Momentum-resolved resonant photoelectron spectroscopic study for 1T-TiSe$_2$: Observation of negative q in the Fano resonance due to inter-atomic interaction in the valence band

TL;DR

This study uses momentum-resolved resonant photoelectron spectroscopy and DFT calculations to reveal inter-atomic interactions in TiSe$_2$, notably observing a negative q Fano resonance in the valence band, indicating novel inter-atomic effects.

Contribution

First to demonstrate a negative q Fano resonance in the valence band of TiSe$_2$, highlighting inter-atomic interactions during photoelectron emission.

Findings

Observation of hybridization between Ti3d and Se4p orbitals.

First clear evidence of negative q Fano resonance in valence band.

Revealed inter-atomic interactions differ from intra-atomic and core-level MARPE.

Abstract

The remarkable properties of (1T-)TiSe$_2$ among the transition metal dichalcogenides have attracted the attention of many researchers due to its peculiar behavior during the charge density wave (CDW) transition. Therefore, it is highly desirable to study its electronic structure down to the atomic orbitals. In the present research, we applied momentum-resolved resonant photoelectron spectroscopy to study TiSe$_2$ at the Ti2p-Ti3d absorption edge by using a momentum microscope, which can simultaneously detect the electronic states in a wide $(k_x,k_y)$ range. We have also used constant initial state (CIS) spectroscopy and density functional theory (DFT) calculations to reveal the hybridization between the Ti3d and Se4p orbitals within the valence band at the Gamma point at room temperature. In addition, an interesting result comes from our analysis of the CIS spectrum for the energy band located at a binding energy of 2 eV at the M-point. This band, mainly composed of the Se4p orbital, exhibited a Fano line profile at the Ti2p edge, with a negative value of the parameter "$q$". This is the first clear evidence of the inter-atomic interaction during the valence band photoelectron emission process. This behavior differs significantly from the standard resonant photoelectron emission, which usually involves intra-atomic interactions. It also differs from the multi-atom resonant photoelectron emission (MARPE) observed in the core-level photoelectron emission, as we focus on the photoelectron emission from the valence band in this research.