Tunable non-integer high-harmonic generation in a topological insulator

Schmid, Christoph; Weigl, Leonard; Grössing, P.; Junk, Vanessa; Gorini, Cosimo; Schlauderer, S.; Ito, Suguru; Meierhofer, Manuel; Hofmann, Niklas; Afanasiev, D.; Crewse, Jack; Кох, К. А.; Tereshchenko, O. E.; Güdde, J.; Evers, Ferdinand; Wilhelm, Jan; Richter, Klaus; Höfer, U.; Huber, Rupert

doi:10.1038/s41586-021-03466-7

Cited by 159 publications

(76 citation statements)

References 44 publications

(138 reference statements)

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“…HHS of solids [7,8], 2D materials [9,10], or nano-structured media [11,12] differs from the gas phase since the optical-field-driven electronic wavepacket is de-localised over many lattice sites, the wavefunction depends on the lattice momentum, and a hole has to match the electron's momentum for recombination to occur [13,14]. Recent experimental efforts extended HHS as non-perturbative probe to quantum materials [9,10,15] and to topological insulators [16][17][18].…”

Section: Introductionmentioning

confidence: 99%

High harmonic spectroscopy of quantum phase transitions in a high-T$_c$ superconductor

Alcalà¹,

Bhattacharya²,

Biegert³

et al. 2022

Preprint

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We report on the new non-linear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase, and another critical point, which marks the transition from strange metal to pseudogap phase. To reveal the underlying microscopic quantum dynamics, a novel strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs. Further, the new theory provides insight into the carrier scattering dynamics and allows to differentiate between the superconducting, pseudogap, and strange metal phases. The direct connection between non-linear optical response and microscopic dynamics provides a powerful new methodology to study quantum phase transitions in correlated materials. Further implications are light-wave control over intricate quantum phases, light-matter hybrids, and application for optical quantum computing.

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Section: Introductionmentioning

confidence: 99%

High harmonic spectroscopy of quantum phase transitions in a high-T$_c$ superconductor

Alcalà¹,

Bhattacharya²,

Biegert³

et al. 2022

Preprint

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“…Ultrashort THz pulses have enabled resonant access to a broad variety of low-energy elementary excitations in condensed matter, such as plasmons, phonons, magnons, and Higgs modes in superconductors 1 – 7 . Strong THz fields have paved the way to extreme nonlinearities 2 , 8 – 11 such as multi-wave mixing 12 – 15 , high-harmonic generation 9 , 16 , lightwave electronics 8 , and ultrafast nanoscopy 10 , 11 , 17 , 18 . Moreover, a wide range of novel photonics applications has employed THz radiation including high-resolution spectroscopy 1 , 19 , near-field microscopy 20 , and telecommunication concepts 21 .…”

Section: Introductionmentioning

confidence: 99%

Field-resolved high-order sub-cycle nonlinearities in a terahertz semiconductor laser

et al. 2021

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The exploitation of ultrafast electron dynamics in quantum cascade lasers (QCLs) holds enormous potential for intense, compact mode-locked terahertz (THz) sources, squeezed THz light, frequency mixers, and comb-based metrology systems. Yet the important sub-cycle dynamics have been notoriously difficult to access in operational THz QCLs. Here, we employ high-field THz pulses to perform the first ultrafast two-dimensional spectroscopy of a free-running THz QCL. Strong incoherent and coherent nonlinearities up to eight-wave mixing are detected below and above the laser threshold. These data not only reveal extremely short gain recovery times of 2 ps at the laser threshold, they also reflect the nonlinear polarization dynamics of the QCL laser transition for the first time, where we quantify the corresponding dephasing times between 0.9 and 1.5 ps with increasing bias currents. A density-matrix approach reproducing the emergence of all nonlinearities and their ultrafast evolution, simultaneously, allows us to map the coherently induced trajectory of the Bloch vector. The observed high-order multi-wave mixing nonlinearities benefit from resonant enhancement in the absence of absorption losses and bear potential for a number of future applications, ranging from efficient intracavity frequency conversion, mode proliferation to passive mode locking.

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“…Analogous processes are also being investigated in solid-state HHG [6][7][8][9][10], leading to the possibility of compact attosecond light sources [11][12][13][14] and to extend these all-optical spectroscopic abilities to solid materials such as semiconductors [15], dielectrics [8] and to a range of quantum materials (QMs). Recent experimental efforts on highharmonic spectroscopy of QMs include the observation of non-perturbative high-harmonics from graphene [16], monolayer transition metal dicacogenides (TMDC) [17], and topological insulators (TIs) [18][19][20] subjected to intense laser fields without damage.…”

Section: Introductionmentioning

confidence: 99%

“…To this aim, in addition to the demonstration of symmetry breaking at the surface through the measurement of even-order harmonics [18][19][20], it is crucial to elucidate the imprint of characteristic features of 2D TIs on the high harmonic spectra, particularly the strong spinorbit coupling (SOC). The SOC gives rise to the band inversion and the crossing of the surface valence and conduction bands at or near the Fermi level.…”

Section: Introductionmentioning

confidence: 99%

All-optical probe of three-dimensional topological insulators based on high-harmonic generation by circularly-polarized laser fields

Baykusheva,

Chacón,

et al. 2021

Preprint

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We report the observation of a novel nonlinear optical response from the prototypical threedimensional topological insulator Bi 2 Se 3 through the process of high-order harmonic generation.We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a detailed analysis of the measured spectra, we reveal that such anomalous enhancement encodes the characteristic topology of the band structure that originates from the interplay of strong spinorbit coupling and time-reversal symmetry protection. Our study reveals a new platform for chiral strong-field physics and presents a novel, contact-free, all-optical approach for the spectroscopy of topological insulators. The implications are in ultrafast probing of topological phase transitions, light-field driven dissipationless electronics, and quantum computation.

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Tunable non-integer high-harmonic generation in a topological insulator

Abstract: The low photon energy of driving fields in the multi-terahertz (multi-THz) spectral window has proven particularly suitable to

Cited by 159 publications

References 44 publications

High harmonic spectroscopy of quantum phase transitions in a high-T$_c$ superconductor

High harmonic spectroscopy of quantum phase transitions in a high-T$_c$ superconductor

Field-resolved high-order sub-cycle nonlinearities in a terahertz semiconductor laser

All-optical probe of three-dimensional topological insulators based on high-harmonic generation by circularly-polarized laser fields

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