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Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse

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 New Journal of Physics The open–access journal for physics

Coherent strong-field control of multiple states

by a single chirped femtosecond laser pulse
M Krug1 , T Bayer1 , M Wollenhaupt1 , C Sarpe-Tudoran1 ,
T Baumert1,4 , S S Ivanov2 and N V Vitanov2,3,4
1
Universität Kassel, Institut für Physik und CINSaT, Heinrich-Plett-Strasse 40,
D-34132 Kassel, Germany
2
Department of Physics, Sofia University, James Bourchier 5 blvd, 1164 Sofia,
Bulgaria
3
Institute of Solid State Physics, Bulgarian Academy of Sciences,
Tsarigradsko chaussée 72, 1784 Sofia, Bulgaria
E-mail: [email protected], [email protected] and
[email protected]

New Journal of Physics 11 (2009) 105051 (17pp)

Received 8 May 2009
Published 30 October 2009
Online at http://www.njp.org/
doi:10.1088/1367-2630/11/10/105051

Abstract. We present a joint experimental and theoretical study on strong-

field photo-ionization of sodium atoms using chirped femtosecond laser pulses.
By tuning the chirp parameter, selectivity among the population in the highly
excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways
enabling control are identified by simultaneous ionization and measurement
of photoelectron angular distributions employing the velocity map imaging
technique. Free electron wave packets at an energy of around 1 eV are observed.
These photoelectrons originate from two channels. The predominant 2 + 1 + 1
resonance enhanced multi-photon ionization (REMPI) proceeds via the strongly
driven two-photon transition 4s ←← 3s, and subsequent ionization from the
states 5p, 6p and 7p whereas the second pathway involves 3 + 1 REMPI via the
states 5f and 6f. In addition, electron wave packets from two-photon ionization
of the non-resonant transiently populated state 3p are observed close to the
ionization threshold. A mainly qualitative five-state model for the predominant
excitation channel is studied theoretically to provide insights into the physical
mechanisms at play. Our analysis shows that by tuning the chirp parameter the
dynamics is effectively controlled by dynamic Stark shifts and level crossings. In
particular, we show that under the experimental conditions the passage through
4
Authors to whom any correspondence should be addressed.

New Journal of Physics 11 (2009) 105051

1367-2630/09/105051+17$30.00 © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft
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an uncommon three-state ‘bow-tie’ level crossing allows the preparation of
coherent superposition states.
Contents

1. Introduction 2
2. Experiment 3
2.1. Excitation scheme . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.2. Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
3. Experimental results and discussion 6
4. Theoretical model 10
4.1. Excitation regimes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
4.2. Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
5. Summary and conclusion 14
Acknowledgments 15
Appendix. Details of calculations 15
References 16

1. Introduction

Selective excitation of preselected target states making use of shaped femtosecond laser pulses
is at the heart of coherent quantum control [1]–[10]. Closed-loop optimization strategies [4],
[11]–[15] have proven to be enormously successful in controlling a huge variety of quantum
systems; however, studies on model systems employing defined pulse shapes are the key to
better understand the underlying physical mechanisms and to further develop quantum control
concepts and techniques. This applies in particular to strong-field quantum control [16]–[20]
characterized by non-perturbative interaction of a quantum system with intense-shaped
laser pulses. Strong-field physical mechanisms involve—besides the interference of multiple
excitation pathways—adiabatic and non-adiabatic time evolution accompanied by dynamic
Stark shifts (DSSs) in the order of hundreds of meV. The latter is responsible for modification
of the atomic states or molecular potential surfaces [21]–[23] such that new pathways become
available and new target states—inaccessible in weak laser fields—open up. Recent studies of
strong-field control on model systems devoted to the analysis of the basic physical mechanisms
revealed that the concept of selective population of dressed states (SPODS) [24] provides
a natural description of controlled dynamics in intense-shaped laser fields. For example, it
was shown that ultrafast switching among different target channels by phase discontinuities
within the pulse [16], [24]–[26], rapid adiabatic passage (RAP) by chirped pulses [27] and
combinations thereof [28] are realizations of this general concept.
Chirped pulses are a well-established tool in quantum control because they usually serve
as a prototype for shaped pulses with controllable envelope and time-varying instantaneous
frequency. Therefore, they have played a prominent role in the development of quantum control
concepts and techniques and are still the ‘workhorse’ to test novel strategies in quantum control.
Examples of quantum control with chirped pulses comprise studies of selective excitation and
ionization of a multilevel system in alkali atoms [19, 27], [29]–[34], control of molecular
dynamics in diatomics and dyes [35]–[41], ([42] and references therein), measurement of
coherent transients [43] and the development of adiabatic passage techniques [44].

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In the present contribution, we employ chirped ultrashort laser pulses resulting from
phase modulation of the laser spectrum to study resonance-enhanced multiphoton ionization
(REMPI) of a multilevel system in sodium atoms. We demonstrate experimentally that different
excitation pathways and, accordingly, different target channels can be addressed selectively
by a single control parameter, i.e. the chirp. The nature of these pathways is unraveled
by measurement of photoelectron angular distributions (PADs) from velocity map imaging
(VMI) [45]–[50], yielding detailed information on the origin of the released photoelectron
wave packets. Theoretical investigations of the light–atom interaction reveal an interplay of
different physical mechanisms governing control. Analysis of the neutral excitation dynamics
for a five-state model atom (including the most relevant states 3s, 4s, 5p, 6p and 7p) under the
influence of a chirped ultrashort laser pulse highlights how physical mechanisms, such as RAP
and DSS, act jointly to either address single states among the high-lying sodium states 5p, 6p
and 7p (cf figure 1) or excite superpositions of any two neighboring states. We point out that
the present paper extends two earlier techniques in several significant directions. The technique
of Melinger et al [29] uses a single chirped picosecond laser pulse to selectively excite the two
fine-structure components 3p1/2 and 3p3/2 in sodium atoms. The present technique adds a DSS to
the control tools, which enables the population of a third state, and also the creation of coherent
superposition states. The technique of Clow et al [34] makes use of a shaped femtosecond pulse
to selectively populate a single highly excited state. The present technique is more flexible, since
it allows to populate several different states by variation of a single parameter: the chirp.
The paper is organized as follows. We start in section 2 by introducing the excitation
and ionization scheme of sodium atoms exposed to ultrashort near-infrared laser pulses, and
subsequently describe the details of our experimental setup. The experimental results are
presented in section 3 along with a physical discussion of general features observed in the
measured PADs supported by numerical simulations of the measurement results. Section 4
provides a detailed theoretical analysis of the strong-field-induced chirped excitation dynamics
in terms of adiabatic states, highlighting different physical mechanisms that govern the
light–atom interaction. We conclude the paper with a brief summary and conclusions.

2. Experiment

In our experiment, we combine spectral phase shaping to produce chirped ultrashort laser pulses
with the measurement of PADs resulting from REMPI of sodium atoms, employing the VMI
technique. In this section, we first introduce the sodium excitation scheme with emphasis on
the different accessible excitation and ionization pathways. Then we describe the experimental
setup and layout of our photoelectron imaging spectrometer.

2.1. Excitation scheme

Figure 1 shows the excitation and ionization scheme of sodium atoms based on energy-level
information taken from the NIST database [51]. Different multi-photon excitation pathways
are accessible during the interaction of sodium atoms with intense ultrashort laser pulses
(laser specifications are given in section 2.2). The predominant excitation pathway is a 2+1+1
REMPI process via the two-photon transition 4s ←← 3s (red arrows in figure 1), which is
nearly resonant with our laser spectrum [52]. Consequential population of states 5p, 6p and 7p
gives rise to photoelectron wave packets in the ionization continuum having s- or d-symmetry.

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Figure 1. Excitation and ionization scheme of sodium atoms illustrating the

excitation pathways that arise during the interaction with an intense 795 nm,
30 fs full width at half maximum (FWHM) laser pulse. These pathways comprise
a 2 + 1 + 1 REMPI (red arrows) and a 3 + 1 REMPI (green arrows) process from
the 3s ground state as well as a two-photon ionization process from state 3p (blue
arrows). Blurred red bars represent the one-, two- and three-photon spectra of our
laser, respectively. Since state 4s lies within the bandwidth of the two-photon
spectrum, the laser strongly drives the transition 4s ←← 3s. Once state 4s is
populated, population flows to states 5p, 6p and 7p, giving rise to photoelectron
wave packets with combined s- and d-symmetry at characteristic kinetic energies
0.76, 1.04 and 1.20 eV in the ionization continuum. A competing excitation
pathway is opened up by three-photon absorption leading to population of
states 5f and 6f in addition. Photoelectrons from this excitation channel are
characterized by a combined d- and g-symmetry of the measured PADs at kinetic
energies 1.02 and 1.18 eV, respectively. Two-photon ionization from the non-
resonant, transiently populated state 3p results in photoelectron wave packets at
about 0.2 eV, having combined p- and f-symmetry. For illustrative purposes, the
relevant symmetries of the released photoelectron wave packets are visualized
on top of the figure in red and blue, encoding the positive and negative signs of
the electron wavefunction, respectively.

The recorded PADs therefore exhibit a combined s- and d-symmetry and are measured at
the distinct kinetic energies 0.76, 1.04 and 1.20 eV, corresponding to states 5p, 6p and 7p,
respectively. Alternatively, a 3 + 1 REMPI process (green arrows in figure 1) based on three-
photon absorption from the 3s ground state with no intermediate resonances is taken into
account, contributing also to the population of states 5p, 6p and 7p but, in addition, transferring
population to states 5f and 6f. One-photon ionization of the latter results in photoelectron
wave packets with d- and g-symmetry at kinetic energies 1.02 and 1.18 eV, respectively.

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Figure 2. Experimental setup. Horizontally polarized femtosecond laser pulses

are sent into a vacuum chamber and refocused by a 50 mm on-axis concave
mirror into sodium vapor provided by an alkali metal dispenser source (not
shown). Photoelectrons emitted by the light–atom interaction are projected
toward a position-sensitive MCP detector using the VMI method. The amplified
signal is recorded by a 1.4 million pixels camera system and sent to a computer.
An Abel inversion is performed using the pBasex algorithm.

These photoelectrons are distinguished from the p-state contributions (at 1.04 and 1.20 eV)
by the symmetry of their angular distributions. In the following, we will refer to the different
photoelectron contributions as different energy channels at nominal kinetic energies of 0.8, 1.0
and 1.2 eV, and infer their origin, i.e. the excitation pathway, from the angular distribution. Both
multi-photon excitation pathways proceed via the intermediate, non-resonant state 3p, which is
only transiently populated. However, since ionization takes place during the excitation also
photoelectrons from this state are detected at low kinetic energies around 0.2 eV (blue arrows in
figure 1). For more details see caption of figure 1.

2.2. Setup
In this section, the experimental setup comprising the laser system and the photoelectron
imaging spectrometer is described. Intense 795 nm, 30 fs FWHM laser pulses provided by an
amplified 1 kHz Ti:sapphire laser system (Femtolasers Femtopower Pro) were phase modulated
in frequency domain by a home-built pulse shaper [53], applying quadratic phase masks of the
form ϕmod (ω) = ϕ2 /2(ω − ω0 )2 , where ω0 is the central frequency of our laser spectrum [27].
The chirp parameter ϕ2 was varied in the range from −2000 fs2 to +2000 fs2 in steps of
1ϕ2 = 100 fs2 . The chirped output pulses of 12 µJ energy were sent into a vacuum chamber
and refocussed by a concave mirror (5 cm focal length; we estimated a peak intensity of
about 1013 W cm−2 for the bandwidth-limited pulse) into sodium vapor supplied by an alkali
metal dispenser source, as shown in figure 2. Photoelectrons released during the strong-
field interaction of the shaped pulses with single atoms were detected by a photoelectron
imaging spectrometer using the VMI method. In order to compensate the residual chirp of
the unmodulated pulse, we performed an in situ adaptive optimization of the multi-photon
ionization of water vapor background (about 4 × 10−7 mbar) in the interaction region of

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the spectrometer. The resulting optimal compensation phase was additionally applied to the
pulse shaper during the experiments, ensuring an error in the chirp parameter ϕ2 of less
than 150 fs2 . The energy calibration of the imaging spectrometer was performed using a
3 + 1 REMPI of xenon atoms excited by a Nd : YAG ns laser system at 355 nm, achieving a
spectrometer resolution of 60 meV at 0.5 eV. Employing the energy-calibrated photoelectron
imaging spectrometer, we studied angular and energy-resolved photoelectron spectra as a
function of the chirp parameter ϕ2 .

3. Experimental results and discussion

Figure 3 (upper row) shows measured PADs from REMPI of sodium atoms with chirped
fs laser pulses for three exemplary values of the chirp parameter ϕ2 . The middle row
displays the corresponding Abel-inverted (retrieved) PADs obtained by employing the pBasex
algorithm [50, 54]. When PADs arise from ionization with polarization-shaped pulses [55],
direct tomography methods have been developed for three-dimensional reconstruction of
ultrashort free photoelectron wave packets [56]. Angular sections through the retrieved PADs at
kinetic energies 0.8, 1.0 and 1.2 eV, as plotted in the lower row, serve to identify the symmetry
of the different energy channels observed in the PADs. The PAD measured for the unmodulated,
i.e., bandwidth-limited pulse is depicted in the central column. Three major contributions are
observed at kinetic energies 0.8, 1.0 and 1.2 eV, related to the energy channels discussed above
(cf section 2.1). The angular section taken at 1.2 eV exhibits two minor nodes between 0◦ and
180◦ , i.e. d-symmetry. This channel is attributed mainly to ionization via state 7p (red excitation
pathway in figure 1), though our numerical simulations (inset of figure 4) indicate that also
ionization via state 6f (green excitation pathway in figure 1) delivers a minor contribution. The
contribution of an s-wave to this channel, as expected from the excitation scheme figure 1,
is reflected in the weak equatorial signal. At an angle of 90◦ s- and d-waves have opposite
sign and, thus, interfere destructively, whereas at the poles, i.e. at 0◦ and 180◦ , both waves
add up constructively. The section taken at 1.0 eV exhibits four nodes between 0◦ and 180◦ ,
corresponding to g-symmetry. This contribution originates predominantly from ionization via
state 5f. The observation that the lobe at 90◦ (and 270◦ , respectively) is slightly lowered with
respect to its two neighbors indicates a weak d-wave contribution interfering destructively with
the g-wave in this angular segment. The contribution measured at 0.8 eV shows again combined
s- and d-symmetry and is ascribed to ionization via state 5p.
Moreover, a weak contribution is observed at about 0.2 eV, a magnification of which is
shown in the inset of figure 3(b). The nodal structure of this signal exhibits distinct f-symmetry.
However, the pronounced poles of the PAD as well as the fact that the nodes at 45◦ and 135◦ in
the angular section are raised with respect to the node at 90◦ give a hint on a p-wave contribution
to the photoelectron signal. Observation of photoelectron wave packets with combined p and
f-symmetry close to the ionization threshold is consistent with two-photon ionization from
state 3p (blue pathway in figure 1). Note that state 3p is—although non-resonant—transiently
populated during the interaction, mediating the multi-photon processes to the state 4s and the
high-lying f states.
For large negative values of ϕ2 (left column in figure 3), i.e. strongly down-chirped laser
pulses, the outer channel at kinetic energy 1.2 eV is considerably enhanced in comparison to
the bandwidth-limited case, whereas the intermediate channel at 1.0 eV is strongly reduced and
the two innermost contributions have essentially vanished. Note the change in symmetry of

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Figure 3. Measured PADs from excitation and ionization of sodium atoms

using both chirped and bandwidth-limited fs laser pulses. In the upper row,
measured PADs for different values of the chirp parameter ϕ2 are shown. (a) ϕ2 =
−2000 fs2 (down-chirp). (b) ϕ2 = 0 (bandwidth-limited). (c) ϕ2 = +2000 fs2 (up-
chirp). All images are scaled to the same maximum value. The middle row
contains the corresponding Abel-inverted PADs obtained using the pBasex
algorithm. Angular sections through the retrieved PADs at kinetic energies of
about 0.2, 0.8, 1.0 and 1.2 eV (lower row) reveal the symmetries of the observed
contributions and shed light on the underlying ionization pathways. The signal
offsets are introduced for better visibility.

the intermediate channel which exhibits combined s- and d-symmetry in this case, indicating
more efficient ionization from state 6p, while the 5f contribution is very small. Changing the
sign of ϕ2 , i.e. using strongly up-chirped laser pulses (right column in figure 3), suppresses
the high-energy channel in favor of the intermediate channel at 1.0 eV, which dominates the
PAD in this case. From its angular section at 1.0 eV, we find a combined d- and g-symmetry,
as in the bandwidth-limited case. This contribution is therefore traced back mainly to state

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Figure 4. Measured photoelectron kinetic energy distributions as a function of

the chirp parameter ϕ2 . The data were obtained by angular integration of the
retrieved PADs. Three main energy channels are observed at 0.8, 1.0 and 1.2 eV,
each of which can be activated by appropriate choice of the chirp parameter.
For ϕ2  0, i.e. strongly down-chirped laser pulses, photoelectrons with high
kinetic energies related to the high-lying state 7p (and minor 6f contribution)
are produced. The intermediate channel at 1.0 eV, related to states 6p and 5f, is
addressed by strongly up-chirped laser pulses with ϕ2  0. Photoelectrons with
kinetic energies around 0.8 eV, corresponding to state 5p, are favored at small
positive values of ϕ2 , i.e. high laser pulse peak intensities. The weak contribution
at 0.2 eV in the same ϕ2 region stems from ionization of the non-resonant state
3p. The inset shows results from a numerical simulation of the multi-photon
excitation and ionization process.

5f. The finding that the symmetry of photoelectrons from the intermediate channel alters from
d to g is rationalized by the change of the ordering of red and blue frequency components
within the chirped pulse. For a down-chirped pulse, i.e. when the blue components arrive first,
initially, the system is in resonance with the two-photon transition 4s ←← 3s implying efficient
ionization via the p states (red pathway in figure 1). On the other hand, up-chirped pulses favor
ionization via state 5f since at early times the system is in resonance with the three-photon
transition 5f ←←← 3s (green pathway in figure 1). Such processes have also been observed
in [39] under different excitation conditions.
In order to provide the full picture of the chirp-dependent population flow to the different
energy channels, we performed an angular integration of all 41 measured PADs and present
the resulting energy-resolved photoelectron spectra in terms of a two-dimensional map as a
function of the kinetic energy and the chirp parameter ϕ2 . The result obtained upon variation of
ϕ2 in the range from −2000 to +2000 fs2 is displayed in figure 4. The three major channels at
0.8, 1.0 and 1.2 eV are clearly visible. Note that for e.g. rare gas atoms under our experimental

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conditions ponderomotive shifts of more than 0.5 eV are calculated. No such shifts are observed
in the experiment, since the high-frequency approximation [57, 58] (necessary condition for the
application of the ponderomotive energy concept) is not valid for alkalis excited by near-infrared
laser radiation. An analysis of the neutral excitation dynamics behind the observed contributions
will be given in section 4. The map illustrates the above statements that for large negative values
of ϕ2 the high-energy channel at 1.2 eV is addressed with high efficiency, i.e. a down-chirped
pulse steers the population predominantly towards the high-lying state 7p. For large positive
chirp values the intermediate channel is selectively addressed, corresponding to predominant
population of states 6p and 5f. The low-energy channel is accessed most efficiently in the
vicinity of ϕ2 = 500 fs2 . In fact, in the regime 0 6 ϕ2 6 1000 fs2 the photoelectron spectrum
is made up of contributions from states 5p, 6p and 5f. Because the excitation (and simultaneous
ionization) takes place on an ultrashort timescale precluding decoherence processes, a coherent
superposition of states 5p, 6p and 5f is excited in this chirp regime. Upon changing the sign of
ϕ2 , i.e. for −1000 fs2 6 ϕ2 6 0, the laser pulse induces a coherent superposition of states 6p, 5f
and 7p. Photoelectrons observed at about 0.2 eV for moderate positive chirps are attributed to
two-photon ionization from state 3p.
The inset to figure 4 shows results from a numerical simulation of the simultaneous
multi-photon excitation and ionization process. The calculations are based on numerical
integration of the time-dependent Schrödinger equation for a neutral 20-state system
(comprising those states labeled in figure 1 and taking the fine structure splitting into account)
interacting with an intense chirped 795 nm, 30 fs FWHM Gaussian input pulse. One-photon
ionization from the high-lying p and f states is treated within a simplified model employing
the first-order perturbation theory. We assume a flat continuum and unit coupling elements
with no additional phases for all bound-free transitions. A more rigorous treatment of the
ionization step involving the determination of radial coupling matrix elements also for the
bound-free transitions is provided by, e.g. single-channel quantum defect theory [59] as
reported for instance in [60, 61]. In order to model the two-photon ionization from state
3p proceeding, for example, via state 3d as indicated by the blue pathway in figure 1, we
employed second-order perturbation theory. For a more detailed description of our method
see [25, 27, 62]. The simulation of photoelectron spectra reproduces the main features of the
experimental results very well. This allows us to look into the underlying neutral excitation
dynamics and follow the population flow within the bound atomic system. We find that
for large negative chirp ϕ2 state 7p is addressed almost selectively, while for large positive
ϕ2 values both states 6p and 5f are populated efficiently in equal measure. The latter is
in accordance with the experimental observation of the PAD with pronounced g-symmetry
in the intermediate channel at 1.0 eV for large positive chirp (see figure 3(c)). The most
efficient excitation of state 5p occurs for moderate positive chirp. However, in this chirp
regime states 6p and 5f receive comparable population confirming the observation of a PAD
with a contribution of g-symmetry at 1.0 eV and zero chirp. At moderate negative chirp,
we obtain a coherent superposition of states 6p, 5f and 7p. Note that the weak contribution
around 0.2 eV and small positive values of ϕ2 observed in the experiment (shown in the
inset to figure 3(b)) is also reproduced in the simulation. Within the framework of our
simulation, these photoelectrons are ascribed to two-photon ionization from state 3p which
receives non-perturbative transient population. We note that in a perturbative regime, ionization
from this transiently populated state could be interpreted as a transition from a virtual
state.

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In the next section, we will further investigate the neutral population dynamics by means of
a reduced atomic system in order to rationalize the general features observed in the experiment
in terms of physical mechanisms governing the excitation process.

4. Theoretical model

In this section, we provide mainly a qualitative description of the system at hand. To this end,
we assume that the photoelectron signal arises most significantly through the 2 + 1 + 1 REMPI
channel (red pathway in figure 1), involving the five states 3s, 4s, 5p, 6p and 7p. The idea of this
reduction is to demonstrate the basic principles influencing the dynamics of the whole system,
which become more transparent in this simplified model, involving the most significant states
for our experiment. In this approach, we adiabatically eliminated state 3p [44, 63, 64] because
it is off resonance and receives smaller transient population than the other coupled states. Its
presence, however, affects the population dynamics significantly for it induces strong DSSs in
the energies of states 3s and 4s, which substantially modify the energy diagram.
The quantum dynamics of this five-state system obeys the time-dependent Schrödinger
equation
d
ih̄ c(t) = H(t)c(t). (1)
dt
The Hamiltonian H(t) in the rotating-wave approximation, rotating with the instantaneous laser
frequency ω(t) = ω0 + 2at (see equation (A.5) in the appendix), is given by [44, 64]

11 − S1 1

 
2 12 0 0 0
 2 12 12 − S2 12 23 12 24 12 25 
 1 
 
H(t) = h̄  0 1
23 13 0 0 . (2)
 
 2 
 0

1

2 24
0 14 0  

0 1

2 25
0 0 15

Here the explicit time dependence is dropped for ease of notation. The vector c(t) =
[c1 (t), c2 (t), . . . , c5 (t)]T consists of the amplitudes of the five states, ordered as shown
above, which are obtained by numerical integration of the Schrödinger equation (1), the
respective populations are Pn (t) = |cn (t)|2 , 1n (t) = ωn − k ω(t) are the generally time-
dependent atom–laser detunings, where ωn are the atomic state eigenfrequencies, with ω3s taken
as zero, k is the transition order, 2n = d2n 0 f (t) represent the one-photon couplings of state
2 to state n (n = 3, 4, 5), 12 = q12 20 f 2 (t) is the two-photon coupling between states 1 and 2,
with f (t) being the chirped laser electric field envelope, dmn are the relevant transition dipole
moments in atomic units, q12 is the effective two-photon transition moment (cf equation (A.1))
and S1 and S2 represent the DSS of states 1 and 2, respectively,
23s3p 23p4s
S1 = , S2 = . (3)
413p 413p
The effect of the DSS due to state 3d is neglected for it is very weakly coupled to the states
whose energies it might influence: the p states are coupled about 10 times stronger to state 4s

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as compared with state 3d; state 3d is not directly coupled to state 3s, but rather through a two-
photon transition. In the first two diagonal elements of the Hamiltonian (associated with the
energies of states 3s and 4s) the atom–laser detuning and the DSS add up to a time-dependent
effective chirp: the former resulting from the time-dependent instantaneous laser frequency ω(t),
and the latter deriving from the time-dependent shift of the level energies due to DSS.

4.1. Excitation regimes

In figure 5, we distinguish five different regimes in regard to the value of the chirp ϕ2 . In all
cases, we plot the bare-state energies and analyze the dynamics by accounting for the presence
of level crossings. Because it is the ionization signal that is observed in the experiment it is also
important when a particular level crossing occurs: a level crossing at early time, and the ensuing
adiabatic passage transition, would translate into a larger ionization signal than a late crossing,
where even a significant population transfer to a certain discrete state would not be reflected in
the ionization signal.
Below we examine the dynamics of our system with particular interest in states 5p, 6p
and 7p. In figure 5, we show the populations and the energies of the five bare states for the
chirp ϕ2 varied between −2000 and 2000 fs2 (from left to right) with the system initiated
in state 3s. For illustrative purposes we pick 0 = 0.3 fs−1 , corresponding to an intensity of
3.7 × 1012 W cm−2 [63] and 1t = 30 fs.

4.1.1. Large negative chirp. For large negative chirp (ϕ2 = −2000 fs2 , figure 5(a)) the laser
field reaches resonances relative to the 7p ← 4s (one-photon) transition and the 4s ←← 3s
(two-photon) transition in nearly the same instant, thus creating a ‘bow-tie’ level crossing
pattern [44], [65]–[69], which is of particular significance because it involves three rather
than two states. This crossing results in efficient population transfer to states 4s and 7p and
depopulation of state 3s. Because state 7p is populated at such early times, it is exposed to
ionization for most of the interaction dynamics and hence has a dominant contribution in the
photoelectron signal (see figure 4 at 1.2 eV and −2000 fs2 ).
Later on we observe almost adiabatic evolution and the population is shared mainly
between states 4s and 7p in the form of Rabi oscillations with fading amplitude [70]. State 6p
acquires only marginal population mainly due to its crossing with state 3s (which is, however,
already depleted due to the preceding ‘bow-tie’ crossing) via a three-photon excitation through
state 4s. The late crossings between states 3s and 5p, and also between states 4s and 6p are of
no importance because they occur after the pulse intensity has essentially vanished. State 5p
remains unpopulated since it is far off-resonant throughout the entire dynamics.

4.1.2. Large positive chirp. For large positive chirps (ϕ2 = 2000 fs2 , figure 5(e)) the energy
diagram is mirrored compared with the one for large negative chirps ϕ2 (figure 5(a)). Then
initially the system evolves adiabatically, with minor (off-resonant) population transfer from
state 3s to state 4s due to their strong mutual couplings. Around the time of the peak laser
intensity, as state 3s sweeps across resonance with 6p, the latter starts to effectively populate
through the three-photon 3s–6p crossing. Because this crossing occurs approximately in the
middle of the laser pulse the population of state 6p is exposed to ionization for a considerable

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12
–2000 fs2 (a) –500 fs2 (b) 0 fs2 (c) 500 fs2 (d) 2000 fs2 (e)
detuning (fs–1)

0.2
Pulse and

0.1
0.0
–0.1

0.6 3s
4s 7p
7p 7p 7p 7p
4
Energies (eV)

4s 3s 4s 4s 4s
6p 6p 6p 6p 6p
2
3s 3s
3s
0 5p 5p 5p 5p 5p

1.0

0.8
Populations

0.6
6p
7p
0.4 7p 5p
5p
0.2 5p
6p 6p
6p 6p 7p
0
–200 0 200 –50 0 50 –30 30 –50 0 50 –200 0 200
Time (fs)

Figure 5. Populations (lower frames) and energies (middle frames) of the states
of interest 5p, 6p and 7p versus time for ϕ2 varied (from left to right) between
−2000 fs2 (down-chirp) and 2000 fs2 (up-chirp), 0 = 0.3 fs−1 and 1t = 30 fs.
In the middle frames, colored and gray lines depict the bare state energies. The
latter are related to states 3s and 4s and include the effective chirp, i.e. the chirp of
the laser as well as the chirp due to ac Stark shifts. The black lines represent the
dressed state energies and the arrows show the population flow. The populations
in the lower frames are consistent with the asymmetry in the experimental results
presented in figure 4: for large chirps states 6p (positive chirp) and 7p (negative
chirp) are predominantly populated, whereas around zero chirp the contribution
comes mostly from state 5p. The envelopes (straight lines) and detunings (dashed
lines) of the modulated pulses are shown in the uppermost frames. Note that the
energies are mirrored when changing the sign of the chirp ϕ2 .

time interval, which results in significant photoelectron signal from 6p (see figure 4 at 1.0 eV and
+2000 fs2 ). For the same reason—the 3s–6p crossing occurring near the laser pulse maximum—
the population transfer from state 3s to state 6p is relatively efficient and only about half of
the population is left in states 3s and 4s thereafter; then only a part of this already reduced
population is transferred to state 7p at the subsequent ‘bow-tie’ crossing 3s–4s–7p. Moreover,

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13
this crossing occurs at late times and hence state 7p is not visible in the photoelectron spectrum.
State 5p remains unpopulated once again as it stays far off any resonance.
We now turn our attention to the regimes of a moderately large chirp ϕ2 , where the
photoelectron spectrum changes from a single-state feature to one displaying double features.

4.1.3. Moderate negative chirp. For a moderate negative chirp (ϕ2 = −500 fs2 , figure 5(b)) an
early crossing occurs between states 3s, 4s and 7p in the rising edge of the pulse, which leads to
a partial population transfer from state 3s to states 4s and 7p, because the laser intensity is not
strong enough to enforce adiabatic evolution. The population in state 7p is exposed to ionization
for the rest of the pulse, whereas the population in state 4s proceeds until the subsequent 4s–6p
crossing where it is partially transferred to state 6p. The leftover temporary flows into state 5p,
which starts to emerge in the photoelectron spectrum, and is finally driven back into state 3s. In
result, all states 5p, 6p and 7p are visible in the photoelectron signal, which is an indication for
the creation of a coherent superposition of these (see figure 4 at about −500 fs2 ).

4.1.4. Moderate positive chirp. For moderate positive chirps (ϕ2 = 500 fs2 , figure 5(d)) state
3s first comes very close to state 5p at times of the laser pulse maximum; during this proximity
the population undergoes Rabi-type oscillations between states 3s and 5p and is exposed to
ionization from state 5p. The signature of state 5p is clearly visible and indeed this is the regime
where this state indisputably dominates in the photoelectron signal (see figure 4 at 0.8 eV and
+500 fs2 ). In other words, it is the DSS induced by the two-photon transition 4s ←← 3s which
makes the population of the far-off-resonant state 5p possible [71]. If this Stark shift were absent
(e.g. if the two-photon transition 4s ←← 3s were instead a single-photon one in a gedanken
scenario) state 5p would never receive sizeable population. As we proceed beyond the pulse
maximum state 3s crosses state 6p and the population is partially transferred to the latter. Hence
state 6p emerges in the photoelectron signal due to the ensuing ionization, whereas state 7p is
invisible in this regime because all population left flows into state 4s.

4.1.5. Zero chirp. In this regime, the laser pulse is unchirped, ϕ2 = 0. Therefore, the effective
chirp is entirely due to ac Stark shift. The latter is symmetric to the pulse because it is induced
by the same pulse. Moreover, because state 3s crosses states 6p and 5p (figure 5(c)), sizeable
population will visit these two states through the respective first crossings 3s–5p and 3s–6p.
A second pair of crossings in the falling edge of the pulse will induce additional transitions
5p ←←← 3s and 6p ←←← 3s. The implication is that states 5p and 6p will contribute
significantly to the photoelectron signal (see figure 4 around ϕ2 = 0). State 7p, on the other
hand, remains well off resonance throughout and receives only a small population due to (weak)
non-resonant interaction. Its contribution to the photoelectron signal should be therefore more
muted than those from states 5p and 6p.

4.2. Discussion
Below we discuss the five excitation regimes in the dressed state (adiabatic) context. When
adiabatic, which demands large couplings and low chirp rates for the avoided crossings in
question, starting in state 3s we end up in state 7p for ϕ2 < 0 or in state 6p for ϕ2 > 0 (figure 5,
middle frames; in the latter case a fully non-adiabatic passage across state 5p occurs, since

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14
the pulse intensity is negligible for the 3s–5p resonance). Therefore, clearly from figure 5, our
system exhibits a somewhat adiabatic behavior for chirp ϕ2 away from the origin. As we get
closer, the crossings shift toward the pulse wings, whereas the pulse gets narrower in time, which
in combination results in breaking adiabaticity. The latter is further hindered by the increased
DSS, which effectively enhances the chirp rate.
We expect adiabaticity to remain almost unaffected for large negative values of the chirp
√
ϕ2 , since the chirp rate a ∝ 1/ϕ2 and  ∝ 1/ ϕ2 , and to break down for large positive values,
for it relies on the three-photon transition 6p ←←← 3s, which gets weaker, as the resonances
relative to 3s–4s and 4s–6p further separate in time. Larger peak intensities 0 strengthen
adiabaticity for the transition 7p ←←← 3s and make complete population transfer possible, as
also indicated in [34], whereas for the transition 6p ←←← 3s due to the unfavorable influence
of the increased DSS we predict the contrary.

5. Summary and conclusion

In this contribution, we presented a joint experimental and theoretical study on strong-field

REMPI of sodium atoms using chirped femtosecond laser pulses. Experimentally, PADs have
proven to be the essential tool to identify the different excitation and ionization pathways.
We observed three distinct ionization pathways contributing to the measured PADs. The
predominant contribution with combined s- and d-symmetry is due to 2 + 1 + 1 REMPI processes
involving the strongly driven two-photon transition 4s ←← 3s, and subsequent ionization from
the states 5p, 6p and 7p. Photoelectrons with combined d- and g-symmetry originated from
3 + 1 REMPI via states 5f and 6f. A weak contribution with combined p- and f-symmetry close
to the ionization threshold is attributed to the third channel, that is two-photon ionization of the
non-resonant transiently populated state 3p.
Selective population of the highly excited states 5p, 6p, 7p and 5f, 6f was achieved by
controlling a single pulse parameter, i.e. the chirp parameter ϕ2 . In particular, we observed
highly selective population of state 7p using strongly down-chirped laser pulses. For strongly
up-chirped laser pulses states 6p and 5f were populated with high efficiency and a dominant
signal from state 5p was obtained for moderately up-chirped laser pulses. Moreover, in the
intermediate chirp regions coherent superpositions of neighboring states have been excited.
Simulations based on numerical integration of the time-dependent Schrödinger equation
for a neutral 20-state system are in agreement with our experimental findings. In addition, a five-
state model was developed in order to provide insights into the physical mechanisms at play. Our
analysis of the time-dependent populations showed that by tuning the chirp parameter distinct
physical mechanisms have been addressed, involving adiabatic and non-adiabatic time evolution
along with DSSs and (multiple) level crossings. It was pointed out that the occurrence of an
uncommon ‘bow-tie’ level crossing is responsible for the excitation of coherent superposition
states as observed in the experiment. The strong DSS of the two-photon transition 4s ←← 3s
turned out to be of particular significance for populating state 5p being inaccessible in weak
laser fields.
Our results highlight the importance of studying model systems experimentally and
theoretically to better understand the physical mechanisms of strong-field coherent control.
Our findings demonstrate that, in general, in strong-field control multiple pathways involving
different physical mechanisms are at play simultaneously.

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15
Acknowledgments

Discussions with P Lambropoulos and F Faisal regarding the measured photoelectron signals
assigned to two-photon ionization from state 3p are gratefully acknowledged. The Kassel
group furthermore acknowledges financial support by the Deutsche Forschungsgemeinschaft
DFG. This work has also been supported by European Commission projects EMALI and
FASTQUAST, and the Bulgarian NSF grants VU-F-205/06, VU-I-301/07, D002-90/08 and
IRC-CoSiM.

Appendix. Details of calculations

Each p state consists of p1/2 and p3/2 substates, coupled by 1/2 and 3/2 , respectively, to a
relevant s state. Therefore initially our system comprises overall 10 states (prior to eliminating
state 3p). To simplify our approach we perform a transformation to a dark-bright basis for each
of the p states and thus eliminate half of the p substates as dark (uncoupled) states, and keep the
rest, which become coupled by the root mean square of the relevant 1/2 and 3/2 and are the
ones to be referred to as p states throughout the theoretical part of the paper.
The effective two-photon transition moment between states 3s and 4s is
da db + dc dd
q12 = − , (A.1)
213 p
where da,c and db,d are the dipole moments for the transitions 3p1/2,3/2 ← 3s1/2 and 4s1/2 ←
3p1/2,3/2 , respectively.
The effect of a quadratic phase modulation in frequency domain of the form
ϕ2
ϕ(ω) = (ω − ω0 )2 (A.2)
2
is described in time domain by a modulated linearly polarized laser electric field E(t) given
as [72]
E (t) = 2Re E + (t) ,

(A.3)
where for the positive-frequency part we have
E 0 −(t 2 /4βγ ) iω0 t i(at 2 −ε)
E + (t) = e e e (A.4)
2γ 1/4
with
1 ϕ2
ε = arctan ,
2 2β
1t 2
β= ,
8 ln 2
ϕ2
 2
γ = 1+ ,
2β
ϕ2
a= 2
8β γ
New Journal of Physics 11 (2009) 105051 (http://www.njp.org/)
16
resulting in the time-dependent instantaneous laser frequency

ω(t) = ω0 + 2at. (A.5)

Here 1t denotes the FWHM of the intensity I (t) of the unmodulated pulse, ω0 is the laser
carrier frequency and ϕ2 is the chirp parameter to be varied.
We define a reference Rabi-frequency (t) = 0 f (t), where f (t) is the laser electric field
envelope
 2 
t
exp − 4βγ
f(t) = . (A.6)
γ 1/4

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