Direct observation of attosecond light bunching

Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10-18 s) timescales. A frequency ‘comb’ of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train1,2. Laser pulses spanning many optical cycles have been used for the production of such light bunching3,4, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts5,6. If these bursts are intense enough to induce a nonlinear process in a target system7,8,9, they can be used for subfemtosecond pump–probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization4,6,10 and ultrafast dynamics11 rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.