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# I Introduction

## I Introduction

There is an urgent need for the rapid assay of chemical and biological unknowns, such as bioaerosols. Substantial progress toward this goal has been made over the past decade. Techniques such as fluorescence spectroscopy Cheng ; Seaver99 , and UV resonant Raman spectroscopy Manoharan90 ; Nelson91 ; Ghiamati ; Manoharan93  have been successfully applied to the identification of biopolymers, bacteria, and bioaerosols.

At present field devices are being engineered Seaver99  which will involve an optical preselection stage based on, e.g., fluorescence radiation as in Fig. 1. If the fluorescence measurement does not give the proper signature then that particle is ignored. Most of the time the particle will be an uninteresting dust particle; however, when a signature match is recorded, then the particle is selected for special biological assay, see Fig. 1b. The relatively simple fluorescence stage can very quickly sort out some of the uninteresting particles while the more time consuming bio-tests will only be used for the “suspects”.

The good news about the resonance fluorescence technique is that it is fast and simple. The bad news is that while it can tell the difference between dust and bacterial spores, it can not differentiate between spores and many other organic bioaerosols, see Fig. 1c.

However, in spite of the encouraging success of the above mentioned studies, there is still interest in other approaches to, and tools for, the rapid identification of chemical and biological substances. To quote from a recent study Terror :

> “Current \[fluorescence based\] prototypes are a large improvement over earlier stand-off systems, but they cannot yet consistently identify specific organisms because of the similarity of their emission spectra. Advanced signal processing techniques may improve identification.”

Resonant Raman spectra hold promise for being spore specific as indicated in Fig. 2b. This is the good news, the bad news is that the Raman signal is weak and it takes several minutes to collect the data of Fig. 2b. Since the through-put in a set-up such as that of Fig. 1b is large, the optical interrogation per particle must be essentially instantaneous.

The question then is: Can we increase the resonant Raman signal strength and thereby reduce the interrogation time per particle? If so, then the technique may also be useful in various detection scenarios.

The answer to the question of the proceeding paragraph is a qualified “yes.” We can enhance the Raman signal by increasing the coherent molecular oscillation amplitude $`R_0`$ indicated in 2c. In essence this means maximizing the quantum coherence between vibrational states $`|b`$ and $`|c`$ of 2a.

Our point of view derives from research in the fields of laser physics and quantum optics which have concentrated on the utilization and maximization of quantum coherence. The essence of these studies is the observation that an ensemble of atoms or molecules in a coherent superposition of states represents, in a real sense, a new state of matter aptly called “phaseonium” ScullyZubairy .

In particular, we note that matter in thermodynamic equilibrium has no phase coherence between the electrons in the molecules making up the ensemble. This is discussed in detail in Section III. When a coherent superposition of quantum states is involved, things are very different and based on these observations, many interesting and counterintuitive notions are now a laboratory reality. These include lasing without inversion (LWI) LWI , electromagnetically induced transparency (EIT) EIT , light having ultra slow group velocities on the order of 10 meters/sec slowlight , and the generation of ultra short pulses of light based on phased molecular states sokolov .

Another emerging technology central to the present paper is the exciting progress in the area of femtosecond quantum control of molecular dynamics originally suggested by Judson and Rabitz Rabitz . This is described and reviewed in the articles by Kosloff et al. Kosloff , Warren, Rabitz and Dahleh Warren93 , Gordon and Rice Gordon97 , Zare Zare , Rabitz, de-Vivie-Riedle, Motzkus and Kompa Rabitz00 , and Brixner, Damrauer and Gerber Brixner01 . Other related work on quantum coherent control includes: The quantum interference approach of Brumer and Shapiro Brumer86 ; the time-domain (pump-dump) technique proposed by Tannor, Kosloff and Rice Tannor86 ; the stimulated Raman Adiabatic Passage (STIRAP) approach of Bergmann and co-workers Bergmann98  to generate a train of coherent laser pulses. The preceding studies teach us how to produce pulses having arbitrary controllable amplitude and frequency time dependence. Indeed the ability to sculpt pulses by the femtosecond pulse shaper provides an important new tool for all of optics, see the pioneering works by Heritage, Weiner, and Thurston Heritage , Weiner, Heritage, and Kirschner Weiner88 , Wefers and Nelson Wefers95  and Weiner Weiner00 .

An important aspect of the learning algorithm approach is that knowledge of the molecular potential energy surfaces and matrix elements between surfaces are not needed. Precise taxonomic marker frequencies may not be known a priori; however, by using a pulse shaper coupled with a feedback system, complex spectra can be revealed.

Thus, we now have techniques at hand for controlling trains of phase coherent femtosecond pulses so as to maximize molecular coherence. This allows us to increase the Raman signal while decreasing the undesirable fluorescence background. This has much in common with the CARS spectroscopy Demtroder  of Fig. 3, but with essential differences as we now discuss.

The presently envisioned improvement over ordinary CARS is based on enhancing the ground state molecular coherence. However, we note that molecules involving a large number of degrees of freedom will quickly dissipate the molecular coherence amongst these degrees of freedom. This is a well known difficulty and is addressed in the present work from several perspectives. First of all, when working with ultra short pulses, we have the ability to generate the coherence on a time scale which is small compared with the molecular relaxation time. Furthermore, we are able to tailor the pulse sequence in such a way as to mitigate, and overcome key limitations in the application of conventional CARS to trace contaminants. The key point is that we are trying to induce maximal ground state coherence, as opposed to the usual situation within conventional CARS where the ground state coherence is not a maximum as is shown later in this paper. With FAST CARS (Femtosecond Adaptive Spectroscopic Techniques applied to Coherent Anti-Stokes Raman Spectroscopy) we can prepare the coherence between two vibrational states of a molecule with one set of laser pulses; and use higher frequency visible or ultra-violet to probe this coherence in a coherent Raman configuration. This will allow us to capitalize on the fact that maximally coherent Raman spectroscopy is orders of magnitude more sensitive than incoherent Raman spectroscopy.

Having stated our goals and our approach toward attaining these goals, we emphasize that the present paper represents essentially an engineering endeavor. We propose to draw heavily on the ongoing work in quantum coherence and quantum control as mentioned earlier.

For example, the careful experiments and analysis of the Würzburg group on the generation and probing of ground state coherence in porphyrin molecules Heid01  by femtosecond-CARS (fs-CARS) are very germane to our considerations. However, ground state coherence is not maximized in these experiments.

In another set of beautiful experiments Chen00  they investigate the selective excitation of polymers of diacetylene via fs-CARS. They control the timing, phase and frequency (chirp) content of their preparation pulses. In these experiments it was necessary to focus attention on the evolution of the excited state molecular dynamics. We hope to avoid this complication as is explained later.

Perhaps closest to our approach is the recent joint work of the Garching Max-Planck and Würzburg groups Zeidler02 . Their paper entitled “Optimal control of ground-state dynamics in polymers” is a prime example of a FAST CARS experiment. However they concentrate on producing highly excited states of the “vibrational motion of a certain bond”. The application of their technique to the production of maximum coherence between states $`|b`$ and $`|c`$ of Fig. 2a in a specific vibrational mode of their molecule would be of great interest to us and is underway.

Finally we wish to draw the reader’s attention to the useful collection of articles in a recent special issue of the “Journal of Raman Spectroscopy” dedicated to fs-CARS JRS00 . Likewise the recent work of Silberberg and coworkers Silberberg  in which they show that it is possible to excite one of two nearby Raman levels, even when they are well within the broad fs pulse spectrum is another excellent example of the power of the FAST CARS technique.

To summarize: the present work focuses on utilization of a maximally phase coherent ensemble of molecules, i.e. molecular phaseonium, to enhance Raman signatures. This will be accomplished via the careful tailoring of a coherent pulse designed to prepare the molecule with maximal ground state coherence. Such a pulse is a sort of “melody” designed to prepare a particular molecule. Once we know this molecular melody, we can use it to set that particular molecule in motion and this oscillatory motion is then detected by another pulse; this is the FAST CARS protocol depicted in Figs 3c and 15b.

In order to establish the viability and credibility of this program, the material covered in the present paper is presented in some detail. It is hoped that scientists who are experts in one phase of the subject, e.g., molecular biology but not with subtleties of modern laser spectroscopy can read the paper without undue appeal to the literature or complicated mathematical developments. On the other hand, some basic facts of life, endosporewise, are important. Hence, a short overview of some aspects of Raman spectroscopy as applied to macromolecules and especially to biological spores is presented.

In Section II, the status of Raman spectroscopy applied to biological spores is reviewed. In Section III, we compare various types of Raman spectroscopy with an eye to the recent successful applications of quantum coherence in laser physics and quantum optics. Section IV presents several experimental schemes for applying these considerations to the rapid identification of macromolecules, in general, and biological spores, in particular. Finally in Section V we propose several scenarios in which FAST CARS could be useful in the rapid detection of bacterial spores. Where appropriate, mathematical details are included in Appendices and comparison between the various types of Raman spectroscopic techniques are discussed with special emphasis on overall sensitivity. As stated earlier, the present paper is an engineering science analysis of a promising approach to the problem of bacterial spore detection. This is not a review paper. If the reader feels that we have missed or misrepresented her research, we would be happy to learn how to use it to improve our design and detection strategy. Indeed, we view this paper as providing a point of departure, and will be pleased if it provokes discussion and debate. If the reader is not provoked we apologize. It is very difficult to annoy everybody in a single paper.

## II Pico-Review of Raman spectroscopy applied to bacterial spores

The bacterial spore is an amazing life form. Spores thousands of years old have been found to be viable. One textbook Black  reports that “endospores trapped in amber for 25 million years germinate when placed in nutrient media.”

A key to this incredible longevity is the presence of dipicolinic acid (DPA) and its salt calcium dipicolinate in the living core which contains the DNA, RNA, and protein as shown in Fig. 4.

A major role of the calcium DPA complex seems to be the removal of water, as per the following quote Talaro  : “The exact role of these \[DNA\] chemicals is not yet clear. We know, for instance, that heat destroys cells by inactivating proteins and DNA and that this process requires a certain amount of water. Since the deposition of calcium dipicolinate in the spore removes water . . . it will be less vulnerable to heat.”

Hence, one of the major components of bacterial spores is dipicolinic acid (DPA) and its ion as depicted in Fig. 5. Calcium dipicolinate can contribute up to $`17\%`$ of the dry weight of the spores. A definitive demonstration Manoharan90  of this conjecture was made by comparing the 242 nm excitation spectra of calcium dipicolinate with spore suspensions of Bacillus megaterium and Bacillus cereus. From Fig. 6, it is seen that good matches were noted for the 1017, 1396, 1446, and 1607 cm<sup>-1</sup> peaks of the calcium dipicolinate.

As has been emphasized by W. Nelson and coworkers Manoharan90 ; Nelson91 ; Ghiamati ; Manoharan93 , the presence of DPA and its calcium salt gives us a ready made marker for endospores. As has been mentioned earlier and as will be further discussed later, this is the key to Raman fingerprinting of the spore.

We note however that fluorescence spectroscopy was one of the first methods used for detection of bacterial taxonomic markers and is still used for detection where high specificity is not required. This technique is an important addition to the “tool kit” of scientists and engineers working in this area.

A possible FAST CARS protocol is as follows: First we obtain size and fluorescence information. If this is consistent with the presence of a particular bacterial spore we could then automatically perform a FAST CARS analysis sensitive to DPA so as to further narrow the number of suspects.

It is important to note that just as resonant Raman is some $`10^6`$ times more sensitive than non-resonant, coherent Raman yields a much stronger signal than ordinary incoherent Raman spectroscopy. This makes it possible to collect the Raman spectra much more rapidly via FAST CARS and this is very important in the ultimate scheme of things.

To summarize: we will generate quantum coherence in macromolecules by working with the now available femtosecond pulse trains in which there exists phase coherence between the individual pulses. In this way, one can enhance coherent Raman signatures. The utilization of “molecular music” to generate maximal phase coherence holds promise for the identification and characterization of macro and bio-molecules.

## III Comparison of different types of Raman spectroscopy

Raman scattering is an inelastic scattering of electromagnetic fields off vibrating molecules. The origin of Raman scattering dates back to a theoretical paper in Naturwissenschaften by A. Smekal in 1923 entitled (translated) “The quantum theory of dispersion” Smekal . It was followed by another paper in a 1923 Physical Review (by A. Compton) entitled “A quantum theory of the scattering of X-rays by light elements” Compton . Some historians feel that these two papers gave C.V. Raman the idea for the experiments that were performed with K.S. Krishnan and led to the discovery of the effect in over 60 liquids. Raman and Krishnan published their results entitled “A new type of secondary radiation” in Nature on March 28, 1928 Raman . It was soon followed by the landmark paper of G. Landsberg and L. Mandelstam who found the same effect in quartz and published a paper entitled (translated) “A novel effect of light scattering in crystals” which appeared on July 13, 1928 in Naturwissenschaften Landsberg . By the end of 1928 dozens of papers had already been published on the “Raman” effect.

In this section we first recall the quantum mechanical picture of a vibrating molecule. We then discuss the principles of different types of Raman spectroscopy.

### III.1 Molecular vibrations

Let us consider a simple diatomic molecule for explanation of the principle. The interatomic oscillation can be visualized via a classical picture of the vibrating molecule as in Fig. 2c. Quantum mechanically, the situation can be understood as depicted in Fig. 7. The potential energy of the molecule depends on the interatomic distance $`z`$ and has a well pronounced minimum. The Hamiltonian of the vibrating molecule has a set of discrete eigenstates; in Fig. 7 we show just the ground state $`|c`$ and the first excited state $`|b`$. Whereas in each of these states the mean displacement from the equilibrium position is zero, a quantum superposition of these states has generally a nonzero mean displacement $`R(t)`$ which varies with time. Assuming that in time $`t=0`$ the molecule is in a superposition state $`|\mathrm{\Psi }(0)=b|b+c|c`$, then in time $`t>0`$ the state is $`|\mathrm{\Psi }(t)=b|b+c\mathrm{exp}(i\omega t)|c`$, where the frequency $`\omega =(E_cE_b)/\mathrm{}`$ is the difference of the energies of the eigenstates $`|c`$ and $`|b`$ divided by the Planck constant $`\mathrm{}`$. The mean displacement $`R(t)`$ is then $`R(t)=\mathrm{\Psi }(t)|\widehat{R}|\mathrm{\Psi }(t)`$ is then

$`R(t)=R_0\mathrm{exp}(\omega t\phi _0)+\text{c.c.},`$ (1)
where

$`R_0=\left|bc^{}\right|b|\widehat{R}|c`$ (2)
is the displacement amplitude, $`\phi _0`$ is the initial phase (determined by the phases of the coefficients $`b`$ and $`c`$), and $`\widehat{R}`$ is the displacement operator. It can be seen from Eq. (2) that one can reach the maximum amplitude of the mean displacement if the superposition coefficients $`b`$ and $`c`$ are of the same magnitude, i.e., $`|b|=|c|=1/\sqrt{2}`$ so that $`R_0^{\text{max}}=b|\widehat{R}|c/2`$. Thus the product $`bc^{}`$ is of special importance for determining the vibrational amplitude. This coherent superposition of states is generally described by the off-diagonal density matrix element $`\rho _{bc}`$ which for the present simple case is given by $`\rho _{bc}=bc^{}`$. Without going into detail we simply state that the density matrix element $`\rho _{bc}`$ is a complex number ($`0|\rho _{bc}|1/2`$) characterizing the quantum state of the molecule and determining the amplitude of the mean displacement. For some quantum states quantum coherence is not present (e.g., energy eigenstates, thermal states, etc.), whereas for some states it can reach the maximum magnitude (i.e., for $`|\mathrm{\Psi }=2^{1/2}(|b+|c)`$).

We emphasize that when all molecules are in the same superposition state, the response of the sample to an optical signal is very different from the thermal state. Preparation and optical probing of molecular vibrations is the essence of Raman spectroscopy.

### III.2 Classical description of the Raman scattering

The simplest classical description of the Raman effect assumes that the polarizability $`\alpha `$ of the molecule is dependent on the relative positions of the atomic nuclei. The polarizability is the proportionality factor between the external electric field $`E`$ and the molecular dipole moment $`P`$, $`P=\alpha E`$, and for a vibrating molecule it is a time-dependent quantity. In the linear approximation, and assuming just the scalar case, the polarizability can be written as $`\alpha (Q)=\alpha (0)+\alpha ^{}Q`$, where $`Q`$ is the generalized coordinate of the vibrating molecule, $`\alpha (0)`$ is the polarizability of the equilibrium state, and $`\alpha ^{}=\alpha /Q`$ with $`Q=0`$. If the molecule vibrates with frequency $`\omega _{bc}`$, the coordinate $`Q`$ changes as $`Q=Q_0\mathrm{cos}(\omega _{ab}t)`$. The electric field irradiating the molecule oscillates as $`E=E_0\mathrm{cos}(\nu _1t)`$. Thus, one finds that the molecular dipole oscillates with several frequencies: with the frequency of the incoming radiation $`\nu _1`$ (leading to the Rayleigh scattering), and with the shifted frequencies $`\nu _1\pm \omega _{bc}`$ (leading to the Stokes and anti-Stokes Raman frequencies).

Even though this model is able to predict the correct frequencies of the scattered light, it cannot tell us anything about the intensities of different field components in spontaneous scattering processes. To get more information about the scattering process, one needs a quantum mechanical model of the molecule. Let us now study the main features of the various Raman scattering processes.

### III.3 Stokes vs. anti-Stokes scattering

Raman scattering is an optical phenomenon in which there is a change of frequency of the incident light. Light with frequency $`\nu _1`$ scatters inelastically off the vibrating molecules such that the scattered field has frequency $`\nu _2=\nu _1\pm \omega _{bc}`$, where $`\omega _{bc}`$ is the frequency of the molecular vibrations. The field with down-shifted frequency $`\nu _2=\nu _1\omega _{bc}`$ is called Stokes field and its generation corresponds to the process depicted in Fig. 8a, whereas the frequency up-shifted radiation is called the anti-Stokes field and corresponds to the process in Fig. 8b.

### III.4 Spontaneous vs. stimulated Raman scattering

There are two basic Raman processes: the so-called spontaneous and stimulated Raman scattering. Spontaneous scattering occurs if a single laser beam with intensity below a certain threshold illuminates the sample. In condensed matter, in propagating through 1 cm of the scattering medium, only approximately 10<sup>-6</sup> of the incident radiation is typically scattered into the Stokes field (see, e.g., Boyd ). Stimulated scattering which occurs with a very intense illuminating beam is a much stronger process in which several percent of the incident laser beam can be converted into the other frequencies. From the quantum-optical point of view, the Raman scattering can be described by means of photon numbers occupied in different modes. The rate of photon number increase in the Stokes mode can be written as $`\dot{n}_S=\eta n_L(n_S+1),`$ where $`n_L`$ is the number of photons in the incident laser mode and $`n_S`$ is the number of photons in the Stokes mode. Here $`\eta `$ is a proportionality constant.

For spontaneous Stokes scattering $`n_S1`$, and the intensity of the scattered field is roughly proportional to the length traveled by the incident field in the medium. On the other hand, for $`n_S>1`$, the stimulated process becomes dominant and the scattered field intensity can increase exponentially with the medium length.

### III.5 Resonant vs. non-resonant Raman processes

The resonant Raman process (appearing when the frequency of the incident radiation coincides with one of the electronic transitions) is much richer than the nonresonant, and we now turn to a discussion of the resonant problem.

Resonant Raman radiation is governed by the oscillating dipole between states $`|a`$ and $`|b`$ (Stokes) and/or $`|a`$ and $`|c`$ (anti-Stokes) in the notation of Fig. 3 and Table 1. In the Stokes case, the steady state coherent oscillating dipole $`P(t)`$, divided by the dipole matrix element $`\mathrm{}_{ab}=ea|r|b`$, is the important quantity. That is $`\rho _{ab}(t)P(t)/\mathrm{}_{ab}`$, as given by Eq. (A20), is

$`\varrho _{ab}=i\left[\mathrm{\Omega }_2(n_an_b)\mathrm{\Omega }_1\varrho _{cb}\right]/\left[\gamma _{ab}i(\omega _{ab}\nu _2)\right]`$ (3)
where the Raman coherence is $`\rho _{bc}`$ as discussed earlier, e.g. Fig. 7. In Eq. (3), $`\omega _{ab}`$ is the transition frequency between the electronic states $`a`$ and $`b`$, $`\nu _2`$ is the frequency of the generated field, and the other quantities are defined in the caption of Table 1.

The main advantage of resonant Raman scattering is that the signal is very strong—up to a million times stronger compared to the signal of nonresonant scattering Nelson91 . It is also very useful that only those Raman lines corresponding to very few vibrational modes associated with strongly absorbing locations of a molecule show this huge intensity enhancement. On the other hand, the resonance Raman spectra may be contaminated with fluorescence. However, this problem can be avoided by using UV light so that most of the fluorescence appears at much longer wavelengths than the Raman scattered light and is easily filtered out.

### III.6 Coherent vs. incoherent Raman scattering from many molecules

An important distinction between different Raman scattering schemes is based on the phase relation of the field scattered off different molecules. In the incoherent case the spontaneous contributions of individual molecules sum up with random phases. The magnitude of the emitted electric field then scales as $`\sqrt{N}`$ (see Fig. 9a). On the other hand, if all the molecules are prepared in the same coherent superposition of their states $`|b`$ and $`|c`$, their contributions to the emitted field have the same phases and the magnitude of their sum is proportional to $`N`$ (see Fig. 9b). Thus, the intensity radiated from the sample is proportional to $`N`$ in the incoherent case and to $`N^2`$ in the coherent case.

There is another important aspect of the coherent vs. incoherent resonant scattering process, namely the rate of emission from the $`N`$ atom ensemble. In the far off resonance, Smekel-Raman limit, the emission and absorption are simultaneous since the transitions to the excited state(s) are virtual. This is not true for the resonant Raman processes. In that case the molecule is excited to the $`|a`$ state of Fig. 10 where, in the case of weak Stokes field $`\epsilon _c`$, it can live for many nanoseconds.

However, the cooperative emission rate from $`N`$ molecules can be much faster than that of a single molecule. As was shown by Dicke, and derived in Appendix B, if the spontaneous emission lifetime of $`N`$ incoherent dipoles is given by $`\tau `$; then the cooperative spontaneous emission lifetime of $`N`$ coherently prepared dipoles can be as short as $`\tau /N`$.

This superradiant “speed up” of the radiation process can have important consequences for the present problem. We recall that the experiments of Nelson and coworkers Manoharan90 ; Nelson91 ; Ghiamati ; Manoharan93  are carried out at 242 nm so as to “ride above” the fluorescence noise, see Fig. 10b. But, if we can enhance the spontaneous emission rate so that the transition rate from the $`a_2`$ manifold to the ground state $`g`$ is faster than from the internal (non radiative) rate from $`a_2a_1`$, it would be possible to mitigate fluorescence noise. Then it would be possible to carry out resonant Raman studies with visible or near UV lasers instead of using the 242 nm wavelength.

## IV FAST CARS

### IV.1 Generation of atomic coherence

The purpose of this section is to demonstrate the utility of pulse shaping as a mechanism for generating maximal coherence. The Raman signal is optimized at the condition of maximal molecular coherence. When in this state, each of the molecules oscillates at a maximal amplitude, and all molecules in an ensemble oscillate in unison. Here we discuss several methods for the preparation of maximal coherence state.

#### IV.1.1 Adiabatic Rapid Passage via Chirped Pulses

A particularly simple and robust approach to the generation of the maximal coherence is to use a detuning $`\delta \omega `$ which is largely independent of inhomogeneous broadening and variations in matrix elements (Fig. 11).

Such multilevel molecular system can be described in terms of an effective two-by-two Hamiltonian CombGeneration . Diagonalization of this Hamiltonian (Appendix C) allows us to analyze the evolution of the system by drawing analogies to 2-state systems. If the excitation is applied resonantly ($`\mathrm{\Delta }\omega =0`$), such that the initial state of the system (the ground state $`|c`$ is projected onto the new basis formed by the eigenvectors $`|+`$ and $`|`$ \[Eq. (C5)\], the system undergoes a sinusoidal Rabi flopping between states $`|b`$ and $`|c`$. In this situation one can choose to apply a $`\pi /2`$ pulse in order to create the maximal coherence $`|\rho _{bc}|=0.5`$.

Alternatively, one can apply an excitation at a finite detuning $`\mathrm{\Delta }\omega `$, to allow all population, which is initially in the ground state, to follow the eigenstate $`|+`$ adiabatically. The coherence $`\rho _{bc}`$ is then

$$\rho _{bc}=\frac{1}{2}\mathrm{sin}\theta e^{i\phi }$$
()
For molecular systems with large detunings, the Stark shifts $`A`$ and $`D`$ are approximately equal and $`\theta \mathrm{tan}^1\left(2|B|/2\mathrm{\Delta }\omega \right)`$, where $`B`$ is the effective Raman Rabi frequency (Appendix C). One method of achieving the condition $`|\rho _{bc}|=0.5`$ is to choose $`\mathrm{\Delta }\omega `$ and to increase the product of the two incident fields until $`\theta `$ is near $`90^{}`$. This is done adiabatically with the product of the fields changing slowly as compared to the separation of the eigenvalues. Instead, at a fixed field, one may allow $`\mathrm{\Delta }\omega `$ to chirp from an initial value toward zero.

We note that earlier, Grischkowsky Grischkowsky  and Oreg et al. Oreg  have described preparation mechanisms in two-state and multi-state systems, and Kaplan et al. Kaplan  have predicted existence of $`2\pi `$ Raman solitons.

#### IV.1.2 Fractional STIRAP

In an all-resonant $`\mathrm{\Lambda }`$ scheme (Fig. 12, with $`\delta \omega =\mathrm{\Delta }\omega =0`$) maximal coherence can be prepared between the levels b and c in a fractional stimulated Raman adiabatic passage (STIRAP) set up by a counterintuitive pulse sequence Bergmann98 ; vss ; Jain , such that the population of the upper state a is always zero and fluorescence from this state is eliminated. This can be accomplished via a counterintuitive sequence of two pulses at frequencies $`\omega _{ab}`$ and $`\omega _{ac}`$. Under the condition of adiabatic passage, the molecule in the initial state $`|b`$ is transformed into a coherent state $`(|b|c)/\sqrt{2}`$.

The principle behind a STIRAP process is the adiabatic theorem as applied to the time-varying Hamiltonian $`H(t)`$. If the system at time $`t_0`$ is in an eigenstate of $`H(t_0)`$, and the evolution from $`t_0`$ to $`t_1`$ is sufficiently slow, then the system will evolve into the eigenstate of $`H(t_1)`$. The three-level atomic system driven by two fields has three eigenstates, one of which is a linear superposition of only the lower levels $`b`$ and $`c`$. The time dependent amplitudes of this eigenstate depend on the pulse shapes of the fields at frequencies $`\omega _{ab}`$ and $`\omega _{ac}`$. Thus, by an appropriate pulse shaping, it should be possible to prepare a maximally coherent superposition of states $`b`$ and $`c`$ as shown in Fig. 12. The expressions for the Hamiltonian and the corresponding eigenstates are given in Appendix D.

Comparing different schemes for the preparation of maximal coherence, we note that the required laser power is much lower for the all-resonant scheme, but in the case of biomolecules, UV lasers are required. The far-detuned scheme will work with more powerful infrared lasers, up to the point of laser damage. As for the comparison of adiabatic and non-adiabatic regimes, we should note that the adiabatic scheme may turn out to be more robust, because it does not rely on a particular pulse area and works for inhomogeneous molecular ensembles and non-uniform laser beams.

#### IV.1.3 Femtosecond Pulse Sequences

In a series of beautiful experiments K. Nelson and coworkers KANelson  have generated coherent molecular vibration via a train of femtosecond pulses, see Fig. 13. They nicely describe their work as: “Timed sequences of femtosecond pulses have been used to repetitively “push” molecules in an organic crystal…, in a manner closely analogous to the way a child on a swing may be pushed repetitively to reach oscillatory motion.”

An interesting aspect of this approach is the fact that the individual pulses need not be strong. Only the collective effect of many weak pulses is required. This may be helpful if molecular “break-up”, due to strong $`_1`$ and $`_2`$, is a problem. This will be further discussed elsewhere.

### IV.2 Adaptive Evolutionary Algorithms

So far we described how one-photon and two-photon resonant pulse sequences can be used to produce a coherent molecular superposition state. The idea is that once this state is created, a delayed pulse can be applied in order to produce Raman scattering which will bear the signature of the molecular system. The Raman signal is expected to be optimized when the molecular coherence is maximal.

In general, however, things are complicated by the Franck-Condon factors. As an example of a more complicated situation consider Fig. 14. There we see a multilevel system with the ground state $`|c`$ and the next state $`|c^{}`$. Matrix elements with Franck-Condon overlap factors yield a weak transition between $`|c^{}`$ and $`|a`$ or $`|a^{}`$ as indicated in the figure. However, given an appropriately nonlinear ground state potential it is quite possible that the next vibrational state could be off-set and have the appropriate position of the peaks of the wave function in order to maximize the Franck-Condon overlap. In this way, the coherence between the states $`|b`$ and $`|c`$ of Fig. 14 could still serve as a strong generator of the anti-Stokes radiation on the $`|a`$ to $`|b`$ transitions.

Given such a configuration, it is not hard to see how to prepare the ground state coherence. We could, for example, radiate the molecule with a chirped Raman pair so as to generate maximal coherence between $`|b`$ and $`|c^{}`$ and then follow that by a Raman $`\pi `$pulse transferring the population from $`|c^{}`$ to $`|c`$. In this way, maximal coherence between $`|c`$ and $`|b`$ would be prepared. And as indicated in the figure, strong matrix elements would be expected between $`|b,|c`$ and the first excited vibrational state of the electronic potential.

The preceding example shows that even in a simplified ideal few-level system, preparation of maximal molecular coherence may require application of a complicated pulse sequence. For large bio-molecules the level structure is not only much more complex, but usually unknown. We now consider how search algorithms can be used to find the optimal pulse sequence for a complicated molecule with an unknown Hamiltonian. This approach will eventually lead to an efficient generation of “molecular fingerprints”.

In order to achieve this goal we will need to (1) utilize a technique for preparation of complex shaped pulse sequences; (2) find the particular pulse sequences, required for the excitation of the particular bio-molecules and for the production of spectral signatures, which will allow one to distinguish (with certainty) the target biological agent from any other species.

Pulse shaping techniques already exist; they are based on “spectral modification”. First, a large coherent bandwidth is produced by an ultra-short pulse generation technique Krausz . Then, the spectrum is dispersed with a grating or a prism, and each frequency component is addressed individually by a spatial light modulator (a liquid crystal array Weiner  or an acoustic modulator Warren ). This way, individual spectral amplitudes and phases can be adjusted independently. Finally, the spectrum is recombined into a single beam by a second dispersive element, and focused onto the target. This technique allows synthesis of arbitrarily shaped pulses right at the target point, and avoids problems associated with dispersion of intermediate optical elements and windows.

A particular shaped pulse sequence can be represented by a three-dimensional surface in a space with frequency-amplitude-phase axes. Each pulse shape, which corresponds to a particular 3-D surface, produces a molecular response. The problem is to find the optimal shape. The search space is too large to be scanned completely. Besides, many local optima may exist in the problem. The solution is offered by “global search” algorithms (such as adaptive evolutionary algorithms) Assion ; Gerber . In this approach the experimental output is included in the optimization process. This way, the molecules subjected to control, are called upon to guide the search for an optimal pulse sequence within a learning loop Rabitz . With the proper algorithm, automated cycling of this loop provides a means of finding optimal pulse shapes under constraints of the molecular Hamiltonian and the experimental conditions. No prior knowledge of the molecular Hamiltonian and the potential energy surfaces is needed in this case.

This adaptive technique was developed for coherent control of chemical reactions Gerber . The idea is that the pulses can be optimized to produce desired chemical products. In our problem we want to optimize Raman generation. In this case both preparation and reading pulses can be adaptively shaped in order to maximize the signal. Fig. 15 shows schematics for the experimental setup that implements these ideas.

Generated spectra will be different for different molecular species. And our task is not only to maximize Raman generation, but also to identify spectral patterns characteristic of particular species and maximize the difference in the spectrum produced by the target bio-molecule from spectra produced by any other bio-molecules. The key idea here is to apply the same adaptive algorithms in order to learn these optimal “molecular fingerprints”.

We note that the complexity of the molecular level structure is not so much a problem as a solution to a problem. We can take advantage of the richness of the molecular structure, and the infinite variety of possible pulse shapes, in order to distinguish different species with the required certainty.

## V Possible FAST CARS measurement strategies for detection of bacterial spores

Having presented the FAST CARS technique in some detail we now return to the question of its application to “fingerprinting” of macromolecules and bacterial spores. Some aspects of the technique seem fairly simple to implement and would seem to hold relatively immediate promise. Others are more challenging but will probably be useful at least in some cases. Still other applications, e.g., the stand-off detection of bioaerosols in the atmosphere present many open questions and require careful study. In the following we discuss some simple FAST CARS experiments which are underway and/or being assembled in our laboratories.

### V.1 Preselection and hand-off scenarios

At present, field devices are being engineered which will involve an optical preselection stage based on, e.g., fluorescence tagging. If the fluorescence measurement does not match the class of particles of interest then that particle is ignored. When many such particles are tested and a possible positive is recorded, the particle is subjected to special biological assay; see Fig. 16a. Such a two stage approach can substantially speed up the detection procedure. The relatively simple fluorescence stage can very quickly sort out many uninteresting scattering centers while the more sophisticated Raman scattering protocol will only be used for the captured “suspects”.

The properly shaped preparation pulse sequence will be determined by, e.g., the adaptive learning algorithm approach as per section IV.2. The amplitude and phase content of the pulse which produces maximum oscillation may be linked to a musical tune. Each spore will have a song which results in maximum Raman coherence. A correctly chosen “melody” induces a characteristic response of the molecular vibrations—a response which is as unique as possible for the bacterial spores to be detected. Playing a melody rather than a single tone is a generalization that enables us to see a multidimensional picture of the investigated object. We note that the optimization can (and frequently will) include not only the preparation pulses 1 and 2 (see Fig. 15b), but also the probe pulse 3, in particular, its central frequency and timing. Analysis of the response to such a complex input is a complicated signal processing problem. Various data mining strategies may be utilized in a way similar to speech analysis.

However, taking into account the fact that we work with femtosecond pulses chained in picosecond to nanosecond pulse trains, the whole analysis can be very short. In particular, if we recall the long sampling time of the complete fluorescence spectra of Ghiamati  being $`15`$min, our estimation of a microsecond analysis is a very strong argument for the chosen approach.

### V.2 Possible further Raman characterization

After a suspect particle has been targeted, it may be subject to a whole variety of investigative strategies. Raman scattering off a flying particle can be very fast, but not necessarily the most accurate method. It will be very useful to pin the particle on a fixed surface and cool it down to maximize the decoherence time $`T_2`$ so that the characteristic lines are narrowed down. The particle can be deflected by optical means (laser tweezers, laser ionization, etc.) and attached to a cooled conducting surface (see Fig. 17). Cooling to liquid helium temperature would enable us to enhance the dephasing time from $`T_210^{12}`$sec at room temperature to $`T_210^9`$sec at a few degrees Kelvin.

### V.3 Possible spore specific FAST CARS detection schemes

We conclude with some speculative observations for long range (stand-off) measurements.

The chemical state of DPA in the spore is of special interest to us because the stuff we hang on the DPA molecule will determine its characteristic Raman frequency. To this end, we quote from article Murrell  by Murrell on the chemical composition of spores: “When DPA is isolated from spores it is nearly always in the Ca-CDPA chelate but sometimes as the chelate of other divalent metals \[e.g. Zn, Mn, Sr etc.\] and perhaps as a DPA-Ca amino complex.”

Thus, since each different type of spore would have its own unique mixture of metals and amino acids, it may be the case that the finer details of the Raman spectra would contain spore specific “fingerprints.” This conjecture is supported by Fig. 2b where the difference between the DPA Raman spectra of the spores of Bacillus cereus and Bacillus megaterium is encouraging.

The open question is: to what extent is the DPA Raman spectra sensitive to its environment? That we might be able to achieve spore specific sensitivity is consistent with the well known fact that substituents, e.g., NO<sub>2</sub> experience a substantial shift of their vibrational frequencies when bound in different molecular configurations, see Fig. 18. Furthermore, recent NMR experiments Leuschner01  show spore specific fingerprints due to the local environment (see Fig. 19).

Clearly there are many oportunities and open questions implicit in the FAST CARS “molecular melody” approach to real time spectroscopy. However it plays out, this combination of quantum coherence and coherent control promises to be a fascinating area of research.

###### Acknowledgements.

The authors gratefully acknowledge the support from Air Force Research Laboratory (Rome, New York), DARPA-QuIST, TAMU Telecommunication and Informatics Task Force (TITF) Initiative, ONR (contract N000014-95-1-0275), and the Welch Foundation. We would also like to thank R. Allen, Z. Arp, A. Campillo, K. Chapin, R. Cone, A. Cotton, E. Eisenstadt, J. Eversole, M. Feld, J. Golden, S. Golden, T. Hall, S. Harris, P. Hemmer, J. Laane, F. Narducci, B. Spangler, W. Warren, G. Welch, S. Wolf, and R. Zare for valuable and helpful discussions.

## Appendix A Three level system driven by two fields

In this appendix we consider the density matrix approach to the Raman scattering and discuss various limiting cases. In particular we present a semiclassical treatment in which the field evolution is described by Maxwell’s equations and the atomic system by the density operator.

We consider a three level atomic system in the $`\mathrm{\Lambda }`$ configuration with upper level a and lower levels b and c. The $`ab`$ transition is driven by a field at frequency $`\nu _1`$ and the $`ac`$ transition is coupled via a signal field at frequency $`\nu _2`$.

The Maxwell’s equations lead to the following equation for the evolution of the signal field,

$`\left({\displaystyle \frac{^2}{z^2}}{\displaystyle \frac{1}{c^2}}{\displaystyle \frac{^2}{t^2}}\right)E`$ $`=`$ $`\mu _o\ddot{P},`$ (A1)
where $`E`$ is the electric field vector of the emitted light, $`\mu _o`$ is the vacuum permeability, and P is the medium polarization. We write the electric field using the slowly varying envelope E as

$`E`$ $`=`$ $`{\displaystyle \frac{1}{2}}(z,t)e^{i(\nu tkz+\varphi )}+c.c.`$ (A2)
and write the polarization in terms of the slowly varying quantity $`P`$ as

$`P`$ $`=`$ $`{\displaystyle \frac{1}{2}}𝒫(z,t)e^{i(\nu tkz+\varphi )}+c.c..`$ (A3)
Working within the slowly varying amplitude and phase approximation, Eqs. (A1), (A2), and (A3) yield

$$\frac{1}{c}\frac{}{t}+\frac{}{z}=\frac{1}{2ϵ_0}k\text{Im}𝒫,$$
(A4)
where

$`𝒫=2𝒩(z,t)\mathrm{}_{ab}\varrho _{ab}e^{i(\nu tkz+\varphi )}.`$ (A5)
Here $`\mathrm{}_{ab}`$ is the dipole moment matrix element, $`\varrho _{ab}`$ is the off-diagonal element of the density matrix for the molecular levels $`a`$ and $`b`$, and $`𝒩(z,t)`$ is the volume density of the molecules. We note that the electromagnetic field is determined by $`\varrho _{ab}`$.

Here we recall the main results of Dream  and apply them to our physical situation (see Fig. 20). First we define the decay rates

$`\gamma _{ab}`$ $`=`$ $`{\displaystyle \frac{\gamma +\gamma _1}{2}}+\gamma _{ab}^p,`$ (A6)
$`\gamma _{ca}`$ $`=`$ $`{\displaystyle \frac{\gamma }{2}}+\gamma _{ca}^p,`$ (A7)
$`\gamma _{cb}`$ $`=`$ $`{\displaystyle \frac{\gamma _1}{2}}+\gamma _{cb}^p.`$ (A8)
Here the decay rates from $`a`$ to $`b`$ is $`\gamma _b`$, and from $`a`$ to $`c`$ is $`\gamma _c`$, and $`\gamma =\gamma _b+\gamma _c`$. Population decay rate from $`b`$ to $`c`$ is $`\gamma _1`$. Purely phase decays are designated by the superscript $`p`$. Complex dephasings are defined as

$`\mathrm{\Gamma }_{ab}`$ $`=`$ $`\gamma _{ab}i\mathrm{\Delta }_{ab},`$ (A9)
$`\mathrm{\Gamma }_{ca}`$ $`=`$ $`\gamma _{ca}+i\mathrm{\Delta }_{ac},`$ (A10)
$`\mathrm{\Gamma }_{cb}`$ $`=`$ $`\gamma _{cb},`$ (A11)
where $`\mathrm{\Delta }_{ac}=\omega _{ac}\nu _1`$ and $`\mathrm{\Delta }_{ab}=\nu _2\omega _{ab}`$. In the following we assume Raman resonance, i.e., $`\mathrm{\Delta }_{ac}=\mathrm{\Delta }_{ab}=\mathrm{\Delta }`$. The main working equations for the off-diagonal density matrix elements are

$`\dot{\varrho }_{ab}`$ $`=`$ $`\mathrm{\Gamma }_{ab}\varrho _{ab}+i\mathrm{\Omega }_2(\varrho _{bb}\varrho _{aa})+i\mathrm{\Omega }_1\varrho _{cb},`$ (A12)
$`\dot{\varrho }_{ca}`$ $`=`$ $`\mathrm{\Gamma }_{ca}\varrho _{ca}+i\mathrm{\Omega }_1^{}(\varrho _{aa}\varrho _{cc})i\mathrm{\Omega }_2^{}\varrho _{cb},`$ (A13)
$`\dot{\varrho }_{cb}`$ $`=`$ $`\mathrm{\Gamma }_{cb}\varrho _{cb}i\mathrm{\Omega }_2\varrho _{ca}+i\mathrm{\Omega }_1^{}\varrho _{ab}.`$ (A14)
The equations for the populations are

$`\dot{\varrho }_{bb}`$ $`=`$ $`i\mathrm{\Omega }_2^{}\varrho _{ab}i\mathrm{\Omega }_2\varrho _{ba}+\gamma _b\varrho _{aa}\gamma _1\varrho _{bb},`$ (A15)
$`\dot{\varrho }_{cc}`$ $`=`$ $`i\mathrm{\Omega }_1^{}\varrho _{ac}i\mathrm{\Omega }_1\varrho _{ca}+\gamma _c\varrho _{aa}+\gamma _1\varrho _{bb},`$ (A16)
and $`\varrho _{aa}`$ is obtained from

$`1`$ $`=`$ $`\varrho _{aa}+\varrho _{bb}+\varrho _{cc}.`$ (A17)
Here $`\mathrm{\Omega }_{1,2}`$ are the Rabi frequencies of the fields having frequencies $`\nu _{1,2}`$, i.e.,

$`\mathrm{\Omega }_1`$ $`=`$ $`{\displaystyle \frac{\mathrm{}_{ac}_1}{\mathrm{}}},`$ (A18)
$`\mathrm{\Omega }_2`$ $`=`$ $`{\displaystyle \frac{\mathrm{}_{ab}_2}{\mathrm{}}},`$ (A19)
The steady state solution of these equations can be obtained by setting all time derivatives equal to zero. The result is

$$\overline{)\varrho _{ab}=\frac{i}{\mathrm{\Gamma }_{ab}}[\mathrm{\Omega }_2(\varrho _{aa}\varrho _{bb})\mathrm{\Omega }_1\varrho _{cb}],}$$
(A20)
and

$`\varrho _{ca}`$ $`=`$ $`{\displaystyle \frac{i\mathrm{\Omega }_1^{}}{𝒟}}\left[(\varrho _{aa}\varrho _{cc})(\mathrm{\Gamma }_{ab}\mathrm{\Gamma }_{cb}+|\mathrm{\Omega }_1|^2)+(\varrho _{bb}\varrho _{aa})|\mathrm{\Omega }_2|^2\right],`$ (A21)
$`\varrho _{cb}`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_2\mathrm{\Omega }_1^{}}{𝒟}}\left[(\varrho _{aa}\varrho _{bb})\mathrm{\Gamma }_{ca}+(\varrho _{aa}\varrho _{cc})\mathrm{\Gamma }_{ab}\right],`$ (A22)
where the common denominator is

$`𝒟=\mathrm{\Gamma }_{ab}\mathrm{\Gamma }_{ca}\mathrm{\Gamma }_{cb}+\mathrm{\Gamma }_{ab}|\mathrm{\Omega }_2|^2+\mathrm{\Gamma }_{ca}|\mathrm{\Omega }_1|^2.`$ (A23)
Equation (A20) is our main working equation. The first term in the parenthesis of Eq. (A20) is responsible for the stimulated emission or absorption on the $`|a|b`$ transition. The second, $`\varrho _{cb}`$, term describes the Raman conversion of $`\nu _1`$ into $`\nu _2`$. As we can see, it is crucial to have the element $`\varrho _{cb}`$ as big as possible for optimum Raman conversion. In the following we present the main properties of $`\varrho _{cb}`$ for various experimental and conceptual configurations and consider various limiting cases for the Raman processes.

### A.1 Off-resonant Raman process, weak driving

First we consider the Raman effect far from electronic resonance ($`\mathrm{\Delta }\gamma _{ab},\gamma _{ac}`$). In this case the upper level $`a`$ is almost completely depopulated and can be eliminated from the dynamics. The system behaves basically as a two-level system with the Rabi frequency of oscillations between levels $`b`$ and $`c`$ equal to $`\mathrm{\Omega }_R=|\mathrm{\Omega }_1^{}\mathrm{\Omega }_2|/\mathrm{\Delta }`$. For dephasing rate $`\gamma _{bc}\mathrm{\Omega }_R`$, we find the steady state solution for the lower state coherence $`\varrho _{cb}`$ as

$`\underset{\mathrm{\Delta }\gamma }{lim}\varrho _{cb}`$ $`=`$ $`i{\displaystyle \frac{\mathrm{\Omega }_1^{}\mathrm{\Omega }_2}{\gamma _{bc}\mathrm{\Delta }}}(\varrho _{cc}\varrho _{bb}),`$ (A24)
which, after substituting into Eq. (A20), yields the density matrix element responsible for the $`\nu _2`$ radiation as

$`\varrho _{ab}^{\text{Raman}}`$ $`=`$ $`i{\displaystyle \frac{\mathrm{\Omega }_2}{\gamma _{ab}i\mathrm{\Delta }}}\left[(\varrho _{aa}\varrho _{bb})i{\displaystyle \frac{|\mathrm{\Omega }_1|^2}{\gamma _{bc}\mathrm{\Delta }}}(\varrho _{cc}\varrho _{bb})\right].`$ (A25)
Note that for the amplification of the $`\nu _2`$ field the so-called Raman inversion $`\varrho _{cc}\varrho _{bb}`$ is necessary. In the simplest case when almost all the molecules are in the lowest state $`c`$, $`\varrho _{cc}1`$, $`\varrho _{bb}0`$, $`\varrho _{aa}0`$, Eq. (A25) reduces to

$`\varrho _{ab}^{\text{Raman}}`$ $`=`$ $`i{\displaystyle \frac{\mathrm{\Omega }_2}{\mathrm{\Delta }}}{\displaystyle \frac{|\mathrm{\Omega }_1|^2}{\mathrm{\Delta }\gamma _{bc}}}.`$ (A26)
### A.2 Off-resonant Raman process, strong driving

In the case of strong driving the transition between states $`b`$ and $`c`$ can be saturated so that both these levels are significantly populated (with virtually no population in the excited state $`a`$). In particular, one obtains from Eq. (A15) the steady state populations of the lower levels

$`\rho _{bb}={\displaystyle \frac{i\mathrm{\Omega }_2^{}\rho _{ab}i\mathrm{\Omega }_2\rho _{ba}}{\gamma _1}},`$ (A27)
and $`\rho _{cc}=1\rho _{bb}`$. Substituting Eq. (A20) into Eq. (A27), and assuming, without loss of generality, that the Rabi frequencies for the laser fields are real ($`\mathrm{\Omega }_1=\mathrm{\Omega }_1^{},\mathrm{\Omega }_2=\mathrm{\Omega }_2^{}`$) we find that for the far off-resonant case ($`\mathrm{\Gamma }_{ab}i\mathrm{\Delta }`$)

$`\rho _{bb}={\displaystyle \frac{2\mathrm{\Omega }_2\mathrm{\Omega }_1\rho _{bc}}{i\mathrm{\Delta }\gamma _1}}.`$ (A28)
Rearranging Eq. (A22) and inserting Eq. (A28), under the condition

$`\gamma _{bc}\left|{\displaystyle \frac{|\mathrm{\Omega }_1|^2}{i\mathrm{\Delta }}}+{\displaystyle \frac{|\mathrm{\Omega }_2|^2}{i\mathrm{\Delta }}}\right|,`$ (A29)
we find that

$`\rho _{bc}={\displaystyle \frac{\mathrm{\Omega }_2\mathrm{\Omega }_1}{i\mathrm{\Delta }\mathrm{\Gamma }_{bc}}}{\displaystyle \frac{4\mathrm{\Omega }_2^2\mathrm{\Omega }_1^2\rho _{bc}}{\gamma _1\mathrm{\Delta }^2\mathrm{\Gamma }_{bc}}}.`$ (A30)
Solving Eq. (A30) for $`\rho _{bc}`$ we obtain

$`\rho _{bc}={\displaystyle \frac{i\mathrm{\Omega }_2\mathrm{\Omega }_1}{\mathrm{\Delta }}}\left(\gamma _{bc}+{\displaystyle \frac{4\mathrm{\Omega }_2^2\mathrm{\Omega }_1^2}{\gamma _1\mathrm{\Delta }^2}}\right)^1.`$ (A31)
It can be shown that the maximum magnitude of the coherence $`|\rho _{bc}|`$ is given by

$`\left|\rho _{bc}\right|=\sqrt{{\displaystyle \frac{\gamma _1}{16\gamma _{bc}}}}.`$ (A32)
This maximum occurs when

$`{\displaystyle \frac{\mathrm{\Omega }_1\mathrm{\Omega }_2}{\mathrm{\Delta }}}={\displaystyle \frac{\sqrt{\gamma _1\gamma _{bc}}}{2}}.`$ (A33)
### A.3 Resonant Raman process, weak driving

In the resonant case ($`\mathrm{\Delta }=0`$), the Raman effect has much in common with the scheme of lasing without inversion (LWI; see, e.g., Dream ). The lower state coherence is then found to be

$$\varrho _{cb}\stackrel{\mathrm{\Delta }=0}{}\mathrm{\Omega }_2\mathrm{\Omega }_1^{}\frac{[(\varrho _{aa}\varrho _{bb})\gamma _{ca}+(\varrho _{aa}\varrho _{cc})\gamma _{ab}]}{\gamma _{ab}\gamma _{ac}\gamma _{cb}+\gamma _{ca}|\mathrm{\Omega }_1|^2+\gamma _{ab}|\mathrm{\Omega }_2|^2}.$$
(A34)
Polarization responsible for the $`\nu _2`$ radiation is then governed by

$$\varrho _{ab}=i\frac{\mathrm{\Omega }_2}{\gamma _{ab}}\left[(\varrho _{aa}\varrho _{bb})\left(1\frac{|\mathrm{\Omega }_1|^2\gamma _{ca}}{D}\right)(\varrho _{aa}\varrho _{cc})\frac{|\mathrm{\Omega }_1|^2\gamma _{ab}}{D}\right],$$
(A35)
where $`D=\gamma _{ab}\gamma _{ca}\gamma _{cb}+\gamma _{ab}|\mathrm{\Omega }_2|^2+\gamma _{ca}|\mathrm{\Omega }_1|^2`$.

In the weak driving limit ($`\mathrm{\Omega }_{1,2}\gamma _{ab},\gamma _{ac},\gamma _{bc}`$), almost all the population remains in state $`c`$ ($`\varrho _{cc}1`$, $`\varrho _{bb}0`$, $`\varrho _{aa}0`$). The atomic coherence of the lower levels is

$$\rho _{cb}=\frac{\mathrm{\Omega }_1^{}\mathrm{\Omega }_2}{\gamma _{ac}\gamma _{bc}},$$
(A36)
and the corresponding expression for the density matrix element $`\rho _{ab}`$ is

$$\varrho _{ab}^{\text{Resonant Raman}}=i\frac{\mathrm{\Omega }_2}{\gamma _{ab}}\frac{|\mathrm{\Omega }_1|^2}{\gamma _{ac}\gamma _{bc}}.$$
(A37)
### A.4 Resonant Raman process, strong driving

In the resonant case we can find the steady state solution of a strongly driven three-level system ($`|\mathrm{\Omega }_{1,2}|\gamma _1,\gamma _{bc}`$) in the form of the so-called dark state. It is useful to consider two superpositions of the lower states $`|b`$ and $`|c`$ defined as

$`|B`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_2|b+\mathrm{\Omega }_1|c}{\mathrm{\Omega }}},`$ (A38)
$`|D`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_1|b\mathrm{\Omega }_2|c}{\mathrm{\Omega }}},`$ (A39)
where $`\mathrm{\Omega }=\sqrt{|\mathrm{\Omega }_1|^2+|\mathrm{\Omega }_2|^2}`$. The state $`|D`$ is completely decoupled from the upper state $`|a`$ ($`\widehat{H}|D=0`$), and is called the dark state. If the molecule starts in any state different from $`|D`$, the fields $`\mathrm{\Omega }_1`$ and $`\mathrm{\Omega }_2`$ will promote it to the upper state $`|a`$, which decays to the lower states by spontaneous emission. If the molecule is in $`|D`$ it stays there unchanged. In this way the dark component of the state increases and finally the system will end up completely in the state $`|D`$. The populations of the levels $`a`$ and $`b`$ are $`\rho _{aa}=0`$ and $`\rho _{bb}=|\mathrm{\Omega }_1|^2/\mathrm{\Omega }^2`$, and the dark state coherence of the lower states is, as given by Eq. (A39),

$`\varrho _{cb}`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Omega }_1^{}\mathrm{\Omega }_2}{\mathrm{\Omega }^2}}.`$ (A40)
Maximum Raman coherence is achieved with $`|\mathrm{\Omega }_1|=|\mathrm{\Omega }_2|`$ so that $`|\rho _{bc}^{\text{max}}|=1/2`$. The element $`\varrho _{ab}`$ \[see Eq. (A20)\] responsible for the radiation is given by

$`\varrho _{ab}^{\text{Dark Raman}}`$ $`=`$ $`{\displaystyle \frac{i}{\gamma _{ab}}}\left[\mathrm{\Omega }_2(\varrho _{aa}\varrho _{bb})+{\displaystyle \frac{|\mathrm{\Omega }_1|^2\mathrm{\Omega }_2}{\mathrm{\Omega }^2}}\right]=0,`$ (A41)
i.e., there is no radiation from the dark state. To obtain Raman signal one can, e.g, switch off the field $`\mathrm{\Omega }_2`$ after reaching the maximum coherence $`|\varrho _{cb}^{\text{max}}|=1/2`$. Then the density matrix element $`\varrho _{ab}`$ goes as

$`\varrho _{ab}^{\text{Max coherence}}=i{\displaystyle \frac{\mathrm{\Omega }_1}{2\gamma _{ab}}}.`$ (A42)
To summarize the main results of this appendix, we display the density matrix elements responsible for the signal field generation in Table 1.

## Appendix B Cooperative Spontaneous Emission

Since the DPA is contained in the small ($`V(1\mu )^3`$) volume of the core and since the number of participating DPA molecules is huge ($`N10^9`$) the possibility of Dicke superradiance should be carefully considered. At the outset, we should note that the short dephasing times of vibronic levels ($`T_2`$ is in the picosecond range) and the unknown inhomogeneous dephasing time $`T_2^{}`$ will tend to wash out the effect. Still, if the spontaneous emission time ($`\tau 110`$ nanoseconds) is reduced by even a small fraction of N, then cooperative spontaneous emission may be important.

Motivated by the proceeding we now turn to a short review of the effect from the present, FAST CARS, perspective. We focus on two levels $`|a`$ and $`|b`$. The previous pulses $`\epsilon _1`$ and $`\epsilon _2`$ beat the coherence between $`|b`$ and $`|c`$ so that at time $`t=0`$

$$|\mathrm{\Psi }(0)=B|b+C|c,$$
(B1)
the third pulse, arriving at time T, promotes $`|c|a`$ so that at time $`t=\tau `$

$$|\mathrm{\Psi }(\tau )=A|a+B|b+C^{}|c.$$
(B2)
Hence the atoms at time $`\tau `$ are in a coherent superposition $`|a`$ and $`|b`$ and this affects the rate of spontaneous emission from the N molecules involved.

For the present purposes it is best to start with the Hamiltonian describing the interaction of N two level systems ($`|a`$ and $`|b`$) and the quantized radiation field given by

$$H_{\text{int}}=\mathrm{\Sigma }_{i,k}\mathrm{}ga_k^+\sigma _ie^{ikr_i}+adj$$
(B3)
where, as discussed, e.g., in ScullyZubairy , $`g_k`$ is the coupling frequency between the molecules and the $`k^{th}`$ mode of the field, $`a_k^+`$ is the usual creation operator and $`\sigma _i=(|ba|)_i`$ is the lowering operator for the $`i^{th}`$ molecule.

Consider next the case in which all molecules are located at $`r_i=r_0`$ in a volume small compared to the radiation wavelength $`\lambda `$, and noting that the coupling constant is a slowly varying function of $`k`$ we may write

$$H_{\text{int}}=\left[g_ke^{ik_0r_0}\underset{k}{}a_k^+\right]\underset{i}{}\sigma _i,$$
(B4)
The important point being that the lowering operator described by Eq. (B4) is symmetric in the molecular lowering operator $`\sigma _i`$.

To glean the physics from Eq. (B4) it is enough to consider 3 molecules which are all started in their upper state, so that

$$|\mathrm{\Psi }_3=|a_1a_2a_3.$$
(B5)
The state (B5) evolves under the influence of the field according to the interaction (B4), and the molecular state develops into $`|\mathrm{\Psi }_3\alpha |\mathrm{\Psi }_3+\beta |\mathrm{\Psi }_2`$ where $`\alpha `$ and $`\beta `$ are uninteresting constants and

$$|\mathrm{\Psi }_2=\underset{i}{}\sigma _i|\mathrm{\Psi }_3=|b_1a_2a_3+|a_1b_2a_3+|a_1a_2b_3.$$
(B6)
In general the symmetric interaction (B4) only couples the $`|a_1a_2a_3`$ state to the symmetric states of Fig. 21.

Thus we may, following Dicke describe our N “spins” by an effective angular momentum of magnitude $`j=\frac{1}{2}(N_++N_{})`$ and projection $`m_j=\frac{1}{2}(N_+N_{})`$.

Using this “angular momentum” picture and recalling that the matrix element governing the transition rate between state $`|j,m_j`$ and $`|j,m_j+1`$ is given by

$$\mu =j,m_j+1|\widehat{J_{}}|j,m_j=\sqrt{(jm_j)(jm_j+1)}$$
(B7)
we have two interesting limits.

First the case when all spins are up i.e., $`N_+=N,N_{}=0`$ (which corresponds to the case of all molecules in $`|a`$); then $`j=\frac{N_++N}{2}\frac{1}{2}`$ and $`m_j=\frac{N_+N}{2}\frac{N}{2}`$ and we have

$$\mu =j,m_j+1|\widehat{J_{}}|j,m_j=\sqrt{N}.$$
(B8)
Therefore the radiation rate goes as $`\mu ^2=N`$, which is the normal result for N independent radiators.

In the other case suppose that $`m_j=0`$ so that $`N_+=\frac{N}{2}`$ and $`N_{}=\frac{N}{2}`$. Then the relevant matrix element is

$$\mu =j,1|\widehat{J_{}}|j,0=\sqrt{j(j+1)}N,$$
(B9)
and the radiation rate goes as $`N^2`$. That is the state $`|j,0`$ decays N times faster than the state $`|j,j`$; and therefore the state for which $`m_j=0`$ (equivalently $`N_+=\frac{N}{2}`$ and $`N_{}=\frac{N}{2}`$) is said to be “superradiant.” In fact, any such state for which $`|m_j||j|`$ is said to be superradiant.

Returning now to our problem in which the levels $`|a`$ and $`|b`$ are coherently prepared, suppose that A and B of Eq. (B1) are both $`\frac{1}{\sqrt{2}}`$. An ensemble of N such coherently prepared molecules will be described by a superposition of $`m_j`$ levels sharply peaked about $`m_j=0`$ and is thus superradiant.

The major potential payoff from our perspective is the hope that the coherent resonant Raman process may direct the molecules from $`cab`$ on a time scale which is of the order $`\tau /N`$ where $`\tau `$ is the spontaneous fluorescence time. This would be interesting since, as emphasized by Nelson and coworkers Manoharan90 : “This \[utilization of resonant Raman spectra\] is possible, however, only in the absence of fluorescence interference.”

But, as is discussed in Section V there are many open questions. For example, will the coherence decay rates $`T_2`$ and $`T_2^{}`$ spoil the effect? These and other questions need to be addressed by careful experiments and further analysis.

## Appendix C Eigenstates and eigenvectors for a molecular system with large one-photon detunings.

In the case of large one-photon detunings $`\delta \omega `$ (such that only small virtual excitation of the upper state is possible), the molecular system of Fig. 11 is described by an effective two-by-two Hamiltonian CombGeneration :

$`H_{\mathrm{eff}}={\displaystyle \frac{\mathrm{}}{2}}\left[\begin{array}{cc}A& \mathrm{\Omega }\\ \mathrm{\Omega }^{}& D2\mathrm{\Delta }\omega \end{array}\right],`$ (C3)
where $`\mathrm{\Omega }=\mathrm{\Omega }_b\mathrm{\Omega }_c/\delta \omega `$ is the effective Raman Rabi frequency, $`A`$ and $`D`$ are dynamic Stark shifts (see CombGeneration  for more details), and $`\mathrm{\Delta }\mathrm{\Omega }`$ is the (two-photon) Raman detuning. The eigenvalues of the Hamiltonian (C3) are

$`E_\pm ={\displaystyle \frac{(A+D2\mathrm{\Delta }\omega )\pm \sqrt{(AD+2\mathrm{\Delta }\omega )^2}+4|\mathrm{\Omega }|^2}{4}},`$ (C4)
and the corresponding eigenvectors are

$`|\pm ={\displaystyle \frac{\mathrm{\Omega }|b+(A+2E_\pm )|c}{\sqrt{|\mathrm{\Omega }|^2+(A+2E_\pm )^2}}}.`$ (C5)
In the case when $`AD`$ we have

$`E_\pm {\displaystyle \frac{A\mathrm{\Delta }\omega \sqrt{\mathrm{\Delta }\omega ^2+|\mathrm{\Omega }|^2}}{2}}.`$ (C6)
The probabilities of occupation of states $`|b`$ and $`|c`$ are

$`P_b`$ $`=`$ $`{\displaystyle \frac{|\mathrm{\Omega }|^2}{|\mathrm{\Omega }|^2+(A+2E_\pm )^2}}`$
$``$ $`{\displaystyle \frac{|\mathrm{\Omega }|^2}{2\left(|\mathrm{\Omega }|^2+\mathrm{\Delta }\omega ^2\pm \mathrm{\Delta }\omega \sqrt{\mathrm{\Delta }\omega ^2+|\mathrm{\Omega }|^2}\right)}},`$ (C7)
$`P_c`$ $``$ $`{\displaystyle \frac{\left(\mathrm{\Delta }\omega \pm \sqrt{\mathrm{\Delta }\omega ^2+|\mathrm{\Omega }|^2}\right)^2}{2\left(|\mathrm{\Omega }|^2+\mathrm{\Delta }\omega ^2\pm \mathrm{\Delta }\omega \sqrt{\mathrm{\Delta }\omega ^2+|\mathrm{\Omega }|^2}\right)}}.`$ (C8)
Thus, if we start at $`t\mathrm{}`$ on eigenstate $`|`$ with $`\mathrm{\Delta }\omega |\mathrm{\Delta }\omega |`$, we have $`P_b(\mathrm{})=0`$ and $`P_c(\mathrm{})=1`$. Chirping $`\mathrm{\Delta }\omega `$ such that for $`t+\mathrm{}`$ we have $`\mathrm{\Delta }\omega |\mathrm{\Delta }\omega |`$, the $`|`$ eigenstate changes adiabatically such that the probabilities get exchanged to $`P_b(\mathrm{})=1`$ and $`P_c(\mathrm{})=0`$. At the moment when $`\mathrm{\Delta }\omega =0`$ we have $`P_b=P_c=1/2`$ and $`\rho _{bc}=1/2e^{i\varphi }`$, where $`\mathrm{\Omega }=|\mathrm{\Omega }|e^{i\varphi }`$. Thus, if we turn off the pulses at this time, we reach full coherence.

## Appendix D Fractional STIRAP

We consider a three-level atomic system driven by resonant pulses at frequencies $`\omega _{ab}`$ and $`\omega _{ac}`$ with Rabi frequencies $`\mathrm{\Omega }_1(t)=\mathrm{}_{ab}_1(t)/\mathrm{}`$ and $`\mathrm{\Omega }_2(t)=\mathrm{}_{ac}_2(t)/\mathrm{}`$, respectively (se vss  for more details). The Hamiltonian for the system in the slowly varying amplitude and phase approximation is

$$H=\frac{\mathrm{}}{2}(\mathrm{\Omega }_1(t)|ab|+\mathrm{\Omega }_2(t)|ac|+H.c.),$$
(D1)
where $`H.c.`$ means Hermitian conjugate and $`|a`$ is the excited state. This system has a dark state. The eigenvalue of the Hamiltonian for this state is equal to zero, $`\lambda _D=0`$, i.e., $`\widehat{H}|D=\lambda _D|D=0`$. For the scheme shown, the dark state is

$$|D=\frac{\mathrm{\Omega }_1(t)|c\mathrm{\Omega }_2(t)|b}{\sqrt{|\mathrm{\Omega }_1(t)|^2+|\mathrm{\Omega }_2(t)|^2}}.$$
(D2)
This state mixes the ground states $`|b`$ and $`|c`$ and is independent of the excited state $`|a`$.

The sequence of pulses with Rabi frequencies $`\mathrm{\Omega }_1(t)`$ and $`\mathrm{\Omega }_2(t)`$ is such that, for the molecular system initially in the state $`|b`$, $`\mathrm{\Omega }_1(t)/\mathrm{\Omega }_2(t)0`$ at $`t\mathrm{}`$ and $`\mathrm{\Omega }_1(t)/\mathrm{\Omega }_2(t)\mathrm{tan}\theta `$ as $`t+\mathrm{}`$. Thus the state evolves adiabatically from $`|b`$ to the coherent state $`\mathrm{cos}\theta |b\mathrm{sin}\theta |c`$. For the case when $`\mathrm{\Omega }_1(t)/\mathrm{\Omega }_2(t)1`$, $`\theta =\pi /4`$ and the resulting state is $`(|b|c)/\sqrt{2}`$. We can see that, unlike the case of conventional STIRAP, the two pump pulses vanish simultaneously. In the conventional STIRAP the main aim is to bring a system from one low-lying energy eigenstate to another without populating an excited state on the way. The pump pulses in the conventional STIRAP are timed such that the pulse connected to the target state starts before the beginning and ends before the end of the pulse connected to the initial state (i.e., the so called counterintuitive sequence). The main aim of the fractional STIRAP is to bring the system from an energy eigenstate to a preselected superposition of two lower lying eigenstates, without populating any other state. This task requires a modified timing of the pump pulses. In contrast to the scheme discussed in the preceding Appendix C, the pump pulses of the fractional STIRAP are resonant which means that much weaker field or shorter duration of the pulses is required.


text:
# Møller Energy-Momentum Complex for an Axially Symmetric Scalar Field

## 1 Introduction

The subject of energy-momentum localization in general relativity continues to be one of the most intricate because there is no given yet a generally accepted expression for the energy and momentum. It is well-known that various energy-momentum complexes - can give the same energy distribution for a given space-time. Recently, Virbhadra  studied if it is possible to obtain the same expression of the energy in the case of a Kerr-Schild metric by using the energy-momentum complexes of Einstein , Landau and Lifshtz , Papapetrou  and Weinberg  ELLPW. He concluded that these definitions lead to the same result. On the other hand, these definitions disagree for the most general nonstatic spherically symmetric metric . Only the Einstein energy-momentum complex gives the same expression for the energy distribution when the calculations are performed in the Kerr-Schild Cartesian and Schwarzschild Cartesian coordinates.

Also, many results recently obtained, , , ,  demonstrated that the Møller energy-momentum complex  is a good tool for obtaining the energy distribution of a given space-time. Møller energy-momentum complex allows to make the calculations in any coordinate system. In his recent paper, Lessner  concluded that the Møller definition is a powerful concept of energy and momentum in general relativity. Very interesting is the Cooperstock  hypothesis. He sustain that the energy and momentum are confined to the regions of nonvanishing energy-momentum tensor of the matter and all non-gravitational fields.

Also, Chang, Nester and Chen  showed that the energy-momentum complexes are actually quasilocal and legitimate expressions for the energy-momentum.

The purpose of this paper is to compute the energy distribution, for an axially symmetric solution that describes the space-time, which is endowed with a scalar field, in the Møller prescription. Recently gravitational lensing due to this space-time has been studied in a great detail , . We use the geometrized units $`(G=1`$, $`c=1)`$ and follow the convention that Latin indices run from $`0`$ to $`3`$.

## 2 Møller Energy-Momentum Complex for on Axially Symmetric Scalar Field

It is well-known that the Kaluza-Klein and the superstring theories predict the scalar fields as a fundamental interaction in physics. Scalar fields are fundamental components of the Brans-Dicke theory and of the inflationary models. Also, they are a good candidate for the dark matter in spiral galaxies. Because they interact very weakly with mater we have never seen one but many of the theories containing scalar fields are in good concordance with measurements in weak gravitational fields. Also, we expect that they can play an important role in strong gravitational fields like at the origin of the universe or in pulsars or black holes. The metric that we consider ,  is an axially symmetric solution to the field equations derived from the action for gravity minimally coupled to a scalar field. The solution is

$$ds^2=\left(1\frac{2m}{r}\right)dt^2\frac{e^{2k_a}dr^2}{1\frac{2m}{r}}r^2\left(e^{2k_a}d\theta ^2+\mathrm{sin}^2\theta d\phi ^2\right),$$
(1)
with

$$e^{2k_a}=\left(1+\frac{m^2\mathrm{sin}^2\theta }{r^2\left(1\frac{2m}{r}\right)}\right)^{1/a^2},$$
(2)
$$\varphi =\frac{1}{2a}\mathrm{ln}\left(1\frac{2m}{r}\right),$$

where $`a`$ is a constant of integration and $`\varphi `$ is the scalar field. This solution is one of the new classes of solutions to the Einstein-Maxwell theory non minimally coupled to a dilatonic field . The metric given by (1) is almost spherically symmetric and represents a gravitational body (gravitational monopole) with scalar field. The scalar field deforms the spherically symmetry. We observe, that when $`a\mathrm{}`$, we recover the Schwarzschild solution. This metric can be employed to model the exterior field of a macroscopic object endowed with a minimally coupled scalar field, and it can be matched to a regular interior solution.

The Møller energy-momentum complex  is given by

$$\theta _i^k=\frac{1}{8\pi }\frac{\chi _i^{kl}}{x^l}$$
(3)
where

$$\chi _i^{kl}=\sqrt{g}\left(\frac{g_{in}}{x^m}\frac{g_{im}}{x^n}\right)g^{km}g^{en}.$$
(4)
The energy in the Møller prescription is given by

$$E=\theta _0^{\mathrm{\hspace{0.33em}0}}𝑑x^1𝑑x^2𝑑x^3=\frac{1}{8\pi }\frac{\chi _0^{\mathrm{\hspace{0.33em}0}}}{\chi ^l}𝑑x^1𝑑x^2𝑑x^3.$$
(5)
The Møller energy-momentum complex is not necessary to carry out the calculations in the quasi-Cartesian coordinates, so we can calculate in the spherical coordinates.

For the metric given by (1) the only required component of $`\chi _0^{\mathrm{\hspace{0.33em}0}l}`$ is

$$\chi _0^{\mathrm{\hspace{0.33em}01}}=2m\mathrm{sin}\theta .$$
(6)
Plugging (6) in (5) and applying the Gauss theorem we obtain

$$E=m.$$
(7)
The energy distribution is given by the mass $`m`$.

## 3 Discussion

We use an axially symmetric solution to the field equations for a scalar field minimally coupled to gravity. Virbhadra et al.  demonstrated that the presence of on object endowed with a scalar field acting as a gravitational lens would manifest through new lensing configurations. For the above situation we obtain the energy for the metric given by (1) by using the Møller energy-momentum complex. The energy distribution is given by the mass $`m`$. In the case of the Schwarzschild metric we obtain the same result. The Schwarzschild solution is a particular case of the metric that we use, when we have $`a\mathrm{}`$.


text:
# 1 Introduction

## 1 Introduction

Berenstein, Maldacena and Nastase (BMN)  have recently put forward a remarkable proposal, extending the regime of gauge theory description from supergravity to the full-fledged closed string theory. The idea is to utilize conserved global charges in the gauge theory and reorganize the perturbative expansion. For example, for $`𝒩=4`$ super Yang-Mills theory in four-dimensions, correlation functions involving operators of scaling dimension $`\mathrm{\Delta }`$ and global charge $`J`$ are reorganizable in a calculable manner in the limit:

$`\lambda ^2=g_{\mathrm{YM}}^2N\mathrm{},g_{\mathrm{eff}}^2={\displaystyle \frac{\lambda ^2}{J^2}}\mathrm{finite},\left(\mathrm{\Delta }J\right)\mathrm{finite}.`$ (1)
In this limit, effective expansion parameter is set by $`g_{\mathrm{eff}}^2`$, in sharp contrast to the ‘t Hooft large-N limit, where the expansion parameter is set by the ‘t Hooft coupling $`\lambda ^2`$.

In the $`𝒩=4`$ super Yang-Mills theory, operators with $`(\mathrm{\Delta }J)>0`$ are long supermultiplets, hence, correspond to massive string oscillator modes of Type IIB string theory. In the new limit Eq.(1), $`J\sqrt{N}`$ is large of order $`𝒪\left(1/\sqrt{g_\mathrm{s}}\right)`$ at weak string coupling limit. The limit Eq.(1) turns out to correspond in the Type IIB string theory to the so-called Penrose limit of the $`AdS_5\times S^5`$ background, yielding pp-wave spacetime with transverse $`𝐑^4\times 𝐑^4`$ geometry and homogeneous RR 5-form field strength . It amounts to boosting the background around a great circle in $`S^5`$ and rescaling so that a neighborhood around null geodesics is blown up. As such, the BMN limit of $`𝒩=4`$ super Yang-Mills theory is interpretable as gauge theory description for discrete light-cone quantization of Type IIB superstring. Interestingly, in the Penrose limit of $`AdS_5\times S^5`$, the total number of isometries as well as spacetime supersymmetries remain the same. Rather, the limit yields a contraction of the $`SU(2,2|4)`$ superconformal algebra (see  for an explicit demonstration).

A central technical feature that facilitates this correspondence is the phenomenon that anomalous dimensions of a certain class of long multiplet operators are parametrically suppressed. Relevance of this sort of operators to the string theory has been first emphasized by Polyakov . In the proposal of BMN, these operators play the prominent role in that they describe the creation and annihilation operators of string oscillation modes.

An immediate question is whether the proposal is applicable to a more nontrivial background of the pp-wave front. In this paper, we extend the BMN proposal to the simplest yet nontrivial situation: pp-wave orbifold — the homogeneous pp-wave background (part of) whose transverse space is orbifolded. Specifically, we will consider orbifolding one of the two $`𝐑^4`$ subspaces transverse to the propagation null vector. Our motivation comes from various corners. First, the plane-wave background considered by BMN preserves all 32 spacetime supersymmetries. It is clearly of interest to investigate if the BMN proposal is extendible to plane-wave backgrounds with fewer number of spacetime supersymmetries. The simplest way to reduce the supersymmetry is to orbifold part of the transverse space. Second, as shown in , the plane-wave background acts as a harmonic potential to the string, and hence dynamical distinction between untwisted and twisted states is less clear. It is thus of intrinsic interest to see if one can find a precise map between Type IIB string oscillation modes and quiver gauge theory operators, both for untwisted and twisted sectors.

This paper is organized as follows. In section 2, we study the discrete light-cone quantization of the Type IIB superstring on pp-wave orbifold, and obtain the energy spectrum. In section 3, we analyze gauge-invariant operators in the dual, $`𝒩=2`$ quiver gauge theory, and find precise correspondence with the spectrum obtained in section 2. In section 4, we compute perturbatively the anomalous dimension of $`(\mathrm{\Delta }J)=1`$ operators at leading order and find agreement with the light-cone energy spectrum of section 2.

Shortly after , several preprints with various generalizations have appeared . In particular, , which has substantial overlap with part of our work, was posted on the archive while we were in the process of writing up our results.

## 2 Type IIB Superstring on pp-wave Orbifold

Begin with dynamics of a Type IIB superstring on pp-wave background. The background, supported by homogeneous RR 5-form and dilaton fields, is given by

$`ds^2`$ $`=4dx^+dx^{}\mu ^2(\stackrel{}{x}^2+\stackrel{}{y}^2)(dx^+)^2+d\stackrel{}{x}^2+d\stackrel{}{y}^2,`$ (2)
$`F_{+1234}`$ $`=F_{+5678}=\mu ,`$ (3)
$`e^\varphi `$ $`g_s=\mathrm{constant},`$ (4)
where $`(\stackrel{}{x},\stackrel{}{y})𝐑^4\times 𝐑^4`$, and is known to be maximally supersymmetric, preserving all 32 spacetime supersymmetries. It was argued that, in the background Eqns.(2)–(4), the Type IIB superstring is exactly solvable , owing mainly to the fact that the light-cone worldsheet dynamics is described by free fields, albeit being massive.

Recently, it was found that the pp-wave background Eqns.(2)–(4) is related to the other known maximally supersymmetric background – $`AdS_5\times S^5`$ with RR 5-form flux threaded on the five-sphere – via the Penrose limit along a large circle of the $`S^5`$ . Note that the isometry group of the eight-dimensional space transverse to the null propagation direction is $`SO(4)\times SO(4)`$: while the spacetime geometry is invariant under $`SO(8)`$, the 5-form field strength breaks it to $`SO(4)\times SO(4)`$. In the Green-Schwarz action of the Type IIB string in the plane-wave background, the reduction of the isometry is due to the coupling of spinor fields to the background RR 5-form field strength.

One is interested in reducing the number of supersymmetries preserved by the background. As alluded to in the introduction, one can reduce the 32 supersymmetries to 16 supersymmetries by taking a $`𝐙_k`$ orbifold of the $`𝐑^4`$ subspace parametrized by $`\stackrel{}{y}`$. The orbifold action is defined by

$$g:(z^1,z^2)(\omega z^1,\omega z^2)\mathrm{where}\omega =e^{\frac{2\pi i}{k}}.$$
(5)
Here, $`z^1\frac{1}{\sqrt{2}}(y^6+iy^7)`$, $`z^2\frac{1}{\sqrt{2}}(y^8iy^9)`$. The orbifold action $`g`$ acts on spacetime fields as $`g=\mathrm{exp}\left(\frac{2\pi i}{k}(J_{67}J_{89})\right)`$, $`J_{67}`$ and $`J_{89}`$ being the rotation generators in the $`67`$ and $`89`$ planes, respectively. Defined so, the orbifold of the pp-wave background is actually derivable from the Penrose limit of $`AdS_5\times S^5/𝐙_k`$ taken along the great circle of the $`S^5`$ that is fixed by the orbifold.

In the light-cone gauge, Type IIB superstring on the pp-wave background Eqns.(2)–(4) is described by eight worldsheet scalars $`x^I`$ and eight worldsheet Majorana fermions $`(\theta _1,\theta _2)`$, all of which are free but massive. The masses of the scalars and the fermions are equal by worldsheet supersymmetry (which descends from the light-cone gauge fixing of the Green-Schwarz action) and equal the RR 5-form field strength, $`\mu `$. Both $`\theta _1,\theta _2`$ are positive chirality Majorana-Weyl spinors of $`SO(9,1)`$, obeying the light-cone gauge condition $`\mathrm{\Gamma }^+\theta _i=0`$. Decomposing the worldsheet fields into $`SO(4)_1\times SO(4)_2`$ subgroups,

$`x^I`$ $`=(\stackrel{}{x},\stackrel{}{y})(\stackrel{}{x},z^1,z^2),g:\stackrel{}{x}\stackrel{}{x},z^m\omega z^m,`$ (6)
$`\theta `$ $`{\displaystyle \frac{1}{\sqrt{2}}}(\theta _1+i\theta _2)(\chi ^\alpha ,\xi ^{\dot{\alpha }}),g:\chi ^\alpha \chi ^\alpha ,\xi ^{\dot{\alpha }}\mathrm{\Omega }_{}^{\dot{\alpha }}{}_{\dot{\beta }}{}^{}\xi ^{\dot{\beta }}.`$ (7)
Here, $`\alpha `$ and $`\dot{\alpha }`$ are spinor indices of $`SO(4)_2`$, ranging over 1,2. We have suppressed the spinor indices of $`SO(4)_1`$ under which $`\chi ^\alpha `$ carry positive chirality, while $`\xi ^{\dot{\alpha }}`$ carry negative one. $`\mathrm{\Omega }=\mathrm{diag}(\omega ,\omega ^1)`$, viz. $`\xi ^{\dot{1}}`$ and $`\xi ^{\dot{2}}`$ transform oppositely under the $`𝐙_k`$ orbifold action. It is convenient to combine $`\xi ^{\dot{1}},\overline{\xi }^{\dot{2}}`$ into a Dirac spinor $`\xi `$, and $`\overline{\xi }^{\dot{1}}`$ and $`\xi ^{\dot{2}}`$ into its conjugate $`\overline{\xi }`$ and analogously for $`\chi `$ and $`\overline{\chi }`$. As the worldsheet theory is free, it is straightforward to quantize the Type IIB superstring in each twisted sector, the only difference among various sectors being the monodromy of the worldsheet fields sensitive to the orbifolding, viz. $`z^1,z^2`$ and $`\xi `$. The other worldsheet fields remain periodic as usual. The monodromy conditions in the $`q`$-th twisted sector, $`q=0,\mathrm{},k1`$, are given by

$$z^m(\sigma +2\pi \alpha ^{}p^+,\tau )=\omega ^qz^m(\sigma ,\tau ),\xi (\sigma +2\pi \alpha ^{}p^+,\tau )=\omega ^q\xi (\sigma ,\tau ),$$
(8)
and result in fractional moding, $`n(q)=n+\frac{q}{k}`$ $`\left(n𝐙\right)`$ of the corresponding oscillator modes.

Physical states are obtainable by applying the bosonic and fermionic creation operators to the light-cone vacuum $`|0,p^+_q`$ of each $`q`$-th twisted sector. They ought to satisfy additional constraints ensuring the level-matching condition:

$$\underset{n𝐙}{}nN_n=0,\underset{n𝐙}{}n(q)\left(N_{n(q)}\overline{N}_{n(q)}\right)=\underset{n𝐙}{}\left(n(q)N_{n(q)}+n(q)\overline{N}_{n(q)}\right)=0,$$
(9)
and $`𝐙_k`$ invariance. The bosonic creation operators consist of

$$\stackrel{}{a}_n^{},\text{ and }\alpha _{n(q)}^m,\overline{\alpha }_{n(q)}^m\left(n𝐙\right).$$
(10)
Here, $`\stackrel{}{a}_n`$ are the $`\stackrel{}{x}`$ oscillators, whereas $`\alpha _{n(q)}^m`$ and $`\overline{\alpha }_{n(q)}^m`$ are $`z^m`$ and $`\overline{z}^m`$ oscillators, respectively. The fermionic creation operators consist, in obvious notation, of

$$\chi _n^{},\overline{\chi }_n^{}\text{ and }\xi _{n(q)}^{},\overline{\xi }_{n(q)}^{}.$$
(11)
Acting the fermionic zero mode oscillators to the light-cone vacua and projecting onto $`𝐙_k`$ invariant states, one fills out $`𝒩=2`$ gravity and tensor supermultiplets of the plane wave background. The action of the bosonic oscillators on these gives rise to a whole tower of multiplets, much as in the $`AdS_5\times S^5`$ case. As an example, we have four invariant states with a single bosonic oscillator

$$\stackrel{}{a}_0^{}|0,p^+_q,$$
(12)
and states with two bosonic oscillators are

$$a_n^\mu a_n^\nu |0,p^+_q,\alpha _{n(q)}^l\overline{\alpha }_{n(q)}^m|0,p^+_q.$$
(13)
In the $`𝐙_2`$ case there are additional invariant states built from two $`z^m`$ or two $`\overline{z}^m`$ oscillators. However, they do not satisfy the level matching condition, Eq.(9).

One straightforwardly obtains the light-cone Hamiltonian in the $`q`$-th twisted sector as

$$H_{\text{LC}}(q)=\underset{n𝐙}{}N_n\sqrt{\mu ^2+\frac{n^2}{(\alpha ^{}p^+)^2}}+\underset{n𝐙}{}\left(N_{n(q)}+\overline{N}_{n(q)}\right)\sqrt{\mu ^2+\frac{n(q)^2}{(\alpha ^{}p^+)^2}}.$$
(14)
The first sum is over those oscillators which are not sensitive to the orbifold. Positive modes label ‘left’ movers, negative ones ‘right’ movers, $`N_n`$ ($`N_{n(q)}`$ and $`\overline{N}_{n(q)}`$) is the total occupation number of bosons and fermions. The ground state energy is cancelled between bosons and fermions. This corresponds to a choice of fermionic zero mode vacuum that explicitly breaks the $`SO(8)`$ symmetry, which is respected by the metric but not the field strength background, to $`SO(4)_1\times SO(4)_2`$ .

## 3 Operator Analysis in $`𝒩=2`$ Quiver Gauge Theory

It is known  that Type IIB supergravity on $`AdS_5\times (S^5/𝐙_k)`$ is dual to $`𝒩=2`$ $`[U(N)]^k`$ quiver gauge theory, the worldvolume theory of $`kN`$ D3-branes sitting at the orbifold singularity. In light of discussions in the previous section, one anticipates that Type IIB superstring on pp-wave orbifold is dual to a new perturbative expansion of the quiver gauge theory at large $`N`$ and fixed gauge coupling $`g_{\text{YM}}^2=4\pi g_sk`$. The factor of $`k`$ in the relation between the string and the gauge coupling is standard, and is easily deducible from moving the D3-branes off the tip of the orbifold into the Higgs branch. See also . In the new expansion, one focuses primarily on states with conformal weight $`\mathrm{\Delta }`$ and $`U(1)_R`$ charge $`J`$ which scale as $`\mathrm{\Delta }`$, $`J\sqrt{N}`$, whose difference $`(\mathrm{\Delta }J)`$ remains finite in the large $`N`$ limit. $`U(1)_R`$ is the subgroup of the orginal $`SU(4)_R`$ symmetry of $`𝒩=4`$ super Yang-Mills theory, which on the gravity side corresponds to the $`S^1`$ fixed under the orbifolding; this $`U(1)_R`$ together with the $`SU(2)_1`$ subgroup of the remaining $`SO(4)SU(2)_1\times SU(2)_2`$ that commutes with $`𝐙_kSU(2)_2`$ forms the $`R`$-symmetry group of $`𝒩=2`$ supersymmetric gauge theory.

The reason for the above scaling behaviour is that $`(\mathrm{\Delta }J)`$ is identified with the light-cone Hamiltonian on the string theory side, whereas 111 Since $`_{S^5/𝐙_k}F_5=N`$, the radius of $`AdS_5`$ is proportional to $`(kN)^{1/4}`$. $`\frac{J}{\sqrt{kN}}p^+`$, $`p^+`$ being the longitudinal momentum carried by the string. When $`(\mathrm{\Delta }J)J`$, the light-cone Hamiltonian Eq.(14) implies that on the gauge theory side there are operators obeying the following relation between the dimension $`\mathrm{\Delta }`$ and the $`U(1)_R`$ charge $`J`$ (we set $`\mu 1`$)

$$(\mathrm{\Delta }J)_n=\sqrt{1+g_{\mathrm{eff}}^2n^2}\text{ and }(\mathrm{\Delta }J)_{n(q)}=\sqrt{1+g_{\mathrm{eff}}^2\left(n(q)\right)^2}.$$
(15)
In the gauge theory, before orbifolding we have $`N\times N`$ matrix valued fields, i.e. the gauge field $`A_\mu `$, complex scalars $`Z=\frac{1}{\sqrt{2}}(X^4+iX^5)`$ and $`\varphi ^m=(\varphi ^1,\varphi ^2)\frac{1}{\sqrt{2}}(X^6+iX^7,X^8iX^9)`$, and fermions $`\chi `$ and $`\xi `$. The fields $`\chi `$ and $`\xi `$ are spinors of $`SO(5,1)`$, transforming as $`\mathrm{𝟒}`$ and $`\mathrm{𝟒}^{}`$, respectively. For defining the $`𝐙_k`$ orbifolding in the gauge theory, we promote these fields to $`kN\times kN`$ matrices $`𝒜_\mu `$, $`𝒵`$, $`\mathrm{\Phi }^m`$, $`𝒳`$ and $`\mathrm{\Xi }`$ and project onto the $`𝐙_k`$ invariant components. The projection is ensured by the conditions

$$S𝒜_\mu S^1=𝒜_\mu ,S𝒵S^1=𝒵,S𝒳S^1=𝒳$$
(16)
and

$$S\mathrm{\Phi }^mS^1=\omega \mathrm{\Phi }^m,S\mathrm{\Xi }S^1=\omega \mathrm{\Xi }.$$
(17)
where $`S=\text{diag}(1,\omega ^1,\omega ^2,\mathrm{},\omega ^{k+1})`$, each block being proportional to the $`N\times N`$ unit matrix.

The resulting spectrum is that of a four-dimensional $`𝒩=2`$ quiver gauge theory  with $`[U(N)]^k`$ gauge group, containing hypermultiplets in the bi-fundamental representations of $`U(N)_i\times U(N)_{i+1}`$, $`i𝐙`$ mod$`(k)`$. More precisely, $`𝒜_\mu `$, $`𝒵`$ and $`𝒳`$ fill out $`k`$ $`𝒩=2`$ vector multiplets with the fermions transforming as doublets under $`SU(2)_R`$ (as its Cartan generator is proportional to $`(J_{67}+J_{89})`$). The $`𝒵`$ field has the block-diagonal form

$$𝒵=\left(\begin{array}{cccccc}Z_1& & & & & \\ & Z_2& & & & \\ & & Z_3& & & \\ & & & & & \\ & & & & & \\ & & & & & Z_k\end{array}\right)$$
(18)
with zeros on the off-diagonal and the diagonal blocks being $`N\times N`$ matrices of $`U(N)_i`$’s. The $`𝒜_\mu `$ and $`𝒳`$ fields take an analogous form. Likewise, the $`\mathrm{\Phi }^m`$ and $`\mathrm{\Xi }`$ fields fill out $`k`$ hypermultiplets, in which the scalars are doublets under $`SU(2)_R`$, whereas the fermions are neutral. The $`\mathrm{\Phi }^m`$ fields take the form

$$\mathrm{\Phi }^m=\left(\begin{array}{ccccccc}0& \varphi _{12}^m& & & & & \\ & 0& \varphi _{23}^m& & & & \\ & & 0& & & & \\ & & & & & & \\ & & & & & & \\ \varphi _{k1}^m& & & & & & \end{array}\right)$$
(19)
and analogously for $`\mathrm{\Xi }`$.

The light-cone vacua of the type IIB superstring in the plane-wave orbifold ought to be described by $`p^{}=0`$. In the quiver gauge theory side, the vacuum then corresponds to $`(\mathrm{\Delta }J)=0`$ operators acting on the Fock space vacuum. What are the operators satisfying $`(\mathrm{\Delta }J)=0`$? Obviously, one can build $`k`$ mutually orthogonal, $`𝐙_k`$ invariant single trace operators $`\text{Tr}[S^q𝒵^J]`$. We propose that these operators are associated to the vacuum in the $`q`$-th twisted sector

$$\frac{1}{\sqrt{kJ}N^{J/2}}\text{Tr}[S^q𝒵^J]|0,p^+_q,(q=0,\mathrm{},k1).$$
(20)
In what sense is this identification unique? After all, in the quiver gauge theory, it appears that the operators $`\text{Tr}[S^q𝒵^J]`$ for any $`q`$ stand on equal footing. However, the orbifold action renders an additional “quantum” $`𝐙_k`$ symmetry (see e.g. ) that acts on fields in the quiver gauge theory.222 This $`𝐙_k`$ should not to be confused with the spacetime $`𝐙_k`$ used for constructing the orbifold. By construction, under the orbifold action, all the fields are invariant. Specifically, one can take an element $`g`$ in this quantum $`𝐙_k`$, $`g=e^{\frac{2\pi i}{k}}`$, to act on an arbitrary field $`T_{ij}`$, $`i,j𝐙`$ mod$`(k)`$, as $`g:T_{ij}T_{i+1,j+1}`$. In particular, one notes that $`g:\text{Tr}[S^q𝒵^J]\omega ^q\text{Tr}[S^q𝒵^J]`$. So one can indeed distinguish classes of operators on the quiver gauge theory side by their eigenvalues under the quantum $`𝐙_k`$ symmetry.

Next, consider the eight twist invariant operators with $`(\mathrm{\Delta }J)=1`$. They are

$`{\displaystyle \frac{1}{kN^{(J+1)/2}}}\text{Tr}[S^q𝒵^J𝒟_\mu 𝒵]`$ $`a_0^\mu |0,p^+_q,`$ (21)
$`{\displaystyle \frac{1}{kN^{(J+1)/2}}}\text{Tr}[S^q𝒵^J𝒳_{J=1/2}]`$ $`\chi _0^{}|0,p^+_q,`$ (22)
$`{\displaystyle \frac{1}{kN^{(J+1)/2}}}\text{Tr}[S^q𝒵^J\overline{𝒳}_{J=1/2}]`$ $`\overline{\chi }_0^{}|0,p^+_q,`$ (23)
and hence identifiable with Type IIB supergravity modes (in each twisted sector) built out of a single zero-mode oscillator acting on the $`q`$-th vacuum. Here, $`𝒟_\mu 𝒵=_\mu 𝒵+[𝒜_\mu ,𝒵]`$ .

Operators corresponding to higher string states on the pp-wave orbifold arise as follows. Oscillators of non-zero level $`n`$ corresponding to the fields not sensitive to the orbifold are identified with insertions of the operators $`𝒟_\mu 𝒵`$, $`𝒳_{J=1/2}`$ and $`\overline{𝒳}_{J=1/2}`$ with a position dependent phase factor $`e^{\frac{2\pi il}{J}n}`$ in the trace $`\text{Tr}[S^q𝒵^J]`$. For instance, for $`(\mathrm{\Delta }J)=2`$,

$$\frac{1}{\sqrt{kJ}N^{J/2+1}}\underset{l=1}{\overset{J}{}}\text{Tr}[S^q𝒵^l𝒟_\mu 𝒵𝒵^{Jl}𝒟_\nu 𝒵]e^{\frac{2\pi il}{J}n}a_n^\mu a_n^\nu |0,p^+_q.$$
(24)
This is exactly the same as in the unorbifolded case – the insertion of the position-dependent phase factor ensures that the level-matching condition is satisfied and that the light-cone energy of the string states is reproduced correctly .

As for the remaining string states involving oscillators with a fractional moding $`n(q)`$ in the twisted sectors, we propose to identify them with insertions of the operators $`\mathrm{\Phi }^m`$ and $`\mathrm{\Xi }_{J=1/2}`$ together with the position-dependent phase factor $`e^{\frac{2\pi il}{J}n(q)}`$. Similarly, insertions of $`\overline{\mathrm{\Phi }}^m`$ and $`\overline{\mathrm{\Xi }}_{J=1/2}`$ are accompanied with the phase factor $`e^{\frac{2\pi il}{J}n(q)}`$. Again, the prescription implements the level-matching condition and, as will be demonstrated in the next section, seems to yield the correct energy of the corresponding string states. For instance,

$$\frac{1}{\sqrt{kJ}N^{J/2+1}}\underset{l=1}{\overset{J}{}}\text{Tr}[S^q𝒵^l\mathrm{\Phi }^r𝒵^{Jl}\overline{\mathrm{\Phi }}^s]e^{\frac{2\pi il}{J}n(q)}\alpha _{n(q)}^r\overline{\alpha }_{n(q)}^s|0,p^+_q.$$
(25)
Note that, for $`𝐙_2`$ orbifold, the state $`_{k,l=1}^J\text{Tr}[S𝒵^k\mathrm{\Phi }^r𝒵^l\mathrm{\Phi }^s𝒵^{Jkl}]e^{\frac{2\pi i}{J}(kn(1)+(k+l)m(1))}`$ corresponding to $`\alpha _{n(q)}^r\alpha _{m(q)}^s|0,p^+_1`$, though being $`𝐙_2`$ invariant, vanishes for all $`m,n`$ due to the cyclicity of the trace, as it should, cf. the remark below Eq.(13).

Finally, operators with insertions such as $`𝒟_\mu 𝒟_\nu 𝒵`$, $`\overline{𝒵}`$ or $`𝒳_{J=1/2}`$ in the trace are present at weak coupling, but should not be present at strong coupling, as there are no corresponding states in the string spectrum. As in , the reason for this might be related to the fact that these operators acquire a large anomalous dimension in this limit .

## 4 Anomalously Suppressed Anomalous Dimensions

In this section, in fixed $`g_{\mathrm{YM}}^2`$, large-$`N`$ and large-$`J`$ perturbation theory, we shall be computing leading-order anomalous dimensions of $`(\mathrm{\Delta }J)=1`$ operators in $`𝒩=2`$ quiver gauge theory, and confirm that our proposal for the twisted sector operators reproduces the correct light-cone string energy spectrum. Amusingly, in the set-up we have outlined above, one can proceed the computations essentially parallel to those of .

The bosonic part of the (euclidean) quiver gauge theory action involving the transverse scalars is given by

$`S_{\text{YM}}={\displaystyle \frac{2}{g_{\mathrm{YM}}^2}}{\displaystyle d^4x}`$ $`\text{Tr}\left[\right|𝒟𝒵|^2+{\displaystyle \underset{m=1}{\overset{2}{}}}|𝒟\mathrm{\Phi }^m|^2{\displaystyle \frac{1}{2}}\left(\right|[𝒵,\overline{𝒵}]|^2+{\displaystyle \underset{m=1}{\overset{2}{}}}|[\mathrm{\Phi }^m,\overline{\mathrm{\Phi }}^m]|^2`$
$`+{\displaystyle \underset{mn=1}{\overset{2}{}}}\left(\right|[\mathrm{\Phi }^m,\overline{\mathrm{\Phi }}^n]|^2+\left|[\mathrm{\Phi }^m,\mathrm{\Phi }^n]|^2\right)+2{\displaystyle \underset{m=1}{\overset{2}{}}}\left(\right|[𝒵,\mathrm{\Phi }^m]|^2+\left|[𝒵,\overline{\mathrm{\Phi }}^m]|^2\right))].`$ (26)
The trace ‘Tr’ runs over the $`kN\times kN`$ matrices, the $`N\times N`$ matrix blocks being invariant under the orbifold action.

Explicitly, the quartic interactions involving $`𝒵`$ with $`\mathrm{\Phi }^m`$ (the last two terms in Eq.(4)) are

$`{\displaystyle \underset{a=1}{\overset{k}{}}}{\displaystyle \underset{m=1}{\overset{2}{}}}{\displaystyle \frac{4}{g_{\mathrm{YM}}^2}}{\displaystyle d^4x\text{tr}\left[Z_a\varphi _{a,a+1}^m\overline{Z}_{a+1}\overline{\varphi }_{a+1,a}^m+Z_a\overline{\varphi }_{a,a1}^m\overline{Z}_{a1}\varphi _{a1,a}^m\right]}`$
$`+{\displaystyle \underset{a=1}{\overset{k}{}}}{\displaystyle \underset{m=1}{\overset{2}{}}}{\displaystyle \frac{2}{g_{\mathrm{YM}}^2}}{\displaystyle }d^4x\text{tr}[Z_a\varphi _{a,a+1}^m\overline{\varphi }_{a+1,a}^m\overline{Z}_a+Z_a\overline{\varphi }_{a,a1}^m\varphi _{a1,a}^m\overline{Z}_a`$
$`+\varphi _{a,a+1}^mZ_{a+1}\overline{Z}_{a+1}\overline{\varphi }_{a+1,a}^m+\overline{\varphi }_{a,a1}^mZ_{a1}\overline{Z}_{a1}\varphi _{a1,a}^m],`$ (27)
the trace ‘tr’ now being over $`N\times N`$ matrices of the $`a`$-th $`U(N)`$ group. The first line contains ‘momentum-dependent’ interactions, while the second and third line ‘momentum-independent’ interactions, respectively.

The free field propagators are

$$\left(Z_a\right)_i^j(x)\left(\overline{Z}_b\right)_k^l(0)=\delta _{ab}\delta _i^l\delta _k^j\frac{g_{\mathrm{YM}}^2}{8\pi ^2}\frac{1}{|x|^2},\left(\varphi _{a,a+1}^m\right)_i^j(x)\left(\overline{\varphi }_{b+1,b}^n\right)_k^l(0)=\delta _{ab}\delta ^{mn}\delta _i^l\delta _k^j\frac{g_{\mathrm{YM}}^2}{8\pi ^2}\frac{1}{|x|^2}.$$
(28)
If our proposed map between gauge theory operators and string modes is correct, according to Eq.(15), anomalous dimension of the operators $`O(x)`$ in Eq.(25) is expected to receive perturbative corrections as

$$(\mathrm{\Delta }J)_{n(q)}=1+\frac{1}{2}g_{\mathrm{eff}}^2(n(q))^2+\mathrm{}.$$
(29)
We now demonstrate that this is precisely what one finds. At leading-order in perturbation theory, the logarithmically divergent contribution to the two-point function from the ‘momentum dependent’ interactions is obtained as

$$O(x)O^{}(0)=\frac{\left(\frac{g_{\mathrm{YM}}^2}{8\pi ^2}\right)^\mathrm{\Delta }}{|x|^{2\mathrm{\Delta }}}[1+\frac{g_{\mathrm{YM}}^2N}{2\pi ^2}\mathrm{cos}\frac{2\pi n(q)}{J}\mathrm{ln}(|x|\mathrm{\Lambda }\left)\right],$$
(30)
whereas, for the ‘momentum-independent‘ interactions, $`\mathrm{cos}\frac{2\pi n(q)}{J}`$ is replaced by $`1`$. Other ‘momentum-independent’ interactions involving gauge bosons and scalar loops cancel, owing to the underlying $`𝒩=2`$ supersymmetry. Hence, at large $`J`$ and $`N`$, the leading-order perturbative correction to the two-point correlation function is, up to overall normalization factor,

$$O(x)O^{}(0)|x|^{2\mathrm{\Delta }}[1\frac{g_{\mathrm{YM}}^2N}{J^2}(n(q))^2\mathrm{ln}(|x|\mathrm{\Lambda }\left)\right].$$
(31)
This implies that

$`(\mathrm{\Delta }J)_{n(q)}=1+{\displaystyle \frac{1}{2}}{\displaystyle \frac{g_{\mathrm{YM}}^2N}{J^2}}\left(n(q)\right)^2+\mathrm{},`$ (32)
reproducing precisely the anticipated perturbative correction Eq.(29), and hence the requisite light-cone energy spectrum Eq.(14) in the $`q`$-th twisted sector. Resummation of the leading logarithms, corresponding to multiple insertions of the above quartic interactions, is straightforward, and reproduces the full square-root form in Eq.(15). Again, this closely parallels the computation of .

## Acknowledgement

We thank Gleb Arutyunov for discussions. NK and SJR acknowledge hospitality of the Isaac Newton Institute for Mathematical Sciences during this work. AP and ST acknowledge support from GIF, the German-Israeli foundation for Scientific Research. NK acknowledges support from DFG.