A third-order pulse correlation ghost is a correlation lobe generated by a real feature in the nonlinear gate, appearing at a delay where no separate input pulse need exist. It is a property of the measurement's cross-correlation, not automatically an optical prepulse or optical postpulse.
The optical pulse temporal contrast article derives the separated-replica model for , and nonoverlapping identical-shape pulses. In third-order intensity autocorrelation, the main, positive-delay and opposite-delay lobe weights are respectively
The physical delayed replica enters linearly when it meets the strong squared gate; its squared contribution to the gate creates the opposite-delay ghost. Lobe separation and negligible pulse overlap are assumptions of this simple decomposition.
For an original , the real postpulse has four percent of the main intensity and equal duration. Normalized to the correlation's main peak, its lobe is , while the ghost is . A feature at negative delay near that latter level does not establish a physical prepulse. The ghost-to-real-lobe ratio is exactly in this model. This ghost-level consistency test for a delayed pulse replica can check an interpretation, although an actual prepulse could also be present.
Figure 1.
A real optical postpulse creates an opposite-delay ghost in an ideal third-order intensity autocorrelation
. Original compact triangular intensity profiles with a delayed replica at4ps and relative peak0.04. Direct numerical correlation produces the opposite-delay lobe near0.0016; the optical profile has no pulse there. Each panel is normalized to its own maximum. Source. Details.
The historical correlator's inserted-etalon test supplies a controlled physical postpulse for checking the delay orientation.[ref] Independent changes to the replica strength, or a reference with known temporal structure, test the ghost interpretation. Overlapping pulses, unequal shapes and instrument backgrounds require a richer model.
Time-resolved spectroscopy measures how a spectroscopic response changes after a defined excitation or other reference event. Instead of only a time-integrated spectrum, it records a response such as as a function of frequency and delay. A changing spectral feature can distinguish population loss, changing molecular environment and motion of a resonance; a single integrated intensity need not separate them.
In pump-probe spectroscopy, a pump pulse prepares the sample and a delayed probe interrogates it. A movable mirror in a double-pass optical path provides a precise delay change:
For an original displacement of 15 micrometres, the delay changes by about 100 femtoseconds. A spectrally resolved detector records the response while delay is scanned. The time resolution is set by pulse overlap, jitter and the detection scheme, rather than by mirror step size alone. Ahmed H. Zewail's lecture explains how such optical timing enabled femtochemistry.[ref]
An original decay example assumes an isolated feature with background already removed and response
If its intensity at 3 picoseconds is of its intensity at 1 picosecond, then and . This inference assumes the same feature is measured at both delays and that the instrument response is sufficiently short. A shifting line observed through a narrow spectral window can change intensity without following that simple population law.
Finite resolution instead produces a convolution. For a time-invariant instrument response function at a selected spectral channel,
For ideal Gaussian pump and probe intensity envelopes, their cross-correlation width is the square root of the sum of their squared widths. Chosen full widths of 80 and 100 femtoseconds therefore give about 128 femtoseconds before other contributions. This original calculation describes pulse-overlap resolution, not an arbitrary material lifetime.
A motivating historical example is Zewail's discussion of the NaI/NaBr experiments reported in 1988. Delay-dependent signals probe evolving molecular motion and final fragments, supplying information absent from a static spectrum. His lecture presents the NaI dynamics in Figure 15.[ref]
A practical experiment compares pumped and unpumped records, checks delay zero and wavelength calibration, and varies excitation strength to test whether the response remains in the intended regime. Negative-delay data, backgrounds and the measured instrument response function help distinguish sample dynamics from timing and detection artifacts.