$. At $`z1`$ it becomes increasingly difficult to shoehorn most galaxies into the Hubble classification system. In the range $`1<z<2`$ galaxy morphology appears to be complex, with some characteristics that are reminiscent of the the Hubble system and others that are similar to those of the galaxies at $`z>2`$. The change in the global rate of star formation between $`z1`$ and $`z2`$ (e.g. Madau, Pozetti & Dickinson 1998, Barkana 2002) might be due to the change in the mode of star formation from one that is merger dominated at $`z>2`$ to a disk dominated phase at $`z<1`$. It is, of course, important to realize that the history of star formation may have been very different from the history of mass assembly and its subsequent re-arrangeement.

### 7.2 Morphology at $`z>2`$

The recent NICMOS $`H_{160}`$ images of galaxies with $`2<z<3`$ by Dickinson (2000) show that (after correcting for a difference in linear resolution) the morphology of galaxies is surprisingly similar at $`\lambda _o=1700`$Å and at $`\lambda _o=4300`$Å. This result suggests that the apparent structure of the images of such distant galaxy is mainly determined by their intrinsic morphology and is not a strong function of bandshift effects. This result shows that: (1) The stars that dominate the light at $`\lambda `$ $`\lambda _o12001800`$Å also dominate at $`\lambda `$ $`\lambda _o40005500`$Å. (2) If components of differing age are present they must usually have a rather well-mixed spatial distribution. (3) Dust extinction cannot be the dominant factor determining the overall structure of most galactic images at high redshift. In view of these results it appears safe to neglect band shift effects for first-order studies of the morphology of galaxies with $`z>2`$.

Many of the galaxies at $`z>2`$ are so different from those at low redshifts that it would be quite meaningless to assign Hubble types to them. Proceeding in an entirely pragmatic fashion van den Bergh and Abraham (2002) have established an empirical classification scheme for these objects which is illustrated in Figure 1. The tentative classification system of van den Bergh & Abraham has two parameters. The first of these indicates whether a system appears to be single (s), binary (b) or multiple (m). It should, of course, be emphasized that such a classification system is somewhat arbitrary because a member of a wide binary might reasonably also be considered a single. Furthermore a system with two bright and one faint components might be classified as a binary, rather than as a multiple system. The second classification parameter describes the structure of the brightest component of the system. Small, compact, circular knots are denoted by “1”, slightly fuzzy brightest components are classified “2”, fuzzy images with a comma-like structures are assigned to class “3”, and tadpole-like objects with a longer tails are designated type “4”. Finally chain galaxies (Cowie, Hu & Songaila 1995) are assigned to class “5”. It is not yet clear if the formation of such galaxy chains is in any way related to the filamentary structures that are found in numerical simulations of the early evolution of cold dark matter. It, perhaps, should be emphasized that the classification types “1”, “2” and “3” refer to the structure of the brightest knots within structures, which may themselves be quite chaotic.

In the nomenclature adopted in the present paper “s1” denotes a compact single object,“b2” a binary with a slightly fuzzy brightest component and “m3” a multiple object with a comma-like brightest component. For objects of types 4 and 5 the s, b and m designations are not appropriate. It is not yet clear if the strictly empirical system described above correlates with luminosity, integrated spectral type or any other physical characteristic of the objects being classified. In this connection it is, however, of interest to note that all 9 of the most distant $`(z>3.5)`$ objects classified by van den Bergh & Abraham are single objects of types s, s1 or s2. The lack of outer “fuzz” in these objects might, at least in part, be due to the effects of cosmological $`(1+z)^4`$ dimming of the faint outer regions of these “galaxies”. From a morphological point of view the most distant objects in the HDF(North) and the HDF(South) might also be assigned to Hubble types E0 - E3 or Sa. It is of interest to note that none of the objects with $`z>3.5`$ appear to be as flattened as edge-on spirals or E4-E7 galaxies. This result is somewhat puzzling because widely accepted cold dark matter evolutionary scenarios (e.g. Kauffmann, White & Guideroni 1993, Baugh et al. 1998) form ellipticals from merging disk galaxies. Why do we not observe such disks at large look-back times? Possibly (Weil,Eke & Efstthiou 1998) such stellar disk would be destroyed by frequent mergers at $`z2`$ and by stellar feedback processes that suppress cooling of gas before $`z1`$. The destruction of disks by tides and mergers at large look-back times might account for the unexpectedly small half-light radii of galaxies at $`z>1.5`$ (e.g. Roche et al. 1998).

If the speculation that the formation of disks is impeded by frequent mergers and tidal effects is correct, then one would not expect large spirals (such as the Milky Way) to contain a very old thin-disk population component.

## 8 CONCLUSIONS

The main results of investigations of the dependence of galaxy morphology on redshift may be summarized as follows:

* A major transition in the dominant mode of galaxy and star formation is observed to occur between $`z1`$ and $`z2`$. At low redshifts most star formation is presnetly taking place quiescently in well-ordered disks. On the other hand much of the star formation at high redshifts appears to be associated with chaotic mergers.
* This change might contribute to the change in the slope of the Madau plot that is observed at $`z1.5`$.
* The majority of objects with $`z<1`$ are disk-like, whereas most of those with $`z>2`$ appear to either be chaotic, or have dominant bulge-like components. A non-exhaustive list of possible scenarious includes: (1) the first disks were destroyed by frequent mergers, (2) that the gas in these disks did not cool before $`z1`$, or (3) early gaseous disks were destroyed by the strong winds resulting from massive starbursts.
* The Hubble tuning fork diagram only provides a good framework for the classification of galaxies with $`z0.5`$.
* Study of artificially degraded images shows that the fraction of all galaxies that are barred spirals decreases with increasing redshift. This effect is tentatively interpreted as being due to the fact that hot (chaotic) disks might not be able to develop global bar-like instabilities.
* The fraction of peculiar galaxies, i.e. objects that do not fit naturally into the Hubble classification scheme increases from 12% at z = 0.0 to 46% at $`z0.7`$.
* Compact early-type (E-Sab) galaxies appear to approach their final morphology more rapidly than do more extended late-type (Sbc-Sc) galaxies. As a result only $``$5% of early type galaxies at $`z0.7`$ appear peculiar, compared to 69% peculiars among late-type galaxies.
* At look-back times greater than 5 Gyr $`(z>0.5)`$ the spiral arm structure of early-type galaxies appears to be under- developed.
* At look-back times greater than 7 Gyr $`(z>0.8)`$ the structure of the spiral arms of late-type galaxies appears less regular (more chaotic) than it does at lower redshifts. It should be emphasized that this is an easily observed gross effect that is not likely to be affected by either noise or image resolution.
* A tentative, and strictly empirical, classification scheme is proposed for those objects that are viewed at look-back times greater than 10 Gyr $`(z>2)`$.

It is a pleasure to thank numerous colleagues who, during the last six years, have contributed to my musings on the evolution of galaxy morphology over time. Particular thanks go to Bob Abraham and Judy Cohen for their encouragement and assistance and to Chuck Steidel for cosmological consultations and to Simon Lilly for interesting suggestions. I am also indebted to David Duncan for drawing Figure 1.

Figure Caption

1. Illustration of a very tentative empirical classification scheme used to describe the morphologies of objects with $`z>2`$.


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# Resonant nonlinear optics in coherently prepared media: full analytic solutions

## I Introduction

Resonant nonlinear optics in atomic gases has received a great impetus in recent years due to new concepts based on the application of specific coherence and interference effects. Two of these concepts attracted particular attention. The first mechanism uses the effect of electromagnetically induced transparency (EIT) har97 ; harr90 , the second maximum coherence between two metastable atomic levels jain96 . Both schemes allow for high-efficiency nonlinear conversion with substantially alleviated phase-matching problems in a rather dilute ensemble of atoms if the medium is driven by an undepleted coherent coupling field or if an undepleted atomic coherence is assumed. These assumptions do not take into account the resources needed to maintain the drive field or atomic coherence. Thus in the considered limit the overall efficiency of the resonant nonlinear processes is small. In the present paper we analyze and compare EIT- and maximum-coherence based systems with each other and with the conventional non-resonant schemes of nonlinear optics taking into account the transparency- or coherence-maintaining fields and their depletion. Effects of inhomogeneous broadening are however disregarded. Deriving analytic solutions for the nonlinear pulse propagation problem, we show that in both systems also a large overall conversion efficiency can be achieved. The physical nature of the conversion can however no longer be associated with EIT or maximum coherence alone.

In EIT a strong resonant electromagnetic (em) field of frequency $`\omega _2`$ is applied to the transition between two excited states $`|2`$ and $`|3`$, (Fig.1a), causing a splitting of both (Autler-Townes effect). When a weak probe field of frequency $`\omega _3`$ resonant with the transition from the ground-state $`|1`$ to the bare state $`|3`$ is applied, its linear interaction with the medium is almost perfectly cancelled. The vanishing of the linear susceptibility, i.e. absorption and refraction, for the probe field is due to a destructive interference between the two excitation paths through the Autler-Townes doublet and persists even for small splittings. If the ground state $`|1`$ is coupled to the intermediate state $`|2`$, on the other hand (e.g. by a two-photon transition), photons of frequency $`\omega _3`$ are generated. While the resonant linear absorption of these photons is suppressed by destructive quantum interference (EIT), the nonlinear susceptibility responsible for the generation of them is only affected by the splitting, which can be rather small. Since there are no resonant contributions to the refractive index, there is furthermore perfect phase matching except for contributions from other off-resonant transitions. Owing to the large dispersion near the transparency frequency of EIT, a small detuning $`\delta _2`$ can be applied to compensate for these contributions and phase matching can easily be obtained without sacrificing the cancellation of absorption. Thus EIT provides a perfect system for large nonlinear conversion with a minimum of atoms. Since the first demonstration of phase matching in EIT-assisted four-wave frequency mixing jain93 , many other experiments confirmed considerable improvement in the conversion efficiency when EIT has been used (see, e.g., Refs. stoi ; maran ).

Another mechanism proposed recently is referred to as nonlinear optics with maximum coherence jain96 ; mer99 . The idea is here to prepare and maintain the atoms in a coherent superposition of atomic states $`|1`$ and $`|2`$ with equal amplitudes. This can be done either by two strong fields exciting the $`|1|2`$ coherence via a Raman transition jain96  or by other means such as rapid adiabatic passage scrap . The coherence, established in such a way, plays the role of a strong local oscillator. If then a relatively weak field $`\omega _2`$ detuned by a sufficiently large amount $`\delta _3`$ from the $`|2|3`$ transition is applied, Fig. 1b, it will beat against the local oscillator to generate the sum (or difference) frequency. Here, the refraction due to resonant transitions does not vanish. But since the nonlinear coupling strength is of the same order as the linear susceptibility, complete conversion occurs over a distance smaller than the coherence length boyd . Consequently there is no need to phasematch the propagating beams. We note that the relation between the $`|1|2`$ coherence and the wave mixing processes has been pointed out in earlier work on nonlinear optics (see, e.g., Refs. wil82  and references therein).

In the limit of undepleted drive or constant coherence, the nonlinear conversion process in both the EIT and maximum coherence scheme affects the quantum state of the atoms only in the perturbative sense. Consequently the probability of photon conversion per atom is small. For the same reason the overall conversion efficiency including the transparency and coherence generating fields is small. We here analyze the properties of the two mechanisms for arbitrary strength of the drive fields taking into account their depletion and compare them to conventional off-resonant nonlinear optics.

The drive depletion turns the propagation problem into a truly nonlinear one. Its solution is particularly challenging for pulses and is in general possible only numerically. In order to obtain transparent analytical solutions we here apply the so-called Hamiltonian approach mel79 ; kryz ; McK90 ; cap91  which allows for a solution in a wide range of physically relevant situations. This approach is especially useful under adiabatic conditions, i.e. when the atoms are excited by the laser pulses in such a way that they remain in the same instantaneous eigenstate of the interaction Hamiltonian during the entire process. In the present work, we will assume that the interaction is adiabatic. The adiabatic approximation requires a slow rate of evolution as compared to the frequency separation of the adiabatic eigenstates. This results usually in a requirement for the product of the pulse duration and the Rabi frequency of the radiation field to be much larger than unity. Thus, for sufficiently intense fields, the process can be adiabatic even for short pulses. It should be noted however that this assumption rules out such important effects as group velocity reduction which results from lowest-order non-adiabatic corrections. For sufficiently large intensities or cw fields these effects do not influence the process. An analysis of non-adiabatic corrections to the Hamiltonian approach taking into account group delays will be given in a future publication.

To simplify the calculations and the interpretation of the analytic results, we restrict ourselves to a somewhat idealized three-level atomic excitation scheme (Fig. 1). The nonlinear three-wave mixing in a three-level system is normally forbidden due to symmetry boyd . However, this scheme provides the simplest example where all above mentioned mechanisms of nonlinear-optical wave mixing may take place. It should be noted that similar results, however with much lengthier expressions and larger number of atomic parameters, can be found for a more realistic three-level scheme where $`|1|2`$ transition is a two-photon one to-be-published . Moreover, the 3-wave-mixing processes is possible when a dc electric field is applied to the atomic sample hak91 .

The paper is organized as follows. In Sec.II we discuss resonant nonlinear optical processes based on EIT or maximum coherence for undepleted drive fields or undepleted coherence, respectively, and compare them to conventional off-resonance nonlinear optics. In Sec.III we outline the Hamiltonian approach, which allows to eliminate the atomic degrees of freedom assuming adiabatic following and to map the pulse propagation problem to the dynamics of a one-dimensional nonlinear pendulum. Making use of this formalism we derive full analytic solution for EIT and maximum-coherence based nonlinear optics in Sec.IV, taking into account drive-field and coherence depletion.

## II Resonant nonlinear optics in a coherently prepared 3-level system

We first consider the propagation of pulsed em fields in a medium of three-level atoms (Fig. 1) in which either a constant drive field mixes the two excited states $`|2`$ and $`|3`$ or in which a constant coherence between the lower two states $`|1`$ and $`|2`$ is maintained. The first case corresponds to resonant nonlinear frequency conversion based on EIT har97 ; harr90 , the second one to nonlinear optics with maximum coherence jain96 . The electric field propagating in the $`z`$-direction is assumed to consist of three components with carrier frequencies $`\omega _1,\omega _2`$ and $`\omega _3=\omega _1+\omega _2`$:

$$E(z,t)=\underset{j}{}(_j(z,t)\mathrm{exp}(i(\omega _jtk_jz))+c.c.).$$
(1)
Here $`k_j=n_j\omega _j/c`$ with $`n_j`$ being the refractive index at frequency $`\omega _j`$ due to levels outside the three-level system of Fig. 1. This background refraction gives rise to the ”residual” phase mismatch determined as:

$$\mathrm{\Delta }k=k_1+k_2k_3.$$
(2)
In the approximation of slowly varying amplitudes and phases Maxwell’s propagation equations read in a moving frame

$$\frac{_j}{z}=i2\pi \frac{\omega _j}{c}𝒫_j,$$
(3)
where $`_j`$ and $`𝒫_j`$ are functions of the coordinate $`z`$ and the retarded time $`\tau =tz/c`$. $`𝒫_j`$ are the components of the medium polarization:

$$P=\underset{j}{}(𝒫_j\mathrm{exp}(i(\omega _jtk_jz))+c.c.),$$

which can be expressed in terms of the atomic probability amplitudes $`c_n`$ in levels $`|1`$, $`|2`$ and $`|3`$:

$`𝒫_1`$ $`=`$ $`Nd_1c_1^{}c_2,`$ (4)
$`𝒫_2`$ $`=`$ $`Nd_2c_2^{}c_3\mathrm{e}^{i\theta i\mathrm{\Delta }kz},`$ (5)
$`𝒫_3`$ $`=`$ $`Nd_3c_1^{}c_3,`$ (6)
$`N`$ being the density of active atoms. $`d_1`$, $`d_2`$ and $`d_3`$ are the real dipole moments of the transitions $`|1|2`$, $`|2|3`$ and $`|1|3`$ respectively. $`\theta `$ is phase of the $`|2|3`$ dipole moment, which in general cannot be chosen freely.

Assuming decay only from the top most state $`|3`$ with rate $`\gamma `$ the state amplitudes obey in rotating wave approximation the equations

$`\dot{c}_1`$ $`=`$ $`i\mathrm{\Omega }_1^{}c_2+i\mathrm{\Omega }_3^{}c_3,`$
$`\dot{c}_2`$ $`=`$ $`i\mathrm{\Omega }_1c_1+i\mathrm{\Omega }_2^{}\mathrm{e}^{i\theta i\mathrm{\Delta }kz}c_3+i\delta _2c_2,`$ (7)
$`\dot{c}_3`$ $`=`$ $`i\mathrm{\Omega }_2\mathrm{e}^{i\theta +i\mathrm{\Delta }kz}c_2+i\mathrm{\Omega }_3c_1+i\left(\delta _3+i\gamma \right)c_3,`$
where $`\delta _2`$ and $`\delta _3`$ are the frequency detunings indicated in Fig. 1.

$$\delta _2=\omega _1\omega _{21},\delta _3=\omega _3\omega _{31},$$
(8)
with $`\omega _{ij}`$ denoting the transition frequencies between the corresponding levels. $`\mathrm{\Omega }_1`$, $`\mathrm{\Omega }_2`$ and $`\mathrm{\Omega }_3`$ are the Rabi frequencies for transitions $`|1|2`$, $`|2|3`$ and $`|1|3`$, respectively:

$$\mathrm{\Omega }_j=\frac{d_j_j}{2\mathrm{}}.$$
(9)
### II.1 EIT with undepleted coupling field

Here, we consider three fields interacting with the 3-level system. For simplicity we assume $`\delta _3=0`$. Furthermore we consider the case of a strong, undepleted drive field with frequency $`\omega _2`$

$$\left|\mathrm{\Omega }_2\right|\left|\mathrm{\Omega }_1\right|,\left|\mathrm{\Omega }_3\right|,\gamma ,\left|\delta _2\right|.$$

Then, the solution of the atomic equations of motion (7) with the initial condition $`c_1\left(t\mathrm{}\right)=1`$ yields

$$\left|c_1\right|1.$$

Assuming quasi-adiabatic evolution, i.e. not too fast changing fields, we find

$`c_2`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_3\mathrm{\Omega }_2^{}e^{i\theta \mathrm{\Delta }kz}i\mathrm{\Omega }_1\gamma }{\left|\mathrm{\Omega }_2\right|^2i\delta _2\gamma }},`$
$`c_3`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_1\mathrm{\Omega }_2e^{i\theta +i\mathrm{\Delta }kz}\mathrm{\Omega }_3\delta _2}{\left|\mathrm{\Omega }_2\right|^2i\delta _2\gamma }}.`$
Substitution into Maxwell’s propagation equations gives:

$`{\displaystyle \frac{_1}{z}}`$ $`=`$ $`{\displaystyle \frac{\pi Nd_1^2}{\mathrm{}}}{\displaystyle \frac{\omega _1}{c}}{\displaystyle \frac{\gamma }{\left|\mathrm{\Omega }_2\right|^2}}_1`$
$`i{\displaystyle \frac{\pi Nd_1d_3}{\mathrm{}\left|\mathrm{\Omega }_2\right|}}{\displaystyle \frac{\omega _1}{c}}e^{i\theta i\mathrm{\Delta }kz}_3,`$
$`{\displaystyle \frac{_3}{z}}`$ $`=`$ $`i{\displaystyle \frac{\pi Nd_3^2}{\mathrm{}}}{\displaystyle \frac{\omega _3}{c}}{\displaystyle \frac{\delta _2}{\left|\mathrm{\Omega }_2\right|^2}}_3`$
$`i{\displaystyle \frac{\pi Nd_1d_3}{\mathrm{}\left|\mathrm{\Omega }_2\right|}}{\displaystyle \frac{\omega _3}{c}}e^{i\theta +i\mathrm{\Delta }kz}_1.`$
Equations (II.1) and (II.1) are linear differential equations, which can easily be solved. We now consider the case in which no $`_3`$ field is incident on the medium, $`_3\left(z=0\right)=0`$. Introducing the normalized intensity (photon flux)

$$\eta _j=\frac{I_j}{\mathrm{}\omega _j}\frac{c\left|_j\right|^2}{8\pi \mathrm{}\omega _j}$$
(12)
and the coupling strength

$$\mu _j=\frac{2\pi \omega _jd_j^2}{\mathrm{}c},$$
(13)
the solution of equations (II.1) and (II.1) reads:

$$\eta _3(z)=\frac{\eta _{10}}{1+\left(\mathrm{\Delta }k^{}/2\kappa \right)^2}\mathrm{e}^{\mathrm{\Gamma }\kappa z}\mathrm{sin}^2\left(\kappa z\sqrt{1+\left(\mathrm{\Delta }k^{}/2\kappa \right)^2}\right),$$
(14)
where $`\eta _{10}=\eta _1(z=0)`$ is the photon flux at the entrance to the medium and we have introduced the conversion coefficient $`\kappa `$:

$$\kappa =\frac{N}{2}\frac{\sqrt{\mu _1\mu _3}}{|\mathrm{\Omega }_2|},$$
(15)
the loss coefficient $`\mathrm{\Gamma }`$:

$$\mathrm{\Gamma }=\frac{\gamma }{|\mathrm{\Omega }_2|}\sqrt{\frac{\mu _1}{\mu _3}},$$
(16)
and

$$\mathrm{\Delta }k^{}=\mathrm{\Delta }k\frac{N}{2}\frac{\mu _3\delta _2}{\left|\mathrm{\Omega }_2\right|^2}$$
(17)
is the total phase mismatch, including the background value $`\mathrm{\Delta }k`$ and the contribution from resonant transition $`|1|3`$. In the EIT case, the resonant contribution to the phase mismatch is always smaller than the conversion coefficient $`\kappa `$ by a factor $`\delta _2/|\mathrm{\Omega }_2|`$. Moreover, a small detuning $`\delta _2`$ can be introduced to compensate the residual phase mismatch. Thus, the EIT scheme represents an ideal situation with complete phase matching, where the optimum conversion occurs for a density-length product

$$Nz|_{\mathrm{opt}}=\pi \frac{|\mathrm{\Omega }_2|}{\sqrt{\mu _1\mu _3}}.$$
(18)
In order to minimize the absorption losses, Eq. (16), the Rabi frequency of the coupling field $`\left|\mathrm{\Omega }_2\right|`$ has to be sufficiently large:

$$|\mathrm{\Omega }_2|\sqrt{\frac{\mu _1}{\mu _3}}\gamma .$$

### II.2 Undepleted coherence $`\rho _{12}`$

In the following we discuss the scheme of resonant nonlinear optics with maximum coherence. For this situation, constant state amplitudes $`c_1`$ and $`c_2`$ are assumed, maintained e.g. by a constant strong drive field $`\mathrm{\Omega }_1`$. In this case the wave vector of the atomic coherence $`c_1^{}c_2`$ is equal to $`k_1`$ which can be changed by, e.g., the small detuning $`\delta _2`$ jain96 . The backaction of the atoms to this field is disregarded and thus the corresponding coupling does not need to be taken into account. Under the condition

$$\left|\delta _3+i\gamma \right|\left|\mathrm{\Omega }_j\right|$$

the amplitude of the excited state can be adiabatically eliminated, which yields

$$c_3=\frac{\mathrm{\Omega }_2e^{i\theta +i\mathrm{\Delta }kz}c_2+\mathrm{\Omega }_3c_1}{\delta _3+i\gamma }.$$
(19)
Substitution of Eqs. (5), (6), (19) into the Maxwell propagation equations (3) gives:

$`{\displaystyle \frac{_2}{z}}`$ $`=`$ $`i{\displaystyle \frac{\pi Nd_2^2}{\mathrm{}}}{\displaystyle \frac{\omega _2}{c}}{\displaystyle \frac{\delta _3i\gamma }{\delta _3^2+\gamma ^2}}\left|c_2\right|^2_2`$
$`i{\displaystyle \frac{\pi Nd_2d_3}{\mathrm{}}}{\displaystyle \frac{\omega _2}{c}}{\displaystyle \frac{\delta _3i\gamma }{\delta _3^2+\gamma ^2}}\rho _{12}e^{i\theta i\mathrm{\Delta }kz}_3,`$
$`{\displaystyle \frac{_3}{z}}`$ $`=`$ $`i{\displaystyle \frac{\pi Nd_3^2}{\mathrm{}}}{\displaystyle \frac{\omega _3}{c}}{\displaystyle \frac{\delta _3i\gamma }{\delta _3^2+\gamma ^2}}\left|c_1\right|^2_3`$
$`i{\displaystyle \frac{\pi Nd_2d_3}{\mathrm{}}}{\displaystyle \frac{\omega _3}{c}}{\displaystyle \frac{\delta _3i\gamma }{\delta _3^2+\gamma ^2}}\rho _{12}e^{i\theta +i\mathrm{\Delta }kz}_2,`$
where $`\rho _{12}=\left|c_1^{}c_2\right|`$.

This is again a set of linear differential equations whose solution has the same form as that for the EIT case, Eq. (14), with the substitution $`\eta _{10}\eta _{20}`$ and corresponding parameters (assuming $`\delta _3\gamma `$):

$`\kappa `$ $`=`$ $`{\displaystyle \frac{N}{2}}{\displaystyle \frac{\sqrt{\mu _2\mu _3}}{\delta _3}}\rho _{12},`$ (22)
$`\mathrm{\Gamma }`$ $`=`$ $`{\displaystyle \frac{\gamma }{\delta _3}}{\displaystyle \frac{\mu _2\left|c_2\right|^2+\mu _3\left|c_1\right|^2}{\rho _{12}\sqrt{\mu _2\mu _3}}},`$ (23)
$`\mathrm{\Delta }k^{}`$ $`=`$ $`\mathrm{\Delta }k+{\displaystyle \frac{N}{2}}{\displaystyle \frac{\mu _3\left|c_1\right|^2\mu _2\left|c_2\right|^2}{\delta _3}}.`$ (24)
The total phase mismatch $`\mathrm{\Delta }k^{}`$ includes the background value $`\mathrm{\Delta }k`$ and the contributions from resonant transitions $`|1|3`$ and $`|2|3`$.

For atomic media which we consider here, the off-resonant (background) contributions to the refractive index $`n_j`$ are of the order of boyd :

$$n_j1+N\frac{c}{\omega _j}\underset{m}{}\frac{\mu _{jm}}{\delta _{jm}},$$
(25)
where $`\mu _{jm}`$ and $`\delta _{jm}`$ are the coupling constants and detunings, respectively, for the wave with frequency $`\omega _j`$ and transition to the far-detuned state $`|m`$ not belonging to the three-level system of Fig. 1. Since $`\delta _{jm}\delta _3`$, the resonant contributions to the phase mismatch are the dominant ones. As can be seen from Eqs.(22) and (24), they are in general of the same order as the conversion coefficient $`\kappa `$ if the atomic coherence $`\rho _{12}`$ is large (of the order of $`1/2`$). Therefore, efficient energy transfer from the $`\omega _2`$ field into the $`\omega _3`$ field: $`\eta _3(l)\eta _{20}`$, occurs already within a length $`l=\kappa ^1L_c=2/\mathrm{\Delta }k^{},`$ the coherence length. This feature constitutes the main advantage of the maximum coherence scheme over conventional nonlinear optics, because the phase matching is no longer important.

If the conversion length $`l`$ is much smaller than the coherence length $`L_c`$, $`l/L_c1`$, and the losses are small, $`\left(\mathrm{\Gamma }/l\right)z|_{\mathrm{opt}}1`$, maximum conversion occurs for a density-length product

$$Nz|_{\mathrm{opt}}=\frac{\pi }{2}Nl=\pi \frac{\delta _3}{\rho _{12}\sqrt{\mu _2\mu _3}}.$$
(26)
$`l/L_c1`$ is realized when the parameters are chosen such that $`\mathrm{\Delta }k^{}`$ is small, or even better, vanishes, i.e. if

$$\frac{2\mathrm{\Delta }k}{N}\frac{\mu _2\left|c_2\right|^2\mu _3\left|c_1\right|^2}{\delta _3}.$$

This can be achieved in different ways: (i) by tuning the wave vector $`k_1`$ of the atomic coherence (e.g., by introducing a detuning $`\delta _2`$, as in Ref. jain96 ), (ii) by selecting the appropriate detuning $`\delta _3`$, as in Ref. mer99 , and/or, by preparation of atoms in a superposition with suitable amplitudes $`c_1,c_2`$.

In order for the absorption losses to be negligible within the optimum propagation distance, the following condition has to be satisfied:

$$\frac{\gamma }{\delta _3}\frac{1}{\rho _{12}}1,$$

which indicates once again that it is indeed advantageous to prepare a large atomic coherence $`\rho _{12}`$.

### II.3 Conventional nonlinear optics: weak excitation

Now, we discuss the case of a weak excitation of atoms which corresponds to the regime of conventional nonlinear optics. The weak excitation takes place, for example, when both detunings are very large:

$$\left|\delta _3\right|,\left|\delta _2\right|\left|\mathrm{\Omega }_j\right|,\gamma .$$

Under this condition, the atomic probability amplitudes are:

$`\left|c_1\right|`$ $``$ $`1,`$
$`c_2`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_1\mathrm{\Omega }_2e^{i\theta +i\mathrm{\Delta }kz}\mathrm{\Omega }_3\delta _2}{\delta _2\left(\delta _3+i\gamma \right)}},`$
$`c_3`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_3\mathrm{\Omega }_2^{}e^{i\theta i\mathrm{\Delta }kz}\mathrm{\Omega }_1\left(\delta _3+i\gamma \right)}{\delta _2\left(\delta _3+i\gamma \right)}}.`$
Since $`\left|c_2\right|,\left|c_3\right|\left|c_1\right|`$, the medium polarization at frequency $`\omega _2`$ is much smaller than for the $`\omega _1`$ and $`\omega _3`$ components: $`\left|𝒫_2\right|\left|𝒫_1\right|,\left|𝒫_3\right|`$. Therefore, we can assume that the $`\omega _2`$ field is almost undepleted, $`\left|\mathrm{\Omega }_2\right|const(z)`$.

The propagation equations read for this case:

$`{\displaystyle \frac{_1}{z}}`$ $`=`$ $`i{\displaystyle \frac{\pi Nd_1^2}{\mathrm{}\delta _2}}{\displaystyle \frac{\omega _1}{c}}_1`$
$`+i{\displaystyle \frac{\pi Nd_1d_3\omega _1}{\mathrm{}c}}{\displaystyle \frac{\left|\mathrm{\Omega }_2\right|}{\delta _2\delta _3}}\left(1i{\displaystyle \frac{\gamma }{\delta _3}}\right)e^{i\theta i\mathrm{\Delta }kz}_3,`$
$`{\displaystyle \frac{_3}{z}}`$ $`=`$ $`i{\displaystyle \frac{\pi Nd_3^2}{\mathrm{}}}{\displaystyle \frac{\omega _3}{c}}{\displaystyle \frac{\delta _3i\gamma }{\delta _3^2+\gamma ^2}}_3`$
$`i{\displaystyle \frac{\pi Nd_1d_3\omega _3}{\mathrm{}c}}{\displaystyle \frac{\left|\mathrm{\Omega }_2\right|}{\delta _2\delta _3}}\left(1i{\displaystyle \frac{\gamma }{\delta _3}}\right)e^{i\theta +i\mathrm{\Delta }kz}_1.`$
The solution of this set of propagation equations has exactly the same form as in the maximum-coherence and EIT cases, Eq. (14), with parameters:

$`\kappa `$ $`=`$ $`{\displaystyle \frac{N}{2}}{\displaystyle \frac{|\mathrm{\Omega }_2|\sqrt{\mu _1\mu _3}}{\delta _2\delta _3}},`$ (29)
$`\mathrm{\Gamma }`$ $`=`$ $`{\displaystyle \frac{\gamma }{\delta _3}}\sqrt{{\displaystyle \frac{\mu _1}{\mu _3}}}{\displaystyle \frac{\delta _2}{|\mathrm{\Omega }_2|}},`$ (30)
$`\mathrm{\Delta }k^{}`$ $`=`$ $`\mathrm{\Delta }k+{\displaystyle \frac{N}{2}}\left({\displaystyle \frac{\mu _3}{\delta _3}}{\displaystyle \frac{\mu _1}{\delta _2}}\right).`$ (31)
We see that the conversion length $`l=\kappa ^1`$ is here much larger than both in the maximum coherence, Eq. (22), and in the EIT, Eq. (15), schemes. In fact, the conversion length is also much larger than the (non-phase-matched) coherence length $`L_c=2/\mathrm{\Delta }k^{}`$ as $`\delta _{2,3}/|\mathrm{\Omega }_2|1`$. Therefore, it is not possible in conventional nonlinear optics to get the complete conversion, $`\eta _3\eta _{10}`$, without careful phase matching.

If such a compensation is performed, i.e. if $`\left(\kappa /2\mathrm{\Delta }k^{}\right)^21`$ (by proper choice of detunings $`\delta _2`$ and $`\delta _3`$), optimum conversion occurs for a density-length product

$$Nz|_{\mathrm{opt}}=\frac{\pi }{2}Nl=\pi \frac{\delta _2\delta _3}{\sqrt{\mu _1\mu _3}\left|\mathrm{\Omega }_2\right|}.$$
(32)
At this optimum propagation distance, the relative absorption losses are given by the parameter $`\mathrm{\Gamma }`$, Eq. (30).

Thus, we conclude that in the limit of undepleted drive field(s) both EIT and maximum coherence schemes perform much better than conventional nonlinear optics, regarding the number of atoms $`Nz|_{\mathrm{opt}}`$ necessary for optimum conversion and robustness to phase mismatch. The aim of the present paper is to investigate whether the em energy can be transferred to the generated wave from both pump fields, and whether the attractive features of EIT- and maximum coherence-assisted conversion survive when the drive field is depleted. This requires the solution of the complete nonlinear propagation problem which we treat with the Hamiltonian formalism outlined in the following section.

## III Hamiltonian approach

The resonant interaction of em fields with atomic systems is described by Maxwell’s equations for the fields and a set of master equations for the density matrix of the atoms. The solution of this coupled set is rather difficult and except for some very special cases impossible analytically. In order to derive analytical solutions for the field propagation, approximations are needed that allow to eliminate the atomic degrees of freedom and to express the polarization in terms of field variables. A common approximation, which is not perturbative in the fields, is the adiabatic solution of the density matrix equations. This straightforward approach provides, when applicable, full information about both atoms and fields in the adiabatic limit.

### III.1 General formalism

Instead of the usual explicit scheme of adiabatic elimination which is rather cumbersome, we use here a different, implicit approach mel79 ; kryz  which yields directly effective field equations. This approach is based on the representation of the medium polarization $`P`$ as a partial derivative of the time-averaged free energy density of a dielectric with respect to the electric field $`E`$ LL :

$$P=N\frac{\widehat{H}}{E},$$
(33)
where $`\mathrm{}`$ denotes quantum-mechanical averaging, and $`\widehat{H}`$ is the single-atom interaction Hamiltonian. For the field given by Eq. (1), we can write:

$$P=N\underset{j}{}\frac{\widehat{H}}{_j^{}}\mathrm{exp}(i(\omega _jtk_jz))+c.c.,$$

so that the propagation equation becomes:

$$\frac{_j}{z}=i2\pi \frac{\omega _j}{c}N\frac{\widehat{H}}{_j^{}}.$$
(34)
We here consider light-atom interaction processes that are adiabatic, that is the atomic system can be assumed to follow the evolution of the instantaneous eigenstates. For example, if the atomic system is at some initial time $`t_0`$ in the nondegenerate eigenstate $`|\psi _0(t_0)`$ of the interaction Hamiltonian, i.e.

$$\widehat{H}|\psi _0=\mathrm{}\lambda _0|\psi _0,$$
(35)
which is at $`t=t_0`$ usually identical to the ground state of the atoms, it will remain in this state at all times. Furthermore, we disregard irreversible dissipation processes. As we show later, for the processes we consider here, this is justified even for rather long pulses, i.e., longer than the natural lifetime $`\gamma ^1`$ of the excited state $`|3`$. In this limit one finds

$$\frac{\widehat{H}}{_j^{}}=\psi _0\left|\frac{\widehat{H}}{_j^{}}\right|\psi _0=\mathrm{}\frac{\lambda _0}{_j^{}}.$$

Hence the propagation equation can be written as:

$$\frac{_j}{z}=i2\pi \frac{\mathrm{}\omega _j}{c}N\frac{\lambda _0}{_j^{}}.$$
(36)
For the following it is useful to express the field amplitude $`_j`$ in terms of photon flux $`\eta _j`$, Eq. (12), and phase $`\phi _j`$:

$$_j=\left|_j\right|\mathrm{exp}\{\phi _j\}.$$

Separating the real and imaginary parts, we find from Eq. (36):

$`{\displaystyle \frac{\eta _j}{z}}`$ $`=`$ $`{\displaystyle \frac{^{}}{\phi _j}},`$ (37)
$`{\displaystyle \frac{\phi _j}{z}}`$ $`=`$ $`{\displaystyle \frac{^{}}{\eta _j}}.`$
These equations have the form of Hamilton equations of classical canonical mechanics with action and angle variables $`\eta _j`$, and $`\phi _j`$, ”time” $`z`$, and the Hamiltonian function $`^{}=\frac{1}{2}N\lambda _0`$.

### III.2 Constants of motion for resonant 3-wave mixing

For atomic systems with a closed loop of transitions, the set of canonical equations (37) can be further simplified and in fact under some conditions explicitely integrated. This is the case when the number of coherent fields involved is not too large. To illustrate the procedure, let us consider the eigenvalue equation (35) for the three-level system in Fig. 1. In rotating-wave approximation, the light-atom interaction Hamiltonian is given by:

$`\widehat{H}`$ $`=`$ $`\mathrm{}\left[\delta _2|22\left|+\delta _3\right|33|\right]`$
$`\mathrm{}\mathrm{\Omega }_1|12\left|+\mathrm{}\mathrm{\Omega }_2e^{i\phi }\right|23\left|+\mathrm{}\mathrm{\Omega }_3\right|13|+H.c.,`$
and the eigenvalues are determined by the characteristic equation:

$`\lambda _0\left(\delta _2+\lambda _0\right)\left(\delta _3+\lambda _0\right)\left(\mathrm{\Omega }_1^2+\mathrm{\Omega }_2^2+\mathrm{\Omega }_3^2\right)\lambda _0`$
$`\mathrm{\Omega }_1^2\delta _3\mathrm{\Omega }_3^2\delta _2=2\mathrm{\Omega }_1\mathrm{\Omega }_2\mathrm{\Omega }_3\mathrm{cos}\phi .`$ (39)
Here $`\mathrm{\Omega }_j`$ are the Rabi frequencies, related to the photon flux via the coefficients $`\mu _j`$, Eq. (13), as $`\mathrm{\Omega }_j=\sqrt{\mu _j\eta _j}`$.

The relative phase $`\phi `$ of the em waves is

$$\phi =\phi _1+\phi _2\phi _3\mathrm{\Delta }kz,$$
(40)
which includes the residual phase mismatch $`\mathrm{\Delta }k`$. Also the multiphoton resonance condition

$$\omega _3=\omega _1+\omega _2$$
(41)
has been used.

One can see from Eq. (39) that $`\lambda _0`$ and, hence $`^{}`$, depend on the field phases $`\phi _j`$ only through the relative phase $`\phi `$. Therefore, we have:

$$\frac{^{}}{\phi _1}=\frac{^{}}{\phi _2}=\frac{^{}}{\phi _3}\left(=\frac{^{}}{\phi }\right).$$
(42)
An immediate consequence of this symmetry of $`^{}`$ is the existence of constants of motion. Substituting the above equations (42) into the first line of Eqs. (37) yields the well-known Manley-Rowe relations boyd :

$$\frac{\eta _1}{z}=\frac{\eta _2}{z}=\frac{\eta _3}{z},$$
(43)
which correspond to two independent constants of motion:

$`\eta _1+\eta _3`$ $`=`$ $`\eta _{10}+\eta _{30},`$ (44)
$`\eta _1\eta _2`$ $`=`$ $`\eta _{10}\eta _{20}.`$
Here $`\eta _{j0}=\eta _j(z=0)`$ are the photon flux values at the entrance to the medium. Taking into account the multiphoton resonance condition (41), one finds furthermore that the total intensity of the em fields is conserved: $`I_1+I_2+I_3=const(z)`$. The Manley-Rowe relations and the constants of motion tell us that in the process under consideration, the energy is transferred from the frequency components $`\omega _1`$, $`\omega _2`$ into $`\omega _3`$ and back, with equal rates and without losses, which of course is expected for a dissipationless nonlinear medium.

The relations Eq. (44) enable us to re-write $`\eta _j`$ as:

$`\eta _1(z)`$ $`=`$ $`\eta _{10}J(z),`$
$`\eta _2(z)`$ $`=`$ $`\eta _{20}J(z),`$ (45)
$`\eta _3(z)`$ $`=`$ $`\eta _{30}+J(z).`$
$`J(z)`$ characterizes the amount of energy exchange between the waves and has the initial condition $`J(z=0)=0`$.

Thus the original problem with six amplitude and phase variables can be reduced to two variables $`J`$ and $`\phi `$ by a canonical transformation. This leads to

$`{\displaystyle \frac{J}{z}}`$ $`=`$ $`{\displaystyle \frac{}{\phi }},`$ (46)
$`{\displaystyle \frac{\phi }{z}}`$ $`=`$ $`{\displaystyle \frac{}{J}},`$ (47)
with the new Hamiltonian function

$$=\frac{1}{2}N\lambda _0+\mathrm{\Delta }kJ\frac{1}{2}N\lambda .$$
(48)
As can be seen from Eqs. (48) and (39), $``$ (or $`\lambda `$) does not depend on the coordinate $`z`$ explicitly. Therefore, $``$ (or $`\lambda `$) is a fourth constant of motion expressing the conservation of the energy density of the medium with respect to $`z`$.

### III.3 Solution of the wave-propagation problem

To solve the remaining two equations of motion for $`J(z)`$ and $`\phi (z)`$, the Rabi-frequencies $`\mathrm{\Omega }_j`$ are expressed in terms of $`\eta _{j0}`$ and $`J`$, and the characteristic equation (39) is written in the form

$$G(\lambda ,J)=g(J)\mathrm{cos}\phi .$$
(49)
Differentiating both sides with respect to $`\phi `$ yields

$$\frac{G}{\phi }=\frac{G}{\lambda }\frac{\lambda }{\phi }=g\mathrm{sin}\phi =\pm \sqrt{g^2G^2}.$$

Substituting this relation into Eq. (46), we find:

$$\frac{J}{z}=\pm \frac{N}{2}\frac{\sqrt{g^2G^2}}{G/\lambda }.$$
(50)
The choice of the sign in Eq. (50) depends on the sign of $`\mathrm{sin}\phi `$ at $`z=0`$. Integration of Eq. (50) gives an implicit solution for $`J(z)`$:

$$\pm \frac{N}{2}z=\underset{0}{\overset{J}{}}\frac{G(J^{})}{\lambda }\frac{dJ^{}}{\sqrt{g^2\left(J^{}\right)G^2\left(J^{}\right)}}.$$
(51)
To analytically evaluate the remaining integral, we note that both functions $`g^2G^2`$ and $`G/\lambda `$ are polynomials in $`J`$:

$`g`$ $`=`$ $`2\sqrt{\mu _1\mu _2\mu _3}\sqrt{\left(\eta _{10}J\right)\left(\eta _{20}J\right)\left(\eta _{30}+J\right)},`$
$`G`$ $`=`$ $`G_0+{\displaystyle \underset{m=1}{\overset{3}{}}}A_mJ^m,`$
$`{\displaystyle \frac{G}{\lambda }}`$ $`=`$ $`{\displaystyle \underset{m=0}{\overset{2}{}}}a_mJ^m.`$
Therefore, equation (50) describes a one-dimensional finite motion of a pendulum in an external potential. The solution is in general given by some combination of elliptic functions ell  with parameters determined mainly by the roots $`J_n`$ of the polynomial equation:

$$g^2\left(J\right)G^2\left(J\right)=0.$$
(52)
The allowed range of $`J`$, corresponding to the region of classically allowed motion of the pendulum, lies between $`zero`$ and the smallest positive root $`J_1`$ of the polynomial (52).

The eigenvalue $`\lambda `$ is a constant of motion (cf. Eq. (48)), and can thus be found from the characteristic equation (49) with parameters taken at the medium entrance $`z=0`$:

$$G_0\left(\lambda \right)=g(z=0)\mathrm{cos}\phi (z=0).$$
(53)
Thus, we have reduced the propagation problem to solving two algebraic equations: (53) for $`\lambda `$ and (52) for the roots $`J_n`$. If this can be done explicitly, the Hamiltonian method provides an analytical solution to the propagation problem. But even if an explicit solution is not possible, it considerably simplifies numerical calculations. Apart from the advantage of being convenient from the formal point of view, the Hamiltonian method allows a deeper insight into the nature of the wave propagation process. For example, the method provides a direct access to the stability analysis of the solution by referring to a well-developed theory of Hamiltonian systems cap91 .

To understand the dynamics of the system, in particular interesting quantities such as the conversion efficiency, it is useful to discuss the physical meaning of the coefficients $`A_m`$ and $`a_m`$. Considering the canonical equation (47) for the relative phase:

$$\frac{\phi }{z}=\frac{N}{2}\frac{\lambda }{J}=\frac{N}{2}\frac{G/J}{G/\lambda }=\frac{N}{2}\frac{A_1+2A_2J+3A_3J^2}{a_0+a_1J+a_2J^2},$$
(54)
one recognizes that the $`A_m`$ and $`a_m`$ describe the linear and nonlinear refraction coefficients of the medium. E.g. if $`J`$ is sufficiently small, the first term $`NA_1/2a_0`$ on the right-hand side of Eq. (54) can be identified with the phase mismatch induced by the linear refraction, including both contributions from the three-level interaction and the residual mismatch $`\mathrm{\Delta }k`$.

### III.4 Generation of field with frequency $`\omega _3`$

In the context of the present discussion we are most interested in the generation of the $`\omega _3`$ mode from vacuum $`\eta _{30}=0`$. In this case, the eigenvalue equation (53) reduces to

$`G_0(\lambda )`$ $`=`$ $`\lambda \left(\lambda +\delta _2\right)\left(\lambda +\delta _3\right)\mu _1\eta _{10}\left(\lambda +\delta _3\right)`$ (55)
$`\mu _2\eta _{20}\lambda =0.`$
The nonvanishing coefficients in the expansion of $`G`$ and $`G/\lambda `$ are given by

$`A_1`$ $`=`$ $`q[(\lambda +\delta _2)(\lambda +\delta _3)+\lambda (\lambda +\delta _2)+\lambda (\lambda +\delta _3)`$
$`\mu _1\eta _{10}\mu _2\eta _{20}]`$
$`+\mu _1\left(\lambda +\delta _3\right)+\mu _2\lambda \mu _3\left(\lambda +\delta _2\right),`$
$`A_2`$ $`=`$ $`q^2\left(3\lambda +\delta _2+\delta _3\right)+q\left(\mu _1+\mu _2\mu _3\right),`$ (57)
$`A_3`$ $`=`$ $`q^3,`$ (58)
$`a_0`$ $`=`$ $`3\lambda ^2+2\lambda \left(\delta _2+\delta _3\right)+\delta _2\delta _3\mu _1\eta _{10}\mu _2\eta _{20},`$ (59)
$`a_1`$ $`=`$ $`2q\left(3\lambda +\delta _2+\delta _3\right)+\left(\mu _1+\mu _2\mu _3\right),`$ (60)
$`a_2`$ $`=`$ $`3q^2,`$ (61)
where

$$q=2\mathrm{\Delta }k/N.$$
(62)
With this one finds for the denominator in the integral (51), which determines the allowed values of $`J`$:

$`g^2G^2`$ $`=`$ $`4\mu _1\mu _2\mu _3J\left(\eta _{10}J\right)\left(\eta _{20}J\right)`$ (63)
$`\left(A_1+A_2J+A_3J^2\right)^2J^2=0.`$
The second term in this expression is non-positive, so the smallest positive root of the polynomial is bounded by the minimum of $`\eta _{10}`$ and $`\eta _{20}`$. This reflects the fact that the conversion process stops when the energy of the weaker of the two pump fields is entirely depleted. In order to reach this limit and thus in order to attain maximum conversion efficiency, the second term in (63) should be small, which corresponds to the phase mismatch to be negligible:

$$A_1+A_2J+A_3J^20$$
(64)
In order to see what parameters are required to approximately satisfy this condition, we have to analyze the coefficients $`A_m`$.

It is worthwhile to point out that the behavior of the total phase is described by Eq. (49):

$$\mathrm{cos}\phi \left(z\right)=\frac{G}{g}=\frac{A_1J+A_2J^2+A_3J^3}{2\sqrt{\mu _1\mu _2\mu _3J\left(\eta _{10}J\right)\left(\eta _{20}J\right)}}.$$
(65)
When the total phase mismatch is compensated, $`A_1+A_2J+A_3J^20`$, the phase follows the equation:

$$\mathrm{cos}\phi \left(z\right)=0,$$

that is, the phase is constant and equal to $`+\pi /2`$ or $`\pi /2`$ when all of the waves are present, and jumps by $`\pi `$ to $`\pi /2`$ or $`+\pi /2`$ when one of the wave intensities approaches zero.

As it is seen from Eqs. (57), (58), the terms $`A_2`$, $`A_3`$ responsible for the intensity-dependent refractive index are both proportional to the residual phase mismatch $`\mathrm{\Delta }k`$. One can show that in atomic (molecular) media, where the background refractive index is given by Eq. (25), $`\mathrm{\Delta }k`$ is always sufficiently small so that the leading term in the phase mismatch is $`A_1`$, while $`A_2J`$ and $`A_3J^2`$ are negligibly small. It is also true, that the influence of the intensity-dependent phase mismatch remains insignificant even when the linear refraction is compensated: $`A_1=0`$. Therefore, in what follows, we will disregard the terms $`A_2J`$ and $`A_3J^2`$. In this case, the solution of the propagation equation (51) gives the following dependence of $`J(z)`$ in implicit form:

$`\pm \kappa z+\chi _0=F[\gamma _1\left(J\right),p]+{\displaystyle \frac{a_1J_2}{a_0}}\{F[\gamma _2\left(J\right),p]`$
$`+(1{\displaystyle \frac{J_1}{J_2}})\mathrm{\Pi }[\gamma _2\left(J\right),p^2,p]\},`$ (66)
where $`\chi _0`$ is an integration constant, and $`F(\gamma ,p)`$ and $`\mathrm{\Pi }(\gamma ,r,p)`$ are the elliptic integrals of the first and third kind, respectively ell . $`\kappa `$ is the nonlinear conversion coefficient defined as

$$\kappa =\frac{N}{2}\frac{\sqrt{\mu _1\mu _2\mu _3J_2}}{a_0},$$
(67)
The parameters of the elliptic integrals are:

$`\gamma _1\left(J\right)`$ $`=`$ $`\mathrm{arcsin}\sqrt{{\displaystyle \frac{J}{J_1}}},`$
$`\gamma _2\left(J\right)`$ $`=`$ $`\mathrm{arcsin}\sqrt{{\displaystyle \frac{J_2\left(J_1J\right)}{J_1\left(J_2J\right)}}},`$ (68)
$`p`$ $`=`$ $`\sqrt{{\displaystyle \frac{J_1}{J_2}}}.`$
with $`J_1`$ and $`J_2`$ being the roots of Eq. (63):

$`J_{2,1}`$ $`=`$ $`{\displaystyle \frac{1}{2}}\left(\eta _{10}+\eta _{20}+B_1\right)`$ (69)
$`\pm {\displaystyle \frac{1}{2}}\sqrt{\left(\eta _{10}+\eta _{20}+B_1\right)^24\eta _{10}\eta _{20}},`$
$`B_1`$ $`=`$ $`{\displaystyle \frac{A_1^2}{4\mu _1\mu _2\mu _3}}.`$
In the next section we discuss the solution of the propagation problem for several field-atom interaction configurations resulting in the EIT-assisted, maximum coherence, and conventional nonlinear-optical regimes of the frequency conversion.

## IV Analytical solutions for resonant 3-wave mixing

We assume in our simple 3-level model system that the transitions $`|1|3`$, $`|2|3`$ as well as $`|1|2`$ are allowed. To take into account the much weaker coupling between levels $`|1`$ and $`|2`$ which in reality is a two-photon transition, we assume $`\mu _1\mu _2`$. An analytic solution for the more general 4-wave mixing system can also be obtained within the Hamiltonian formalism to-be-published . The explicit results are however rather lengthy and not very instructive.

### IV.1 EIT-based upconversion

The EIT scheme implies two-photon resonance between the states $`|1`$ and $`|3`$: $`\delta _3=0`$. According to the idea of EIT-assisted nonlinear optics, we suppose here that $`\eta _{20}\eta _{10}`$. Since $`\mu _2`$ $`\mu _1`$, we always have $`\mathrm{\Omega }_2\mathrm{\Omega }_1`$. We allow, for the moment, for spontaneous decay from state $`|3`$ out of the system, but require the initial Rabi frequency $`\mathrm{\Omega }_{20}`$ to be much larger than the decay rate: $`\mathrm{\Omega }_{20}\gamma `$. Under these conditions, the eigenstate that asymptotically connects to the ground state of atoms for $`t\mathrm{}`$ is the state

$$|\psi _0(z=0)\frac{\mathrm{\Omega }_{20}}{\sqrt{\mathrm{\Omega }_{10}^2+\mathrm{\Omega }_{20}^2}}|1\frac{\mathrm{\Omega }_{10}e^{i\phi }}{\sqrt{\mathrm{\Omega }_{10}^2+\mathrm{\Omega }_{20}^2}}|3.$$

corresponding to the complex eigenvalue

$$\lambda i\gamma \frac{\mathrm{\Omega }_{10}^2}{\mathrm{\Omega }_{20}^2}.$$

Since $`\mathrm{\Omega }_{10}\mathrm{\Omega }_{20}`$ one has: $`\left|\lambda \right|\gamma `$. Correspondingly, the probability of spontaneous decay of the state $`|\psi _0`$, which can be defined as Im($`\lambda `$)$`\tau `$ with $`\tau `$ being the characteristic pulse length, remains small even for rather long pulses: $`\tau \tau _0\left(\mathrm{\Omega }_{20}^2/\mathrm{\Omega }_{10}^2\right)\gamma ^1`$ with $`\tau _0\gamma ^1`$. For such pulses, we can safely disregard the spontaneous emission and put $`\lambda 0`$, which means that the corresponding adiabatic state is the usual dark state of EIT. Moreover, since $`\mathrm{\Omega }_{10}`$ $`\mathrm{\Omega }_{20}`$ the eigenstate $`|\psi _0(z=0)`$ is an only slightly disturbed ground state $`|1`$. Therefore, the requirement of adiabaticity of the process is satisfied automatically at the medium entrance, $`z=0`$.

The coefficients $`A_1`$ and $`a_m`$ are given for the regime of EIT by the following expressions:

$`A_1`$ $``$ $`q\mu _2\eta _{20}\mu _3\delta _2,`$ (70)
$`a_0`$ $``$ $`\mu _2\eta _{20},`$ (71)
$`a_1`$ $`=`$ $`2q\delta _2+\left(\mu _1+\mu _2\mu _3\right).`$ (72)
#### IV.1.1 Undepleted EIT-generating field

In the original proposal of EIT-assisted frequency conversion, the $`\omega _2`$ field is assumed to be very strong and undepleted. The latter condition implies $`\eta _{10}\eta _{20}`$. In this situation the solution (66) can be well approximated by

$`J`$ $`=`$ $`{\displaystyle \frac{\eta _{10}}{1+\left(\frac{\mathrm{\Delta }k^{}}{2\kappa _e}\right)^2}}\mathrm{sin}^2\left(\kappa _ez\sqrt{1+\left({\displaystyle \frac{\mathrm{\Delta }k^{}}{2\kappa _e}}\right)^2}\right),`$ (73)
$`\kappa _e`$ $`=`$ $`{\displaystyle \frac{N}{2}}\sqrt{{\displaystyle \frac{\mu _1\mu _3}{\mu _2\eta _{20}}}},`$ (74)
$`\mathrm{\Delta }k^{}`$ $`=`$ $`\mathrm{\Delta }k{\displaystyle \frac{N}{2}}{\displaystyle \frac{\mu _3\delta _2}{\mu _2\eta _{20}}},`$ (75)
which, of course, coincides with that obtained in Sect. II, Eqs. (14) and (15), under the undepleted drive approximation. The influence of the intensity-dependent phase mismatch (terms $`A_2J`$ and $`A_3J^2`$) is negligible in this case, as was discussed above.

One can immediately see from Eqs. (70), (57), (58) that for vanishing residual phase mismatch $`q=0`$ (which can be realized by adding a buffer gas with proper dispersion buf ) and for $`\delta _2=0`$ there is perfect phase matching: $`A_1=A_2=A_3=0`$. Consequently maximum energy transfer into the generated wave $`\omega _3`$ is possible. This applies also for the case when linear refraction is compensated by a detuning $`\delta _2`$:

$$\delta _2=\frac{2}{N}\frac{\mu _2\eta _{20}}{\mu _3}\mathrm{\Delta }k.$$
(76)
For both of these phase matching procedures, the maximum value of $`\eta _3=J`$ achieved at $`z_e=\pi /2\kappa _e`$ is equal to $`\eta _{10}`$. Thus the instantaneous fractional conversion efficiency, defined as

$$ϵ\frac{J_{\mathrm{max}}}{\mathrm{min}(\eta _{10},\eta _{20})}$$
(77)
can become unity. It should be noted, that $`ϵ=1`$ is in general only achieved at a specific instant of time since $`\kappa _e`$ depends on time via $`\eta _{20}\left(tz/c\right)\overline{\eta }_{20}f_{20}\left(tz/c\right)`$ ($`\overline{\eta }_{20}`$ is the amplitude and $`f_{20}\left(tz/c\right)`$ is the temporal envelope of the $`\eta _{20}\left(tz/c\right)`$ pulse). Hence the transfer of energy is complete only for the part of the $`\omega _1`$ pulse which satisfies the condition $`\sqrt{f_{20}\left(tz/c\right)}1`$. A high overall conversion requires a flat temporal profile of the ”coupling” pulse $`\omega _2`$. This is easy to implement, however, since always $`\eta _3=J\eta _2`$ ($`\eta _{20}`$) and $`\eta _1\eta _{20}`$. We have then $`\mathrm{\Omega }_1,\mathrm{\Omega }_3\mathrm{\Omega }_2`$ for the whole medium which means, in particular, that all the atoms throughout the medium are essentially in the ground state. Therefore, the $`\omega _2`$ pulse can be arbitrarily long.

In contrast to the fractional conversion efficiency, Eq. (77), the total conversion efficiency, defined as

$$W(z)\frac{{\displaystyle dt\omega _3\eta _3(z,t)}}{{\displaystyle dt\left[\omega _1\eta _1(z,t)+\omega _2\eta _2(z,t)\right]}}$$
(78)
remains very small because $`\eta _{10}\eta _{20}`$.

#### IV.1.2 Depletion of the pump fields

Conversion with $`\epsilon 1`$ can be achieved, however, also for the case when both pump fields $`\omega _1`$ and $`\omega _2`$ are of comparable intensity. For example, for exact phase matching and $`\eta _{10}=\eta _{20}`$ $`\eta _0`$ (which would correspond, e.g., to the second harmonic generation), the solution Eq. (66) can be written as:

$$\frac{\mu _2}{\mu _3}\kappa _ez=\text{Arth}\left(\sqrt{\frac{J}{\eta _0}}\right)\frac{\left(\mu _1+\mu _2\mu _3\right)}{\mu _3}\sqrt{\frac{J}{\eta _0}},$$
(79)
which demonstrates that $`J`$ monotonically approaches $`\eta _0`$ as $`z`$ increases. The form of this solution for given retarded time is shown in Fig. 2. The monotonic dependence ensures that after sufficiently long propagation length all parts of the pulse $`\eta _{10}=\eta _{20}`$ are converted into the $`\omega _3`$ wave so that not only $`\epsilon 1`$, but also the total energy conversion efficiency $`W`$ reaches unity.

When the phase mismatch is not compensated, the solution for $`\eta _{10}=\eta _{20}`$ $`\eta _0`$ is given by more general expression Eq. (66) with $`B_1=\eta _0\left(\mathrm{\Delta }k^{}/2\kappa _e\right)^2`$ and $`J_{2,1}\eta _0\left(1\pm \mathrm{\Delta }k^{}/2\kappa _e\right)`$. The spatial dependence of the generated field intensity (Fig. 3) differs only slightly from

$$J=\eta _0\left(1\frac{\mathrm{\Delta }k^{}}{2\kappa _e}\right)\text{sn}^2[\kappa _ez\sqrt{1+\frac{\mathrm{\Delta }k^{}}{2\kappa _e}};\sqrt{\frac{J_1}{J_2}}],$$

where sn$`[x;p]`$ is the Jacobi elliptic sine function. The period of intensity oscillations seen in Fig. 3 can be estimated as ell

$$z_e\mathrm{ln}\left(16\kappa _e/\mathrm{\Delta }k^{}\right).$$

Since in EIT regime we have always: $`\mathrm{\Delta }k^{}2\kappa _e`$, very high total conversion efficiency is achieved without phase matching also for $`\eta _{10}\eta _{20}`$ when the drive fields are substantially depleted.

#### IV.1.3 Evolution of the atomic state

In the case of EIT with comparable intensities of the $`\omega _1`$ and $`\omega _2`$ pump fields, the intensity of the $`\omega _3`$ wave increases with $`z`$ and eventually exceeds the one of the $`\omega _1,\omega _2`$ waves. Therefore, the adiabatic state of the atomic system will no longer approximately coincide with the ground state $`|1`$ over the entire medium length at a given retarded time. It will evolve via different superpositions of the bare states $`|1`$ and $`|2`$ following the change of the fields (Fig. 2 and 3) kors . We see that the ”conventional” EIT regime (one strong and one weak field, and thus one highly populated and one slightly populated state) does not hold over the full conversion cycle. We should stress, however, that the atoms remain in the adiabatic state corresponding to $`\lambda =0`$, i.e., in the dark state. Therefore, all the features of the EIT-assisted conversion process such as vanishing linear absorption and refraction as well as resonantly enhanced nonlinearity are present even when the pump field is depleted.

When most of the input energy is transferred to the $`\omega _3`$ pulse, i.e. for larger propagation distances into the medium, the dark state $`|\psi _0`$ approaches the bare state $`|2`$

$$|\psi _0|2,$$

which does not coincide with the initial atomic state (i.e. the ground state $`|1`$). Thus we encounter two problems: First, since all atoms are in the ground state before the arrival of the pulses, there must be an adiabatic transfer in the initial phase from $`|1`$ to $`|\psi _0`$. This requires a specific time-order of the pulses. In particular $`\mathrm{\Omega }_2`$ should arrive after the other pulses. This time ordering is however not reflected in our solutions. Second, after the interaction with the pulses, there is energy left in the atomic system. This is in apparent contradiction to the fact that full conversion of photon energy has taken place and no energy got lost. It should be noted though that the size of the effect is rather small in the considered limit of a large initial number of photons. This contradictory behavior is a result of the limited validity of the assumptions made. We have here completely neglected non-adiabatic corrections, which are small on the level of individual atoms, but add up in the field evolution when integrated over the whole sample. The most important effect ignored by this is the group velocity delay of the weak fields.

Although the group delay cannot be treated within the current approach, it may resolve the problems. In the first part of the medium, i.e. for small $`Nz`$ the generated field is still small. Thus the group velocities of the pulses $`\mathrm{\Omega }_1`$ and $`\mathrm{\Omega }_3`$ should be smaller than that of the strong drive field $`\mathrm{\Omega }_2`$. Then the leading edge of the $`\mathrm{\Omega }_2`$-pulse will always propagate ahead of the other pulses, guaranteeing that the adiabatic state $`|\psi _0`$ asymptotically matches with the ground state at early times for all values of $`z`$. For larger propagation distances into the medium and for times in the central part of the pulses a substantial portion of the energy is transferred to the field $`\mathrm{\Omega }_3`$. Now the situation is reversed. $`\mathrm{\Omega }_3`$ is strong and $`\mathrm{\Omega }_2`$ is weak. Thus the pulse $`\mathrm{\Omega }_2`$ will have a smaller group velocity and should lag behind at the trailing edge of the pulses. Consequently also for large times the adiabatic eigenstate $`|\psi _0`$ approaches asymptotically the ground state $`|1`$.

A full quantitative account of the leading order non-adiabatic corrections requires however a reformulation of the Hamiltonian approach. This is beyond the scope of the present work and will be presented in a future publication.

### IV.2 Maximum coherence case

The mechanism of the nonlinear optics with maximum coherence is realized when the detuning $`\delta _3`$ is much larger than the other parameters including all Rabi frequencies and $`\delta _2`$. In this case the coefficients $`A_1`$ and $`a_m`$ are as follows:

$`A_1`$ $``$ $`q\left[\left(2\lambda +\delta _2\right)\delta _3\mu _1\eta _{10}\mu _2\eta _{20}\right]`$
$`+\mu _1\delta _3+\mu _2\lambda \mu _3\left(\lambda +\delta _2\right),`$
$`a_0`$ $``$ $`\left(2\lambda +\delta _2\right)\delta _3\mu _1\eta _{10}\mu _2\eta _{20},`$ (81)
$`a_1`$ $`=`$ $`2q\delta _3+\left(\mu _1+\mu _2\mu _3\right).`$ (82)
#### IV.2.1 Preparation of maximum atomic coherence

The energy eigenvalue for large $`\delta _3`$ is given by:

$$\lambda =\frac{1}{2}\left(\delta _2\frac{\mathrm{\Omega }_{20}^2}{\stackrel{~}{\delta }_3}\right)+\frac{1}{2}\sqrt{\left(\delta _2\frac{\mathrm{\Omega }_{20}^2}{\stackrel{~}{\delta }_3}\right)^2+4\mathrm{\Omega }_{10}^2},$$
(83)
where $`\stackrel{~}{\delta }_3=\delta _3+i\gamma `$. The amplitudes of the adiabatic state corresponding to this eigenvalue at the entrance to the medium, $`z=0,`$ are:

$`c_1`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_{10}}{\sqrt{\lambda ^2+\mathrm{\Omega }_{10}^2}}},`$ (84)
$`c_2`$ $`=`$ $`{\displaystyle \frac{\lambda }{\sqrt{\lambda ^2+\mathrm{\Omega }_{10}^2}}},`$ (85)
$`c_3`$ $``$ $`c_1,c_2.`$
Similar to the EIT case, the probability of spontaneous decay of the state $`|\psi _0`$ is small: Im($`\lambda `$)$`\tau 1`$ for large detuning assumed here, $`\delta _3\gamma `$, even for pulses that are longer than $`\gamma ^1`$: $`\tau \left(\delta _3^2/\mathrm{\Omega }_{20}^2\right)\gamma ^1`$. Again, we will consider only such pulses and neglect spontaneous emission.

The situation of the maximum coherence, $`\left|c_1\right|=\left|c_2\right|=1/\sqrt{2}`$, takes place when the Rabi frequency exceeds the detuning on transition $`|1|2`$ including the ac Stark shift induced by the $`\omega _2`$ field: $`\mathrm{\Omega }_{10}\left|\delta _2\mathrm{\Omega }_{20}^2/\delta _3\right|`$. In this case $`\lambda \mathrm{\Omega }_{10}`$ and the atomic state at the medium entrance is the superposition: $`|\psi _0(z=0)=\left(|1|2\right)/\sqrt{2}`$. However, in order for the atoms to get there from the ground state, one first has to have the inverse situation $`\delta _2\mathrm{\Omega }_{10}`$, and then adiabatically decrease $`\delta _2`$, simultaneously increasing $`\mathrm{\Omega }_{10}`$. This can be accomplished by, e.g., Stark-chirped rapid adiabatic passage scrap . We will not include this process explicitly in the consideration, but assume that when the $`\omega _2`$ pulse arrives, the condition $`\mathrm{\Omega }_{10}\delta _2`$ is already satisfied. As a consequence, the energy taken from the leading edge of the $`\omega _1`$ pulse for the superposition preparation, is not taken into account. However, if the number of photons in the $`\omega _1`$ pulse is much larger than the total number of atoms along the field propagation path, these preparation energy losses ($`\mathrm{}\omega _1/2`$ per atom) can be neglected.

#### IV.2.2 Undepleted coherence-generating field

When a strong, undepleted $`\omega _1`$ field is supposed: $`\eta _{20}\eta _{10}`$ (implying also undepleted coherence on $`|1|2`$ transition), the generated field intensity experiences sinusoidal oscillations with respect to the propagation length:

$`J`$ $`=`$ $`{\displaystyle \frac{\eta _{20}}{1+\left(\frac{\mathrm{\Delta }k^{}}{2\kappa _m}\right)^2}}\mathrm{sin}^2\left(\kappa _mz\sqrt{1+\left({\displaystyle \frac{\mathrm{\Delta }k^{}}{2\kappa _m}}\right)^2}\right),`$ (86)
$`\kappa _m`$ $`=`$ $`{\displaystyle \frac{N}{4}}{\displaystyle \frac{\sqrt{\mu _2\mu _3}}{\delta _3}},`$ (87)
$`\mathrm{\Delta }k^{}`$ $`=`$ $`\mathrm{\Delta }k{\displaystyle \frac{N}{4}}\left(\sqrt{{\displaystyle \frac{\mu _1}{\eta _{10}}}}+{\displaystyle \frac{\left(\mu _2\mu _3\right)}{\delta _3}}\right),`$ (88)
in correspondence with the analysis of Sec. II, Eqs. (14), (22) and (24), and assuming $`\left|c_1\right|^2=\left|c_2\right|^2=\rho _{12}=1/2`$.

Since $`\kappa _m`$ is of the order of $`\mathrm{\Delta }k^{}`$, substantial transfer of energy from the $`\omega _2`$ field into the $`\omega _3`$ field occurs even without compensation of the phase mismatch. If one can manage to make $`\mathrm{\Delta }k^{}`$ small: $`\mathrm{\Delta }k^{}\kappa _m`$ then the best possible regime for conversion can be attained: not only complete transfer for the pulse maximum is realized: $`J_1J_{max}=\eta _{20}`$, but also the conversion length $`l=\kappa _m^1`$ does not depend on time, and hence, all parts of the $`\omega _2`$ pulse are homogeneously converted into the $`\omega _3`$ wave.

There are several possibilities to reach this regime. First, one may set $`\mathrm{\Delta }k`$ to zero by use of the buffer gas, and choose the input laser parameters such that:

$$\delta _3=\frac{\left(\mu _2\mu _3\right)}{\mu _1}\sqrt{\mu _1\eta _{10}}.$$
(89)
This condition can be satisfied only for the time interval when $`\sqrt{f_{10}\left(tz/c\right)}1`$. That is, a flat temporal profile of the $`\omega _1`$ pulse is required. Since this is not always possible, another method can be used. One may simply increase the intensity $`\eta _{10}`$ so that the refraction contribution of the $`|1|2`$ transition becomes small: $`\sqrt{\mu _1/\eta _{10}}\left(\mu _2\mu _3\right)/\delta _3`$, and choose the detuning $`\delta _3`$ as

$$\delta _3=\frac{\left(\mu _2\mu _3\right)}{2q}.$$
(90)
Since in this regime $`\eta _3=J\eta _{10}`$, we have at any propagation distance: $`\mathrm{\Omega }_1\mathrm{\Omega }_2^2/\delta _3`$, $`\mathrm{\Omega }_3^2/\delta _3`$. Therefore, the atoms remain in a superposition $`|\psi _0=\left(|1|2\right)/\sqrt{2}`$ throughout the medium.

It should be noted that although the instantaneous conversion efficiency $`ϵ`$ can reach unity, the total energy conversion efficiency is always small, $`W1`$, because $`J_1\eta _{20}\eta _{10}`$.

#### IV.2.3 Depletion of the pump fields

The situation is completely different for comparable intensities of the two pump waves: $`\eta _{20}\eta _{10}`$.

For the maximum coherence regime, $`\left|c_1\right|=\left|c_2\right|=1/\sqrt{2}`$, to be attained, the condition $`\mathrm{\Omega }_1\mathrm{\Omega }_2^2/\delta _3`$ must be satisfied (see above), which reduces to $`\sqrt{\mu _2\eta _{10}}\delta _3\sqrt{\mu _1/\mu _2}`$ at $`\eta _{20}\eta _{10}`$. That is, the intensity of the pump pulses cannot be large, and the refraction contribution of the $`|1|2`$ transition ($`\sqrt{\mu _1/\eta _{10}}`$) is not small, so that $`\mathrm{\Delta }k^{}\left(N/4\right)\sqrt{\mu _1/\eta _{10}}\kappa _m`$. Thus, the ”exact maximum coherence” regime fails when the drive field is depleted.

However, the phase matching can still be performed for $`\eta _{20}\eta _{10}`$ if the requirement for $`\left|c_1\right|=\left|c_2\right|=1/\sqrt{2}`$ is lifted. One of the possibilities is to cancel the residual refraction by addition of buffer gas: $`\mathrm{\Delta }k=0`$ (then $`A_2=A_3=0`$), and to choose the interaction parameters such that $`A_10`$. The latter condition can be satisfied for specific relations between the detuning $`\delta _2`$ and/or $`\delta _3`$, and the input intensities $`\eta _{10},\eta _{20}`$. For example, for $`\eta _{10}=\eta _{20}`$ $`\eta _0`$ and when $`\mu _2<\mu _3`$, one may choose the detunings $`\delta _2=0`$ and $`\delta _3`$ such that

$$\mu _3\eta _0=\frac{\mu _1}{\left(\mu _3\mu _2\right)}\delta _3^2.$$
(91)
Taking into account condition (91), the eigenenergy $`\lambda `$ is reduced in this regime to:

$$\lambda =\sqrt{\mu _1\eta _0}\sqrt{\frac{\mu _3}{\left(\mu _3\mu _2\right)}}=\mathrm{\Omega }_{10}\zeta ,$$
(92)
and the corresponding adiabatic state at the entrance to the medium is:

$$|\psi _0(z=0)=\frac{1}{\sqrt{1+\zeta ^2}}\left(|1\zeta |2\right).$$
(93)
Thus, the atoms are prepared not with maximum coherence, $`\rho _{12}=1/2`$, but in a specific superposition with $`\rho _{12}=\zeta /\left(1+\zeta ^2\right)`$ which is also not small.

The propagation problem solution in this case resembles that of the EIT regime, Eq. (79):

$`\kappa _m{\displaystyle \frac{2}{\zeta }}z`$ $`=`$ $`\text{Arth}\left(\sqrt{{\displaystyle \frac{J}{\eta _0}}}\right){\displaystyle \frac{\mu _1+\mu _2\mu _3}{\mu _3}}\sqrt{{\displaystyle \frac{J}{\eta _0}}},`$ (94)
$`\zeta `$ $`=`$ $`\sqrt{{\displaystyle \frac{\mu _3}{\left(\mu _3\mu _2\right)}}},`$ (95)
which is demonstrated in Fig. 4. The conversion coefficient differs from that of the undepleted coherence case $`\kappa _m`$, Eq. (87), only by a numerical factor $`2\sqrt{\left(\mu _3\mu _2\right)/\mu _3}`$.

As we can see, although the total conversion efficiency may approach unity, the robustness of the maximum coherence scheme to the phase mismatch is lost. One has to fulfill the phase matching conditions (like (91)) with sufficient accuracy to get a large conversion. A considerable transfer of energy into the generated wave can be expected when the envelope of the pump pulse satisfies the condition:

$$1\sqrt{f_{10}\left(tz/c\right)}\sqrt{\frac{4\mu _2}{\left(\mu _3\mu _2\right)}},$$

and the detuning $`\delta _3=\delta _3^0+\delta _3^{}`$ differs from the value $`\delta _3^0`$, given by condition (91), by not more than

$$\delta _3^{}\sqrt{\frac{\mu _2}{\left(\mu _3\mu _2\right)}}\delta _3^0.$$

Both of these conditions require that the values of the transition coupling constants, $`\mu _2`$ and $`\mu _3`$, be close.

Similar to the EIT regime, the adiabatic superposition does not coincide with the state $`|\psi _0(z=0)`$, Eq. (93), over the entire medium, but will evolve in the course of propagation, following the change of the fields (Fig. 4). For large density-length products $`Nz`$ when $`\mathrm{\Omega }_1\mathrm{\Omega }_3^2/\delta _3`$, the atomic state tends to the ground state: $`|\psi _0|1`$. Thus, ”the maximum coherence” is not maintained throughout the light propagation path, although it is still sufficiently large for most part of the medium. One can see from Fig. 4 that as the coherence gets smaller, the conversion slows down, and for very large $`Nz`$ (hence, for small atomic coherence), the generated intensity only slowly approaches its maximum.

Here again we encounter an apparent contradiction related to the limited validity of the adiabatic approximation. The atoms do not return to the initial state despite the overall energy conservation. Now the preparation energy for the atomic coherence is extracted as well. Under the conditions discussed here, i.e. large photon number as compared to number of atoms, this is however a small effect. A resolution of this problem should be found when non-adiabatic corrections are taken into account, which will be the subject of further investigations.

### IV.3 Conventional nonlinear optics (weak excitation)

Finally, we consider the regime corresponding to conventional nonlinear optics. This regime takes place at weak excitation when both detunings $`\delta _2`$ and $`\delta _3`$ are much larger than all Rabi frequencies. Then we have $`\lambda \mathrm{\Omega }_{10}^2/\delta _2`$ and $`|\psi _0|1`$ for all atoms in the medium.

The coefficients $`A_1`$ and $`a_m`$ do not depend on laser intensities in this case:

$`A_1`$ $``$ $`q\delta _2\delta _3+\mu _1\delta _3\mu _3\delta _2,`$ (96)
$`a_0`$ $``$ $`\delta _2\delta _3,`$ (97)
$`a_1`$ $`=`$ $`2q\left(\delta _2+\delta _3\right)+\left(\mu _1+\mu _2\mu _3\right).`$ (98)
Since $`a_1\mathrm{min}(\eta _{10},\eta _{20})a_0`$, the solution Eq. (66) can be well approximated by

$`J`$ $`=`$ $`J_1\text{sn}^2[\kappa _nz;\sqrt{J_1/J_2}],`$ (99)
$`\kappa _n`$ $`=`$ $`{\displaystyle \frac{N}{2}}{\displaystyle \frac{\sqrt{\mu _1\mu _2\mu _3J_2}}{\delta _2\delta _3}},`$ (100)
with $`J_{2,1}`$ determined from Eqs. (69), (96). This formula is valid for any relation between $`\eta _{10}`$ and $`\eta _{20}`$.

When the phase mismatch is compensated: $`A_10`$, which is made by proper tuning:

$$q=\frac{\mu _3}{\delta _3}\frac{\mu _1}{\delta _2},$$
(101)
the roots $`J_{2,1}`$ are: $`J_1=\mathrm{min}(\eta _{10},\eta _{20})`$, $`J_2=\mathrm{max}(\eta _{10},\eta _{20})`$. Therefore, the optimum conversion can be realized also in the case of the off-resonant nonlinear optics. In particular, for $`\eta _{10}\eta _{20}`$ the complete transfer of energy to the generated wave occurs:

$$J=\eta _0\text{sn}^2\left[\kappa _nz;p1\right]\eta _0\mathrm{tanh}^2\left(\kappa _nz\right),$$

leading to perfect total conversion efficiency, $`W1`$. However, the nonlinear conversion coefficient $`\kappa _n`$ is much smaller in this case than in the EIT and maximum coherence regimes ($`\kappa _e`$ and $`\kappa _m`$, Eqs. (74) and (87), respectively). Therefore, the energy transfer is accomplished for much larger density-length products $`Nz`$.

At last, we note that if the phase mismatch is not compensated, we have $`B_1\left(\eta _{10}+\eta _{20}\right)`$ and the solution is reduced to traditional formula of nonlinear optics boyd :

$$J=N^2\frac{\mu _1\mu _2\mu _3\eta _{10}\eta _{20}}{4\delta _2^2\delta _3^2}\frac{\mathrm{sin}^2\left(\mathrm{\Delta }k^{}z/2\right)}{\left(\mathrm{\Delta }k^{}/2\right)^2},$$
(102)
with the total phase mismatch $`\mathrm{\Delta }k^{}=\mathrm{\Delta }kN\mu _1/2\delta _2+N\mu _3/2\delta _3`$.

## V Summary

Resonant optical processes based on atomic coherence effects such as EIT or maximum coherence allow for a maximum nonlinear conversion of photons within a much smaller density-length product than possible in schemes of conventional off-resonant nonlinear optics. Since degrading mechanisms such as phase-mismatch and absorption scale with the same density length product, EIT or maximum coherence can thus substantially reduce the requirements for efficient nonlinear optics. As a measure for the efficiency of using atoms for nonlinear conversion processes, one can introduce the ratio of the number of converted photons $`n𝒜\tau _j\overline{\eta }_{j0}`$, to the number of atoms $`N_{at}=N𝒜lN𝒜/\kappa `$ needed ($`𝒜`$ is a cross-sectional area and $`\tau _j`$ is the duration of the pulse). This figure of merit $`n/N_{at}`$ is largest for the EIT scheme: $`n/N_{at}=\tau _1\mathrm{\Omega }_{10}`$, considerably smaller for the maximum coherence method: $`n/N_{at}=\tau _2\mathrm{\Omega }_{20}\left(\mathrm{\Omega }_{20}/\delta _3\right)`$ (with $`\mathrm{\Omega }_{20}/\delta _31`$), and is very small for conventional nonlinear optics: $`n/N_{at}=\tau _2\mathrm{\Omega }_{20}\left(\mathrm{\Omega }_{10}\mathrm{\Omega }_{20}/\delta _3\delta _2\right)`$ (with $`\mathrm{\Omega }_{20}/\delta _31`$ and $`\mathrm{\Omega }_{10}/\delta _21`$).

In previous theoretical studies of EIT- and maximum-coherence based nonlinear optics, undepleted drive fields or a constant coherence where assumed. If one takes into account the resources to maintain the drive field or the constant coherence, the overall efficiency of the processes is in this limit tiny. We have shown in the present paper that when this restriction is lifted and coherence- or transparency maintaining fields with comparable intensities to the pump fields are considered, it is possible to achieve also a maximum overall conversion. To study the conditions for this, we have derived analytical solutions for the pulse interaction in the adiabatic limit using an approach that maps the propagation problem to that of a nonlinear pendulum. Under certain conditions this problem could be explicitly integrated allowing for a simple discussion of the physical processes involved.

We have found that when the coherence- or transparency maintaining fields are depleted, the atomic state does not remain constant but evolves along the propagation path following the change of the fields. Therefore, the conversion process cannot be associated with maximum coherence or EIT in traditional sense alone. Nevertheless, the main features of EIT, - reduced linear absorption and refraction, and enhanced nonlinearity are still present in the latter mechanism. Although in the ”maximum coherence” mechanism the robustness to the phase mismatch is lost, the nonlinear conversion coefficient remains much larger than in conventional nonlinear optics. Thus, for both mechanisms, a complete conversion can be achieved within a small density-length product.

We have also encountered several limitations of the strong adiabatic assumption used in the Hamiltonian approach. An extension of the approach to take into account non-adiabatic corrections and thus such important effects as group delay is currently under investigation and corresponding results will be presented elsewhere.

The work of E.A. K. was supported by Alexander von Humboldt Foundation. We would like to thank R. Unanyan for bringing to our attention the Hamiltonian formalism in nonlinear optics and the relevant publications mel79 ; kryz , and him and K. Bergmann for many useful discussions. E.A. K. would also like to thank K. Bergmann for the hospitality and his continuous support.