Circularly polarized driving pulses

Independently of the precise dynamics in the silicon crystal, circular harmonics from circular drivers (CHCD) could be expected in a broad sense by requirements of symmetry. The selection rules for circular polarization can be calculated quite easily for specific cases [141] and have been extended to arbitrary symmetry groups and higher harmonics by Tanget al. with group theoretical methods (see also Sec.

1.2.3). There, Tanget al. pointed out that for cubic systems, harmonics should all be circularly polarized with alternating helicities. Nevertheless, although obvious in a sense, this does not mean that the generation of circularly polarized harmonics is trivial or not worth being looked at. As argued in Sec. 1.1.4, there is great interest in generating circularly polarized high harmonics and the complexity of doing so in gases makes its solid HHG counterpart quite appealing.

Fig. 2.15ashows a polarizer scan of the three harmonics HH5-HH9 from silicon with circular driving excitation. For all harmonics there is almost no variation in intensity over polarizer rotation ξ. For reference, high harmonics have been gen-erated with the same driving pulses but with a higher intensity of approximately 40 TW cm⁻² from 50µm-thin z-cut α-SiO₂ samples. A corresponding ξ-scan is shown in Fig. 2.15b, showing two harmonics from SiO₂. The trigonal symmetry group of SiO₂ allows for even harmonics to be generated, hence HH4 can be

ob-Chapter 2. Visible high harmonics and their response to ellipticity

b c

a

Figure 2.15: Polarizer scans of high harmonics from Si (a) and SiO₂ (b). Solid lines are sin²-fits. c shows |_n| (radial) from Si versus sample rotation (angle). In all figures, the driving pulses are circularly polarized. Adapted from [161].

b c a

HH4 HH5

45 75 105 135

Driver RHCP Driver LHCP

ψ(°)

Si SiO₂ SiO₂

HH3 HH5 HH7 HH9

45 75 105 135

Driver RHCP Driver LHCP

ψ (°)

Figure 2.16: Observation of selection rules from Si and SiO₂ with circular ex-citation. The polarization rotation angle ψ following propagation of harmonics through a second QWP for the cases of HHG from Si (a) and SiO₂ (b). c: The harmonic yields of HH3 and HH4 from SiO₂ when going from linear to circular driver polarization. Adapted from [161].

served. The selection rules will be elaborated on below. Also here, both harmonics do not show any variation in intensity over ξ.

Fig. 2.15c shows another polar plot but this time it is not a ξ-scan. Here, the radial variable is |_n| and the sample rotation is the angular variable. For pulses that are at least a couple of cycles long, a rotation of the sample should not cause variations in |_n| or the harmonic yield when the driving pulses are circularly polarized. This is because there is no specific time where electrons are born because the magnitude of the electric field varies little over the course of a cycle. Then it does not matter if the sample is rotated, and all sample rotations should be equivalent (except for a phase shift, as is shown in the supplement of Ref. [147]). In Fig. 2.15c this is clearly visible in the form of very little variation of |_n| over 180^◦-variation of θ. Residual variation stems from the driving pulses not being perfectly circularly polarized, but instead ≈0.97 (see Sec. 2.1.5).

The selection rules of CHCD can be seen as conservation of spin angular mo-mentum of light [147]. In cubic materials for instance, it is required by selection rules that the helicities of successive harmonics are alternating [105,147,148],

mean-ing successive harmonics rotate in opposite senses. One method to measure the helicity of a circular wave, relies on phase-shifting one polarization direction to the one perpendicular by λ/4. This is easy to see. In Jones calculus, a circularly polarized wave is written as

J_circ= 1

√2





1

±i



. (2.9)

The + sign (- sign) in front of the imaginary unit is applied for left handed (right handed) polarization. Using the Jones matrix for a QWP with fast axis along the x-axis:

Jˆ_qwp·J_circ = e^−iπ/4

√2





1 0 0 i



·





1

±i



= e^−iπ/4

√2





1

∓1



. (2.10)

Thus, the resulting wave will be linearly polarized and its polarization axis ψ will be rotated to the x-axis by 45^◦ or −45^◦ depending on its initial helicity. On the experimental side, a QWP that works sufficiently for the wavelength range of observed harmonics (700 nm to 230 nm) could not be found. Therefore, in these experiments a tunable QWP from Alphalas made of α-BBO has been used. It is not a broadband QWP by itself, but the mount of this QWP allows tilting the angle of incidence, thereby optimizing the QWP for different wavelengths. In Fig.

2.16a and b, this procedure has led to the measurement of ψ, the polarization-axis rotation angle with respect to the x-axis. There, one can see, that successive harmonics are indeed counter-rotating.

While selection rules of cubic materials require odd harmonics to have alternat-ing helicities, the symmetry group of SiO₂ requires 2 of 3 harmonics to exist with alternating helicities [148]. Every third harmonic disappears when going from lin-ear to circular polarization. This is confirmed experimentally in Fig. 2.16c, where the yield of HH3 drastically decreases with increasing . In total, the yield di-minishes below the noise floor after a reduction of four orders of magnitude going from linear to circular driving polarization, unambiguously confirming the selection rules.

Another interesting thing to note from Fig. 2.16cis that the yield of HH4 does not decrease with elliptical or even circular driving polarization. In fact, it even increases, peaking around ≈ 0.4. The yield with = 0 and = 1 is equal. A similar behavior has also been observed by Saito et al. from GaSe [147]. This raises interesting questions because from gas HHG one would always expect the harmonic yield to decrease with increasing . One possible explanation could lie in the intraband mechanism dominating the harmonic emission process in these cases. Here, electrons and holes do not need to overlap again and therefore the yield does not necessarily decrease with increasing. For the case of SiO₂ this is a likely explanation because these harmonics are far below the band gap of 9.2 eV. It should however be mentioned that at this point it has not been confirmed generally that the interband mechanism diminishes the yield with elliptical excitation. In that

Chapter 2. Visible high harmonics and their response to ellipticity

case the precise behavior is unclear because holes are mobile too and electrons can re-encounter holes from neighbouring atomic sites [90]. Both these circumstances should affect the recombination probability differently than in the gas HHG case but should also be band-structure dependent.

It should be pointed out that the observation of a constant harmonic yield over polarizer rotationξ is no unambiguous proof of circular polarization. In principle, harmonics could be fully unpolarized and in such a ξ-scan, one would not notice.

To fully characterize the polarization states of CHCD, a characterization of the Stokes parameters is performed in Sec. 2.3.3.