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Shaping Frequency Correlations of Ultrafast Pulse-pumped Modulational Instability

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**M. A. FINGER,1,* N. Y. JOLY,2,1 P. ST.J. RUSSELL ,1,2 AND M. V. CHEKHOVA1,2,3
**

1Max

Planck Institute for the Science of Light, and 2Department of Physics, University of Erlangen-Nuremberg, Guenther-Scharowsky Straße 1 /

Bau 24, 91058 Erlangen, Germany

3M. V. Lomonosov Moscow State University, 119899 Moscow, Russia

*Corresponding author: martin.finger@mpl.mpg.de

We vary the time-frequency mode structure of ultrafast pulse-pumped modulational instability (MI) in an argon-filled

hollow-core kagomé-style PCF by adjusting the pressure, pump pulse chirp, fiber length and parametric gain. Compared

to solid-core systems, the pressure dependent dispersion landscape brings increased flexibility to the tailoring of

frequency correlations. The resulting mode content is characterized by measuring the multimode second-order

correlation function g(2) and by directly observing frequency correlations in single-shot MI spectra. We show that, from

such measurements, the shapes and weights of time-frequency Schmidt (TFS) modes can be extracted and that the

number of modes directly influences the shot-to-shot pulse-energy and spectral-shape fluctuations in MI. Using this

approach we are able to change the number of TFS modes from 1.3 (g(2) = 1.75) to 4 (g(2) = 1.25) using only a single fiber.

OCIS codes: (190.4380) Nonlinear optics, four-wave mixing; (270.2500) Fluctuations, relaxations and noise; (190.7110) Ultrafast nonlinear optics;

(190.4370) Nonlinear optics, fibers.

**modes allow us to describe the generated quantum state in an effective,
**

low dimensional Hilbert space instead of using the whole frequency

continuum. The controlled generation, manipulation and detection of

such frequency modes is, despite many promising experiments, still a

challenging topic [11, 13], the optimal number of TFS modes being

dependent upon the application being considered.

If a bipartite system can be described with a single TFS mode pair,

the state is factorable in frequency. This means that there is no

frequency correlation between signal and idler photons. If one of the

two photons is detected, no information about the frequency of the

second photon can be extracted. At the same time, there can still exist

strong correlations in other degrees of freedom, for example in the

photon number for twin beams. In contrast, when the state consists of

many TFS modes, strong frequency correlations are observed. In terms

of applications, a moderate number of frequency modes is interesting

for increasing the security of quantum key distribution [15], which

requires a larger alphabet, or for enlarging the information capacity of

optical communication channels [16], while heralding single photons

and high interference contrast experiments require ideally single-TFSmode states [17, 18]. This shows that being able to design frequency

correlations is essential in all fields of quantum optics and also becomes

increasingly important in classical nonlinear optics.

Here we investigate the frequency correlations generated by

femtosecond pulse-pumped modulational instability (MI) in an argonfilled hollow-core photonic crystal fiber (PCF) at high gain. We study the

influence of various parameters such as fiber length and parametric

gain, focusing especially on the chirp of the input pulse and the pressure

of the filling gas. In previous work we showed that the spectral location

of the photon-number correlated MI sidebands can be tuned [19]. More

importantly, we show in this work that the modal frequency content is

tunable and can be precisely adjusted on demand. Generally, such a

system is interesting for quantum optics because it allows the

1. Introduction

The study of frequency correlations is an active research topic in both

classical and quantum optics. Since the advent of the dispersive Fourier

transform method, which allows single-shot spectral information to be

recorded at high repetition rates [1], there has been increasing interest

in investigating frequency correlations in the classical nonlinear optics

domain, e.g., in supercontinuum generation [2, 3] and in modulational

instability [4, 5]. This has applications in source development,

generation of random numbers [6] and can be used to study other

analogous nonlinear physical systems [4]. In quantum optics, one of the

most relevant fields for the study of frequency correlations is source

engineering. Controlling photon correlations in all degrees of freedom

(e.g., momentum, frequency, and polarization) is of fundamental

importance for biphoton and twin-beam sources. Depending on the

application, correlations between the emitted photons can be an

essential experimental resource, or an unwanted feature that corrupts

the performance. In general, spatial correlations can be removed using

waveguide sources, based either on crystals or on amorphous materials

such as glasses. Frequency correlations depend on the dispersion and

are difficult to modify in any system, so that special care must be taken

to eliminate them [7 – 9].

In the field of quantum optics, frequency correlations and

entanglement are usually discussed by introducing so-called timefrequency Schmidt (TFS) modes [10 – 13]. These are natural collective,

broadband frequency modes of bipartite systems and are a particular

example of the broader concept of coherent modes, which are used in

the description of partially coherent light sources [14]. The concept of

frequency modes is not restricted to the quantum domain but also holds

true for classical light fields and is helpful in the discussion of frequency

correlations, as we show in this paper.

Here, following the usual conventions, we call the two parts (photons

or beams) of the bipartite system signal and idler. The remarkable

feature of TFS modes is, that when signal and idler modes of twin beams

are properly selected, their photon numbers are perfectly correlated.

Since normally only a moderate number of these modes are excited, TFS

1

the joint spectral intensity (JSI = |JSA|2) can be measured by spectrally resolved coincidence counting [21] or by stimulated emission tomography [22]. it is instructive to look at the timeintegrated Hamiltonian describing the quantum state of biphotons and twin beams: Hˆ di ds F i . The chirp is controlled using a single-prism compressor [20]. Despite the equivalent description of the generated state. As pump we use 140 fs pulses from an amplified Ti:sapphire laser operating at 800 nm with a repetition rate of 125 kHz. PBS – Polarizing beam splitter. 1 shows the experimental set-up. the fiber needs to be pumped in normal dispersion for FWM and the phase matching is due to higher-order dispersion. exp i k s .1 nm BP (transform-limited pulse duration: 280 fs) in order to reduce the self-phase modulation broadening of the pump. where I s and I i are the intensities in the signal and idler beams. In the case of MI in a fiber with degenerate pump wavelengths. 2. (1) In this expression aˆ † (s . L the fiber length and Dk the phase mismatch. the JSI lacks phase information. The JSA is a complex-valued function and has not been directly accessed in any experiment so far. 1. After the compressor. Maya2000 PRO: Minimum integration time of 6 µs) in the single-shot regime. The pulse chirp is controlled using a singleprism pulse compressor. i . while the experiments with chirped pulses employ a 5 nm BP (transform-limited pulse duration: 240 fs). The quantum state produced through MI is similar to that generated by four-wave mixing (FWM). The pump spectral amplitude is assumed to be Gaussian and only linear phase mismatch is considered [7]. however. In order to understand how frequency correlations are generated and how they can be influenced.i ) are monochromatic-wave signal and idler photon creation operators and the joint spectral amplitude (JSA) F (i s ) describes the frequency correlations between them. the frequency correlations in a system are difficult to change because of the rigid dispersion landscape and the normally fixed pump wavelength. s aˆ † i aˆ † s h.000 fs2. we replace the spectrometer with a Fig. From this figure we see 2 . Alternatively. SP – Shortpass filter. This is to avoid saturation of the spectrometer. 2 2 where a (w ) is the spectral amplitude of the pump. It allows us to introduce a chirp of up to 40. HWP – Half-wave plate. Experimental setup and theoretical background We characterize the frequency mode structure with two methods. AC – Achromat. Instead. chirp-dependent frequency correlations. it still makes sense to distinguish the two processes due to their different macroscopic behavior. Generally. in that their dispersion depends on the gas type as well as the filling pressure.generation of tunable Raman-free photon-number correlated twin beams in a single spatial mode [19]. However. Kagomé-PCFs are much superior. based on a highly dispersive SF66 prism and a retroreflector [20]. Fig. The pulses are characterized using a commercial pulseCheck FROG from APE. The waveguide is a kagomé-style hollow-core PCF (kagomé-PCF) with a core diameter of 18. Fig. BP – Bandpass filter. while for MI the fiber is pumped in the anomalous dispersion regime and phase-matching is achieved with the help of the Kerr effect. the repetition rate of the laser is reduced from 125 kHz down to 80 Hz by means of a Pockels cell placed between two orthogonal polarizers. After the PCF the pump spectrum is suppressed in a 100 nm wide band using a shortpass filter at 750 nm and a longpass filter at 850 nm. we use a bandpass filter (BP) to reduce the input spectral width.c. s ) d s i L L (2) sinc k s . we study the spectral correlations of single-shot MI spectra and second. 2 shows a typical numerically calculated JSI for a gas-filled kagomé-PCF pumped at 800 nm. Experimental set-up for studying single-shot. First. photodiode to measure the pulse energy of the signal or idler and calculate g(2). we investigate the statistics of pulse-energy fluctuations with the normalized multimode second-order correlation function g (2) I s I i / I s I i . making it possible to tune the frequency correlations by changing the pressure.5 µm and a core wall thickness of 240 nm. LP – Longpass filter. the JSA is F (i . i . All experiments with unchirped pulses are carried out with a 3. In order to use the spectrometer (OceanOptics.

each one depending on just the signal or the idler frequency. One then obtains the correct Schmidt eigenvalues by taking the square-root of the calculated singular values because in the high-gain regime vn un . We can see that the mode shapes resemble Hermite-Gaussian functions. Here. the orientation of the JSA – and of spectral cross correlations in general – is connected to the number of TFS modes and gives a first indication of how many modes exist in the system. ∆k is the width and ∆φk is the tilt of the phase matching function. fewer modes are excited in the case of the red bars. 3(a) and the red bars to the nearly spatiotemporal single mode case of Fig. which is proportional to the fiber length. To our knowledge. covariance in terms of TFS modes (for the derivation. 3(a)) [23]. which is proportional to the coincidence rate in the case of two-photon light. Furthermore.34±0. its normalized (2) 2 . N (s . 2. see Supplement 1). the approximate modal shapes can now be found by making a singular value decomposition of the square-root of the covariance. This involves expressing the JSA as an expansion in terms of two sets of independent orthonormal modes n s and n i . un cosh G n .e. therefore. 6. Clearly. The effective number of modes K can be found from the Schmidt eigenvalues: Fig. ∆ωp is the spectral width of the pump. 3(b)). The underlying TFS mode structure can be revealed by carrying out a Schmidt decomposition of the JSA [10]. which n assumes that a single mode has thermal statistics. N j N i N j N i N j . This shows that. Fig. by taking the square-root of the measured covariance.37 (Fig.3 m. 3(c) and (d) show the shapes of the first three signal and idler TFS modes. We obtain very good agreement between the photodiode measurement of g(2) = 1. Determining TFS modes from joint measurements Instead of measuring the JSI.. n n are known as the Schmidt eigenvalues. n sinh G n . Fig. and G is the parametric gain. such a measurement gives much more information about the frequency mode structure than a standard g(2) measurement. i. At the same time. For this. Cov N s . which are the analytical solutions for a double-Gaussian JSA [12]. Figure 3 shows the TFS modes reconstructed for a fiber length of 0. since such fluctuations are transferred to the signal and idler and lead to an artificially increased g(2) value. Theoretical joint spectral intensity (JSI) of a gas-filled kagoméstyle photonic crystal fiber pumped in the MI regime at 800 nm.that the JSI is the product of two contributions. Moreover.i ) are the photon numbers at the signal and idler frequencies. g(2) directly from the shape of the covariance. left panel) and the value found by analyzing only the spectral correlations g(2) = 1. a pressure of 76 bar and an unchirped 280 fs pulse. where N (i . that the shape of the cross-correlation is independent of the pump laser fluctuations.03 (see also Fig. a natural way to quantify spectral cross-correlations at high gain (large photon numbers) is to record a set of single-shot spectra and calculate the covariance between the photon numbers registered at individual frequencies (Fig.s n n s n i . so that F i . the usual g(2) measurement requires a laser with relatively low pulse energy fluctuations. 6. 3(b) shows the distribution of the Schmidt eigenvalues (modal weights) for two cases. A certain system is called singlemode in frequency if the JSA can be written as a single product of some 0 s and 0 i modes. j ) is the photon number at frequency w i . right panel. j and the angle brackets denote averaging over different pulses. permitting reliable measurements of the frequency mode content even with fluctuating laser sources. The blue bars correspond to Fig. Nevertheless. In this way. namely the pump and the phase matching [21]. These relations can now be used to find correlation function is g sm factorable. this is the first experimental demonstration of the 3. we have direct access to the shapes of the TFS modes. nonlinearity and pump power. meaning in other words that the JSA is 1 (2) K n 2 . The covariance is defined as: Cov N i . The covariance is calculated from 2500 single-shot spectra. asymmetric losses lead to distortions of the mode shapes. We found that from such a measurement it is possible to calculate directly the shapes and weights of the TFS modes. N i vnunn* (s ) n (i ) 2 (3) n where n and n are the n-th TFS modes. K is also related to g(2) via g 1 1/ K . Another advantage of this method is. n are the Schmidt eigenvalues. we write the expression for the 3 . This method does not however give any information about the phase of the modes.

j 2 2 2 represents the variance of the photon numbers at the frequencies i . unlike in solid-core fibers. The red bars give the Schmidt eigenvalues for the case shown in the top righthand figure of Fig. Panels (c) and (d) show the first three TFS modes for the case of panel (a). 2). N j N i N j . resulting in a g(2) value of 1.40 to 1. Due to the fixed dispersion in all solid-core waveguides based on either ( 2) or (3) materials. which implies that the instantaneous frequency varies across the pulse. associated with a linear frequency up-chirp. 3. to be controlled. the frequency correlations can be modified.40 at 82 bar and 1. In particular. SPMbroadening of the pump is also affected by stronger Kerr nonlinearity at higher pressure. The tilt angle ∆φk of the phase-matching condition is the result of group velocity mismatch between signal. the pump in c (3) -based systems is always subject to spectral broadening induced by self-phase modulation (SPM). which must be considered for tailoring frequency correlations. it is possible to control the effective pump width ∆ωp in the fiber by prechirping the input pulse [24]. Cij is symmetric with respect to frequency. 0. showing that by changing only the pressure. This is caused by a temporally varying nonlinear phase. higher peak powers and stronger nonlinearity [23]. The measurements were taken in a 1. Due to the high peak power of the ultrafast pump pulses. In the following subsections we show how we can directly influence the spectral correlations by Fig.75 at 71 bar. The tilt of the cross-correlation distribution can be seen to change from 55° to 67°. 6 and gives g(2) = 1. We study the frequency cross-correlations of the generated sidebands by plotting the correlation coefficient Cij. Chirp tuning In ultrafast pulse-pumped systems. Ultrafast pulse-pumped systems therefore offer an additional degree of freedom for controlling 4 . as well as the spectral phasematching bandwidth. perfect anti-correlation. 76 bar and unchirped 280 fs pulses). The SPMinduced chirp adds to the initial chirp of the pump pulses.37. leading to the generation of new frequencies and spectral broadening. Pressure tuning Pressure tuning allows one to vary the balance between the normal dispersion of the gas against the weak anomalous geometrical dispersion of the waveguide and thus change the dispersion landscape [25] and consequently also the MI spectrum [19]. 2). since Cij takes values between ±1. SPM broadening is inherent to sources based on the Kerr-effect. 9]. As a result.5 m long fiber pumped with 390 fs pulses. control parameter. 4. A. +1 mean. which is the gas pressure. this effect can also be used to tune spectral correlations by varying the pump pulse chirp. 2. resulting in different pulseenergy fluctuations. Although usually considered disturbing. Therefore. At the same time. In contrast. (a) Square-root of the covariance in Eq. no correlation and perfect correlation.000 fs2. and thus the frequency correlations.3 m.77. idler and pump photons [7] and in the MI regime depends weakly on the peak power. gas-filled hollow-core PCF introduces an additional. Moreover. the most accessible parameters influencing frequency correlations in solid-core waveguides are the interaction length and the pump spectrum [21. SPM broadens the pulse spectrum ∆ωp during propagation and becomes stronger when the initial bandwidth of the pump pulses is increased. Fig. respectively. 3) and has the advantage that the strength of the correlations can be directly seen and easily interpreted. as well as for longer propagation lengths. and the usual difficulties with changing the pump wavelength. B. pumped with 390 fs long pulses (up-chirped with 29. 4 illustrates the effect on the frequency cross-correlations of changing the pressure from 82 to 71 bar. (b) Schmidt eigenvalues for the case shown in panel (a) (blue bars). changing such parameters also influences the spectral bandwidth of the phase-matching ∆k (Fig. while an upchirp increases the spectral broadening. Pressure-dependent change of the frequency cross-correlations in a 1. SPM broadening is. Shaping spectral correlations In solid-core and hollow-core fibers. 4. Cij = – 1. which had a chirp of 29. so that Cij = Cji (see Supplement 1). the spectral correlations can be changed by modifying either the pump spectrum or the phase matching condition (Fig. quantified by a change in g(2) from 1. easy to handle. In the time domain.5 m long PCF. are functions of the gas pressure. A down-chirp of the pump pulses compensates for the SPM and leads to a narrower pump. The g(2) correlation is 1. changing the pressure and how the pump pulse chirp allows the SPM broadening. to a good approximation.(3) (parameters: 0. j .000 fs2). where N i . This is a normalized version of the covariance used above (preceding Eq.intriguing link between frequency correlations and intensity fluctuations in MI. Fig. the tilt angle ∆φk of the phase-matching condition in Fig. It reduces with increasing length and peak power due to the power-dependent spectral shift of the MI sidebands.75. The correlation coefficient is defined as Cij Cov N i .

we investigate how the number of TFS modes influences the shot-to-shot spectra and the pulse-energy fluctuations and demonstrate that the number of TFS modes is not a constant but depends on the gain in the system. Bottom right: Distorted correlation for a strongly SPMstructured pump. the drop in g(2) for chirp values below 25. Bottom left: Cross-correlation when the pump spectrum exhibits only a single peak. a strongly SPMbroadened pump leads to distortion and splitting of the crosscorrelation signal.the spectral width ∆ωp. which can be imprinted on the JSA. Further. which can be understood from Fig.5 m long PCF at 71 bar. The dashed rectangle marks the residual pump (P) signal.3 (g(2) = 1. 5(b) the number of frequency modes increases with increasing chirp. although strong SPM broadening leads to spectral oscillations. Spatiotemporal few-mode source In this section we show that. Furthermore. 5. 2. The increasing content of uncorrelated pump light in the measurement range leads to a strong reduction in g(2). where a narrower pump leads to stronger frequency correlations and increases the number of TFS modes.5 m long PCF filled with 76 bar argon. varying the pump chirp allows the effective number of TFS modes in ultrafast pulse pumped systems to be continuously tuned. Fig. the number of TFS modes can be changed from 1. pumped with down-chirped (29. (a) Top: Chirp-dependent spectral evolution of the pump power spectral density (PSD) after propagation along 1. Comparing the measured cross-correlations. A.75) to 4 (g(2) = 1.000 fs2) 390 fs pulses. As we see in Fig. which directly influences the frequency correlations. normally unavoidable. it may be seen that the frequencies are strongly anti-correlated in the 5 . 5. 6 compares the cross-correlations generated in two different configurations. the gas-filling pressure and the chirp of the input pulse the MI frequency correlations can be shaped. Fig.4 and ~1.000 fs2 can be explained by the overlap of the broadening pump spectrum with the detection bandwidth of the signal. bottom left). 5(b). This means that in Fig. this can be side-stepped by appropriately pre-chirping the pump pulses. In Fig. SPM. In this way. filled with 76 bar argon and pumped with unchirped 280 fs pulses.5 m PCF at 76 bar. using the methods above.6. chirping the input pulse allows one to obtain clean frequency correlations even in systems with strong. 5(a) we see that with increasing chirp we can compensate for SPM broadening in the fiber. The chirp has the advantages of being continuously tunable and avoiding losses due to truncating the pulse spectrum. by changing the kagomé-PCF length. we obtain a clean cross-correlation signal (Fig. However. The exact functional form of the reduction depends on the orientation of the cross-correlation signal. In conclusion. Fig. The first system is a 30 cm long PCF. Here we investigate the influence of pulse chirp on the frequency cross-correlation in a 1. As we have seen in Section 3. The chirp-dependent pump width after the fiber clearly resembles the g(2) curve. In this way. 5(b) shows that the auto-correlation function g(2) of the signal decreases with increasing chirp. 5(a) (bottom right). we can avoid the characteristic splitting of the pump due to the oscillations in the SPM spectrum.25) with a single fiber. in the figure it varies between ~1. the effective number of TFS modes K is related to g(2) by the relation K 1/ ( g (2) 1) . 5(a). Influence of TFS mode number on shot-to-shot fluctuations As we have seen. From the top panel of Fig. (b) Spectral width of the pump after the fiber at 1/e2 of the pump amplitude and second-order auto-correlation function g(2) of the signal intensity for varying chirp values. if we chirp the input pulse more strongly so that the pump maintains a single-peak spectrum. The second system is a 1.

it is beneficial to excite a large number of TFS modes. Secondary nonlinear processes lead to a decrease in g(2) above a certain value of gain. 76 bar. for g(2) = 1. Right column: 1. We observe good agreement between the integrated spectrometer and the photodiode measurements as can be seen in Fig. which change from 1. which is the result of the superposition of differently populated. 28]. Fig. with corresponding Schmidt eigenvalue n . 71 bar. 390 fs pulses chirped with 29. To this end we numerically filtered out a narrow spectral band (4 nm) from the singleshot spectra (so as to obtain a single frequency mode) and calculated g(2) from it.case of the 30 cm long fiber. 13]: N n sinh 2 G n (4) where N n is the number of photons in the n-th mode. This can be interpreted as a gain-dependent redistribution of the normalized Schmidt eigenvalues. Consequently. with a corresponding increase in g(2). We can see that the curve approaches 2 at moderate gain values. Indeed. Figure 7(a) shows gain-dependent measurements of g(2) for three different parameter sets: (I) 0. Gain-dependent number of TFS modes Finally.3 m. unchirped 280 fs pulses (3.5 m. This effect. The shape of the spectra fluctuates from shot to shot for g(2) = 1. while the dark cyan markers are retrieved Fig. by examining the gain-dependent spectral evolution of the sidebands (Fig. unchirped 280 fs pulses The strong frequency correlations lead to shot-to-shot fluctuations in spectral shape. this theory predicts that every system collapses to a single frequency mode when the gain is high enough.1 nm BP).000 fs2).75 the shape of the spectra remains quite constant while its amplitude fluctuates—an indication that a single mode is predominantly populated. unchirped 280 fs pulses. secondary sidebands form through pairwise escape of photons from the signal sideband. 390 fs pulses (downchirped with 29. the influence of the reduced number of TFS modes on the single-shot spectra is clearly visible when comparing the bottom row of images of Fig. Consequently. they start to spectrally overlap with the main sidebands. (a) Dependence of the g(2) for the signal beam on the pump power. Since the number of modes derived from the g(2) measurement is equal to the product of the numbers of spatial and temporal modes. and (III) 1. suggesting that the single-mode statistics change at high values of gain. 76 bar. if the aim in a classical system is to reduce the shot-to-shot power fluctuations due to MI. This state also supports an exceptionally broad spectral width of 20 THz (FWHM) at 720 nm for the signal. 76 bar. The difference in correlations is also reflected in the measured g(2) values. 7(a)). as the gain increases (Fig. eventually resulting in the whole spectrum broadening to a supercontinuum. At this point spectral correlations vanish almost completely (see Supplement 1). In contrast. lower-order modes. This confirms that the system is spatially single-mode. we observe that the reduction in g(2) begins when the secondary sidebands appear.000 fs2. Left column: 0. g(2) can be used to work out the number of spatial modes in the system.3 m. Influence of frequency correlations on spectral fluctuations in single-shot spectra. The 6 . 7(a). 7(b)). we observe a reduction in the number of modes. 6. The intrinsic pulse-energy fluctuations arise from the noise-seeded nature of the MI light and have thermal statistics (g(2) = 2) in the single-mode case. by integrating single-shot spectral measurements and examining the fluctuations.5 m. 7. The nearly single-mode frequency state leads to a constant spectral shape from shot to shot. However. Moreover. which have larger eigenvalues (compare Fig. but cannot reach a value of g(2) = 2 by just increasing the power because two-photon absorption reduces g(2).34. while becoming damped for multimode light. meaning that there are higher pulseenergy fluctuations in the more factorable state. B. 3(b)). 6. get more strongly amplified with increasing gain than higher-order modes. The resulting curve is marked “filtered” in Fig. This figure illustrates neatly the applicability of the TFS mode picture to classical systems. 71 bar. In the end. while they are asymmetric and almost factorable for the 1. 7. comparing trace (II) with the dark cyan “unfiltered” curve. The black markers are measured with a photodiode.5 m long fiber. Subsequently. we made a direct (unfiltered) measurement of g(2) as a function of pump power. (II) 1 m. This can be explained by two-photon loss of the signal in the fiber: at high gain. The increase in g(2) with pump power is due to gain-dependent redistribution of the Schmidt eigenvalues. for higher gain even the filtered g(2) decreases. Therefore. independent spectral modes. which resembles a two-photon absorber.34 to the nearly single-mode state of 1.75. is known to suppress intensity fluctuations and can even lead to sub-Poissonian statistics [27. The same reasoning also explains the higher pulse-energy fluctuations in the case of fewer TFS modes. Theory predicts that the number of photons per mode scales with the parametric gain G [26.

A. Walmsley. O. 14931 (2015). U’Ren. Tikhonova and M. P. Sipe and V. 7507 (2012). Express 20. Larger. California. P. Eberly. A. Larger. Bourennane. Lacourt. This method can be extended to reconstructing the shapes and weights of coherent temporal and spatial modes in classical partially coherent radiation. Opt. Nonlinear fiber optics 3rd ed. Pérez. Law. Cao. Sh.-J. T. M. Opt. Nature Photon. 1096 (2016). 030302 (2014). P. Lett. Goda and B. 7. J. O. S. 2922 (2010). A. 11143 (2012). Eckstein. Suche. Cerf. V. L. something that is impossible in solid-core waveguide because of the rigid dispersion landscape. N. Spasibko. 82. 123603 (2009). T. A. R. 1881 (2014). A. Liu. H. Lorenz. Y. 5. Lett. M. V. L. Rev. J. 116. Cassemiro and C. M. V. T. 14870 (2007). Phys. G. Hölzer. In: Frontiers of Non-equilibrium Statistical Physics. (II) 1 m. Willner. Rev. Sci. G. Opt. Rev. J. Dudley. M. Blow. in contrast to g(2) measurements. D. Kudlinski. 280 fs pulses. 143602 (2015) 20. N. 76 bar. See Supplement 1 for supporting content. Joly. Y. A. 7 . K. Instrum. R. Ahmed. Mosley and C. Phys. Phys. yield more information on the time-frequency mode structure. Nature Photon. Express 20. G. V. Phys. S. (III) 1. Wang. M. Mosley and I. K. S. B. 7. A. 22. Alfano and A. St. L. B. Laiho. 71 bar. N. (b) Spectral evolution of (III) when the gain (G) is increased from 8 to 15. Lerouge. Christ. Phys. A. 10. A. Wetzel. 013603 (2011). K. Dinev. Bartley. Sansoni and C. P. Rev. The red arrow marks the gain value of the red trace in Fig. Genty. 12. W. Rep. P. A. Krasiński and S. Cohen. Silberhorn. Sylvestre. Iskhakov. Liscidini. Opt. McGuinness. E. Mussot. Sharapova. F. 033027 (2011). Mandel and E. Scharrer and P. X. Radic. A. Direct (unfiltered) g(2) measurements confirm that. Optica 1. 76 bar. Harder. 24. edited by G. Lett. Silberhorn. Kimmel. and I. allowing observation of the connection between spectral correlations and single-shot fluctuations of MI spectral shape. Y. J. Ben Salem. G. Chekhova. 143601 (2016). Zghal. M. Gu. Walmsley and J. Quiquempois and A. E. 127902 (2002). A. B.dark cyan curve is calculated from single-shot spectra. A. Xie. K. Agrawal. B. Y. M. Opt. Tuning the chirp of ultrafast pump pulses allows the effective number of TFS modes in Kerr-effect based systems to be precisely adjusted without introducing losses and distortions through truncating the pump spectrum. Migdall and S. Genty. Chekhova and P. 106. 115. T. G. Iskhakov and M. 19. while the black dots are measured with a photodiode. 2. Dudley. Wetzel. Lavery. B. M. 102. J. J. Cohen. Opt. Wetzel. A. Dias and J. 8. Mahou. A. K. A unique feature of kagomé-PCF is its flexibility in tuning spectral correlations by changing the pressure or the filling gas. Gerrits and C. 18. Rev. Wong. The red trace marks the spectrum above which there is decrease in g(2) with increasing gain. Rev. 28. K. Bigot. Y. Liu. Silberhorn. Akturk. B. Lett. Sci. REFERENCES 1. J. 2001). K. 281 (2014) 23. (I) 0. Finger. This simplifies source engineering and brings increased freedom to the experimental modification of spectral correlations. R. G. Kudlinski. These studies contribute to the understanding and tailoring of frequency correlations. Commun. New J. Guo. Walmsley. Lundeen. S. Rev. Puentes. Opt. Photon statistics. Phys. 84. P. M. A. A. Podlipensky. P. 18. G. Mussot. Bigourd. Douay.3m. R. 16. Y. Leuchs. Opt. Sylvestre. Milione. Eckstein. M. Largerand J. (Academic Press. Walmsley. S. K. Chekhova. I. 424 (1976). A. G. Rev. Express 14. D. A. Optical coherence and quantum optics (Cambridge University Press. 26. S. H. Y. Express 21. Lett. A. Scully (Plenum Press. 23589 (2009). L. Cohen. J. A. C. Gisin. Tur. N. Russell. E. 1986). Russell. Trebino. 14. the number of TFS modes in a system is not a constant but depends on the gain. 6. Phys. which. Nazarkin. 13. 88. S. A. P. Stefani. O. Huang. 102 (2013). 17. Christ. O. Dias and J. Merolla. 6. Godin. antibunching and squeezed states. 3. The shapes and weights of TFS modes can be retrieved from photon-number covariance measurements. Nam. Express 22. Ou. Eckstein. 11. Karlsson and N. B. Rangel-Rojo. X. 071101 (2011). Yang. G. 043816 (2015). L. Herink. J. N. D. M. 463 (2012). Rep. Cambridge. Ren. Wong. Polyakov. F. Li and Z. Brecht. 39. Li. X. 27. W. Phys. G. A 91. Quiring. Smith. 5. 390 fs pulses chirped with 29. K. M. Lundeen. J. Wolf. enabling experimental verification of theoretical predictions about TFS modes in the high-gain regime. K. Fang.5 m. San Diego. “Filtered” refers to numerical truncation to a 4 nm band. Nguyen. 1995). Nolan. J. M. Opt. G. V. New York. B. promising more stable supercontinuum generation or tunable physical random number generators. V. 15. 5304 (2000). Smith. A. R. J. K. St. J. Ricken. Sh. 280 fs pulses. 882 (2012). J. Conclusion Bright twin-beams with a tunable frequency mode content can be produced by modulational instability in gas-filled hollow-core kagoméPCF. Turitsyn. Dudley. Phys. Garay-Palmett. L. Solli. McKinstrie. Opt. M. J. Jalali and C. O. H.J. A. G. A 90. B. Mussot. Eisaman. (b).000 fs2.J. Lett. A. 13. Silberhorn. M. X. 18452 (2013). 4. T. Rev. Raymer. 25. United Kingdom. M. R. J. 6. 21. Kudlinski. T. T. 9. L. M. Millot. Nold. Fan. O. Express 24. 10101 (2006). Ropers. Cohen. Lett. 35. J. Yu. Lita. Jalali. A. O. Sci. 2. H. T. in accordance with theory. Lett. M. D. Lundeen and I. C. Express 17. which is already of high importance for applications in quantum optics and will become also increasingly important in classical nonlinear optics. A. J. A. Moore and M.

ACS. Germany 3M. and idler beams.I – Auto-correlation signal or idler.* N. Y. Comparison to simulation Fig. 91058 Erlangen.2. In all other figures we will concentrate only on the cross-correlation signal (CC). Looking at the crosscorrelation. V. V. RUSSELL . because of the limited dynamic range of the spectrometer. and derive the spectral covariance in terms of time-frequency Schmidt modes.J.1. Power-dependent spectral correlations Fig. One can see that the simulation and experiment are in very good agreement. which is the sensitivity limit of the silicon chip in the spectrometer. The system studied is a 1 m . FINGER. The measured spectra are a bit narrower than the simulated ones. which is marked as region of interest (ROI) in Fig. we can only see the sidebands appearing at rather high gain values (G = 11. signal. University of Erlangen-Nuremberg. Consequently. P – Pump.1 P. Lomonosov Moscow State University. Due to the symmetry of the correlation coefficient we can also see the mirror image of the cross-correlation signal (CCM). Here. JOLY.1 and higher). S1. since it leads to the saturation of the spectrometer. 2. S2 shows the power dependent evolution of the frequency correlations. A. Russia *Corresponding author: martin. we can clearly notice the frequency anti-correlation between the signal and idler beams. 119899 Moscow. and 2Department of Physics.de This document provides supplementary information to “Shaping frequency correlations of ultrafast-pulse pumped modulational instability in gas-filled hollow core PCF”.3 1Max Planck Institute for the Science of Light. S1. with Cij calculated for the complete spectrum. we did not filter out the pump light. CHEKHOVA1. We present additional information on the comparison between the experimental frequency cross-correlation and the nonlinear pulse propagation simulation.mpg. ROI – Region of interest. CCM – Mirrored cross-correlation. show the powerdependent evolution of the spectral correlations of the pump.2 AND M. corresponding to ~1050 nm. corresponding to the CC signal. meaning that the low idler frequencies are correlated with the high signal frequencies. The pump (P) is filtered out in the experiment. On the signal side this is a result of the smaller dynamic range. 1. pumped with unchirped 300 fs pulses with an energy of 220 nJ.1.finger@mpl. In all other figures in the paper we show only the ROI. Correlation coefficient for a 30 cm long PCF filled with 76 bar Ar gas.03) and the actual measurement. S1 shows the comparison between the generalized nonlinear Schrödinger equation simulation with the fiber dispersion taken from [1] (s-parameter = 0. Fig. whereas on the idler side the spectrum gets cut at around 286 THz. ST. CC – Cross-correlation. Guenther-Scharowsky Straße 1 / Bau 24.Shaping frequency correlations of ultrafast-pulse pumped modulational instability in gas-filled hollowcore PCF: supplementary material M.2.

Fig.8. The figure corresponds to curve (II) in Fig. [aˆn . It can be see how correlated MI sidebands appear and lose their correlation again at high pump powers. bˆm† ] nm . Also. These modes are orthogonal. except the trivial autocorrelations.1 nm bandpass filter). (S4) where Eˆ s ( ) (s ) aˆn†n (s ). * n for the respective Schmidt modes. defined as 3. The diagonal stripes seen in the top-row figures are caused by the electronic noise of the spectrometer. This is due to the overlap of the sidebands with the pump. where aˆ † (s ) and bˆ† (i ) are the standard monochromatic-wave photon creation operators. The two-mode Hamiltonian is now of the form (S3) where n n is the interaction strength. Here. For the broadband operators the usual commutation relations hold. so that () * n ( )d nm and ( )d nm . the Bogoliubov transformations (input-output equations) always couple the TFS modes pairwise. almost all correlations. aˆm† ] nm .0 and getting stronger at G = 12. G being the coupling strength for the whole amplifier and n are initial “two-photon” Schmidt eigenvalues. sinh G . It is known that the Schmidt modes form a basis for which the Hamiltonian is diagonal [3]. In the first two panels of the top row (G = 9. aˆn un aˆn 0 vn bˆn†0 .1 the MI sidebands appear. [bˆn . long kagomé-PCF filled with 76 bar argon gas and pumped with unchirped 280 fs long pulses (3. Gain (pump power) dependence of the whole spectrum including the pump in a 1 m long PCF filled with 76 bar argon.4. Eˆ i ( ) (i ) bˆn† n (i ). For a parametric amplifier. and [aˆn . S1. n 0 m () (S1) dt cosh G . bˆn un bˆn 0 vn aˆn†0 . This measurement corresponds to curve (II) in Fig. We express the negative-frequency field operators for signal and idler as a series expansion in terms of TFS modes. 10. un cosh n0 vn 2 n n n (S5) . 7(a). With increasing pump power. This description is valid for parametric down-conversion and four-wave mixing processes without pump depletion. The characteristic shape arises from spectral jittering due to the fluctuations of the pump power [2]. n and n are the TFS modes of the signal and idler. which cannot be seen in the figure because it is outside the dynamic range of this measurement. This corresponds to the case where a broad supercontinuum is generated. It can be identified as the anticorrelation (dark blue) areas. are lost when the gain is further increased. we see that the SPM loses its correlation. aˆ n† and bˆn† are photon creation operators (S2) bˆn† d i bˆ† (i ) n (i ). Their cross-correlation shape is distorted due to strong SPM in the system (compare Fig. At G = 11. Derivation of the covariance for a twin-beam parametric amplifier in terms of TFS modes We describe a spectrally multimode twin-beam parametric amplifier and derive its non-normalized second-order correlation function and covariance in terms of time-frequency Schmidt (TFS) modes. 5(a)). we can observe pump depletion starting at G = 12. 7(a). Finally. m aˆn† d s aˆ † (s )n (s ).3) one can only see the SPM broadened pump. bˆm† ] 0 .

i ) calculate the mean photon number in the signal channel v u * n n n n N (s ) Eˆ s ( ) (s ) Eˆ s ( ) (s ) n. C. i ) 2 n Substituting the fields leads to vnunn* (s ) n (i ) vn 2vm 2 n (s ) m (i ) . Opt. Law. Larger. (S10) From this. M. T. Finger. Opt. Express 21. 2 2 (S8) n. Russell. Rev. Zghal. it is clear that the covariance has to be positive and the shape of the TFS modes can be accessed by measuring the photon number covariance. I. we are now calculating the cross-correlation function Gsi(2) (s . G dt(t ) is the parametric gain. Sylvestre. Ben Salem. A. Weiss and P.m This can be transformed to the final form : 3 . which is not considered here. Kudlinski. H. (S7) References 1. Lett 84. In the next step. M. 2. M.Here. T. 3. i ) Eˆ s ( ) (s ) Eˆ i ( ) (i ) Eˆ s ( ) (s ) Eˆ i ( ) (i ) v u * n n n 2 (s ) n (i ) . St. 39. 821 (2014). n N( )i expression for the covariance reads: vn 2 n (s ) . G. Eberly. Y. A. A. A. Dudley. Dias and J. 18452 (2013). T. Mussot. From this. Lett. Wetzel. L. N( i)) Gsi(2) N( s) (S6) .k 0 The covariance at high photon numbers expressed in terms of Gsi(2) aˆn† aˆk n* (s )k (s ) is Cov( N( s). Genty. N i n and similar for the idler. Joly. The measured negativity in Fig. A. Walmsley and J. Godin. Gsi(2) (s . S2 is related to pump depletion. 5304 (2000).J. F. so that the final 2 Cov N s . (S9) 2 (s ) n (i ) N (s ) N (i ) . we can Gsi(2) (s . N. B. K. Phys.

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