Ballistic and shift currents in the bulk photovoltaic effect theory

TL;DR

This paper critically examines the theoretical foundations of the bulk photovoltaic effect, emphasizing the importance of charge-transport principles and correcting misconceptions about shift current calculations to guide future research.

Contribution

It clarifies the fundamental principles of BPVE, critiques recent misconceptions, and advocates for a more accurate theoretical framework for shift current analysis.

Findings

Highlights the importance of charge-transport phenomena in BPVE

Identifies flaws in the widespread shift current relation

Calls for revisiting theoretical models to align with experimental data

Abstract

The bulk photovoltaic effect (BPVE) -- generation of electric currents by light in noncentrosymmetric materials in the absence of electric fields and gradients -- has been intensively investigated in the end of the last century. The outcomes including all main aspects of this phenomenon were summarized in review and books. A new upsurge of interest to the BPVE occurred recently and resulted in a flux of misleading theoretical and experimental publications centered around the so-called shift current. Numerous top-rated recent publications ignore the basic principles of charge-transport phenomena and the previous results of joined experimental-theoretical studies. Specifically, dominating (or substantial) contributions to the currents caused by asymmetry of the momentum distributions of electrons and holes are missed. The widespread starting relation for the shift current, originating from the quadratic nonlinear response theory and pretending to be omnipotent, is in fact incomplete. It ignores kinetic processes of relaxation and recombination of photo-excited electrons and leads to non-vanishing shift currents in thermal equilibrium. The goals of this methodical note is to specify and argue the benchmarks of the BPVE theory and return the studies on the right track in the interest of development of photovoltaic devices.